**SFB 925**Light induced dynamics and control of correlated quantum systems

# Publications

## Project A

### Project A1

#### Circular Dichroism in Multiphoton Ionization of Resonantly Excited He+ Ions

*M. Ilchen, N. Douguet, T. Mazza, A. J. Rafipoor et. al.*

Intense, circularly polarized extreme-ultraviolet and near-infrared (NIR) laser pulses are combined to double ionize atomic helium via the oriented intermediate He+(3p) resonance state. Applying angle-resolved electron spectroscopy, we find a large photon helicity dependence of the spectrum and the angular distribution of the electrons ejected from the resonance by NIR multiphoton absorption. The measured circular dichroism is unexpectedly found to vary strongly as a function of the NIR intensity. The experimental data are well described by theoretical modeling and possible mechanisms are discussed.

#### Angle resolved photoelectron spectroscopy of two-color XUV-NIR ionization with polarization control

*S. Düsterer, G. Hartmann, F. Babies, A. Beckmann et. al.*

Electron emission caused by extreme ultraviolet (XUV) radiation in the presence of a strong near infrared (NIR) field leads to multiphoton interactions that depend on several parameters. Here, a comprehensive study of the influence of the angle between the polarization directions of the NIR and XUV fields on the two-color angle-resolved photoelectron spectra of He and Ne is presented. The resulting photoelectron angular distribution strongly depends on the orientation of the NIR polarization plane with respect to that of the XUV field. The prevailing influence of the intense NIR field over the angular emission characteristics for He(1s) and Ne(2p) ionization lines is shown. The underlying processes are modeled in the frame of the strong field approximation (SFA) which shows very consistent agreement with the experiment reaffirming the power of the SFA for multicolor-multiphoton ionization in this regime.

#### Coherent control with a short-wavelength Free Electron Laser

*K.C. Prince, E. Allaria, C. Callegari, R. Cucini et. al*

Extreme ultraviolet and X-ray free-electron lasers (FELs) produce short-wavelength pulses with high intensity, ultrashort duration, well-defined polarization and transverse coherence, and have been utilized for many experiments previously possible only at long wavelengths: multiphoton ionization1, pumping an atomic laser2 and four-wave mixing spectroscopy3. However one important optical technique, coherent control, has not yet been demonstrated, because self-amplified spontaneous emission FELs have limited longitudinal coherence4, 5, 6, 7. Single-colour pulses from the FERMI seeded FEL are longitudinally coherent8, 9, and two-colour emission is predicted to be coherent. Here, we demonstrate the phase correlation of two colours, and manipulate it to control an experiment. Light of wavelengths 63.0 and 31.5 nm ionized neon, and we controlled the asymmetry of the photoelectron angular distribution10, 11 by adjusting the phase, with a temporal resolution of 3 as. This opens the door to new short-wavelength coherent control experiments with ultrahigh time resolution and chemical sensitivity.

#### Angular distribution and circular dichroism in the two-colour XUV+NIR above-threshold ionization of helium

*T. Mazza, M. Ilchen, A. J. Rafipoor, C. Callegari et. al.*

The photoelectron angular distribution and the circular dichroism in two-colour XUV+NIR above-threshold ionization of helium atoms have been investigated both experimentally and theoretically. Circularly polarized XUV pulses from the free electron laser FERMI have been spatially and temporally overlapped with circularly polarized optical pulses in the interaction region with an atomic helium jet. The emitted electrons were energy and angle analyzed by means of a velocity map imaging spectrometer. Asymmetry parameters of the angular distribution were determined and compared to theoretical predictions based on the strong field approximation and perturbation theory, respectively. For low NIR intensities, the ratio of the partial waves in the two-photon ionization process and their relative phase could be deduced. For high NIR intensities, the influence of multi-photon processes is discussed. Circular dichroism was revealed in both cases and is in good agreement with the results of the strong field approximation.

#### Dichroism in the photoionisation of atoms at XUV Free Electron Lasers

*T. Mazza, E.V. Gryzlova, A.N. Grum-Grzhimailo, A.K. Kazansky, N.M. Kabachnik, M. Meyer*

Two-color photoionization of atomic He has been investigated by angle-integrated and angle-resolved electron spectroscopy. The combined action of intense radiation pulses from the XUV free-electron laser (FEL), FERMI or FLASH, and a synchronized optical laser on the target atom gives rise to a rich sideband structure in the photoemission spectrum. Measurements of the angular distribution parameters and the determination of the circular and linear dichroism for the two-color photoionization enable a detailed analysis of the symmetry of the outgoing electron waves and of the dynamics underlying the multi-photon processes. The experimental results are in excellent agreement with theoretical results obtained using perturbation theory (low intensity regime) and the strong field approximation. For the particular case of two-photon ionization the measurements represent an ideal tool for characterizing certain FEL parameters, here for example the degree and the sign of circular polarization. Finally, new features of the dichroism are theoretically predicted originating from the non-dipole contribution into the photoionization amplitudes.

#### Probing photoelectron angular distributions in molecules with polarization-controlled two-color above-threshold ionization

*T. Leitner, R. Taieb, M. Meyer, Ph. Wernet*

We present polarization-controlled multiphoton two-color above-threshold ionization (TCATI) of molecules. The intensity modulations of valence photoelectron intensities of molecules arising from varying the relative orientation of the linear polarization vectors of femtosecond infrared (IR) and vacuum-ultraviolet (VUV) radiation in TCATI of the highest occupied molecular orbitals of H2O, O2, and N2 are reported. The results on the molecular systems are compared to the 3p photoionization of atomic Ar, which serves as a reference system. Modeling the large differences of the modulation amplitudes within the soft-photon approximation enables us to extract the one-photon-ionization anisotropy parameter β2. Accounting only for the first sideband due to two-photon TCATI by one VUV and one IR photon we find satisfactory agreement between experiment and simulation for H2O and O2. However, the model fails for N2 and possible reasons are discussed. We discuss that the described approach may represent an alternative way of determining photoelectron angular distributions from valence shells of molecules and indicate future directions for modeling TCATI of molecules.

#### Isotope effects in resonant two-color photoionization of Xe in the region of the 5p5(2P1/2)4f [5/2]2 autoionizing state

*E. V. Gryzlova, P. O. Keeffe, D. Cubaynes, G. A. Garcia, L. Nahon, A. N. Grum-Grzhimailo, M. Meyer*

Isotope effects in two-photon two-color photoionization are investigated by a combined theoretical and experimental study of the ionization of xenon atoms. A combination of variable polarization synchrotron and laser radiations are used to excite the 5p5(2P1/2)4f[5/2]2 autoionizing resonance via the intermediate 5p5(2P3/2)5d[3/2]1 state. Electrons and ions are detected in coincidence in order to extract the photoelectron angular distributions and the values of the linear and circular dichroism and to determine how these depend on the isotope. A complete theoretical model of the two-photon process in atoms is given in order to describe these parameters as a function of the polarization of the exciting light sources (both linear and circular polarization). Furthermore, the hyperfine depolarization due to the coupling of the electronic and nuclear angular momenta in the intermediate state is taken into account. The results of the theoretical model are in agreement with the experimental results and allow estimation of the previously unknown hyperfine structure (HFS) constant for the case of overlapping HFS levels.

Isotope effects in resonant two-color photoionization of Xe in the region of the 5p5(2P1/2)4f[5/2]2 autoionizing state (PDF Download Available). Available from: https://www.researchgate.net/publication/275584741_Isotope_effects_in_resonant_two-color_photoionization_of_Xe_in_the_region_of_the_5p52P124f522_autoionizing_state [accessed Feb 17, 2016].

#### Femtosecond all-optical synchronization of an X-ray free-electron laser

*S. Schulz, I. Grguraš, C. Behrens, H. Bromberger, J. T. Costello, M. K. Czwalinna, M. Felber, M. C. Hoffmann, M. Ilchen, H. Y. Liu, T. Mazza, M. Meyer, S. Pfeiffer, P. Prędki, S. Schefer, C. Schmidt, U. Wegner, H. Schlarb, A. L. Cavalieri*

Many advanced applications of X-ray free-electron lasers require pulse durations and time resolutions of only a few femtoseconds. To generate these pulses and to apply them in time-resolved experiments, synchronization techniques that can simultaneously lock all independent components, including all accelerator modules and all external optical lasers, to better than the delivered free-electron laser pulse duration, are needed. Here we achieve all-optical synchronization at the soft X-ray free-electron laser FLASH and demonstrate facility-wide timing to better than 30 fs r.m.s. for 90 fs X-ray photon pulses. Crucially, our analysis indicates that the performance of this optical synchronization is limited primarily by the free-electron laser pulse duration, and should naturally scale to the sub-10 femtosecond level with shorter X-ray pulses.

#### Determining the polarization state of an extreme ultraviolet free-electron laser beam using atomic circular dichroism

*T. Mazza, M. Ilchen, A. J. Rafipoor, C. Callegari, P. Finetti, O. Plekan, K. C. Prince, R. Richter, M. B. Danailov, A. Demidovich, G. De Ninno, C. Grazioli, R. Ivanov, N. Mahne, M. Meyer et al*

Ultrafast extreme ultraviolet and X-ray free-electron lasers are set to revolutionize many domains such as bio-photonics and materials science, in a manner similar to optical lasers over the past two decades. Although their number will grow steadily over the coming decade, their complete characterization remains an elusive goal. This represents a significant barrier to their wider adoption and hence to the full realization of their potential in modern photon sciences. Although a great deal of progress has been made on temporal characterization and wavefront measurements at ultrahigh extreme ultraviolet and X-ray intensities, only few, if any progress on accurately measuring other key parameters such as the state of polarization has emerged. Here we show that by combining ultra-short extreme ultraviolet free electron laser pulses from FERMI with near-infrared laser pulses, we can accurately measure the polarization state of a free electron laser beam in an elegant, non-invasive and straightforward manner using circular dichroism.

#### Isotopically Resolved Photoelectron Imaging Unravels Complex Atomic Autoionization Dynamics by Two-Color Resonant Ionization

*P. O’Keeffe, E. V. Gryzlova, D. Cubaynes, G. A. Garcia, L. Nahon, A. N. Grum-Grzhimailo, M. Meyer*

Angle-resolved electron spectroscopy in coincidence with high-resolution mass spectroscopy has been applied to study two-color resonant photoionization in atomic xenon. Separation of different isotopes enabled us to extract results for the electronic dynamics free from depolarization effects, which are generally introduced by the coupling of the electronic and nuclear angular momenta. The concerted experimental and theoretical analysis of the photoelectron angular distributions in the region of an autoionizing resonance emphasizes the strong sensitivity of the observed structures to the fine details of the treatment of the underlying dynamics.

#### Accelerator- and laser-based sources of high-field terahertz pulses

*N. Stojanovic, M. Drescher*

At present we are witnessing a rapid development of sources for terahertz (THz) pulses with very strong electromagnetic fields. These pulses are reaching a stage where they can be used to not only probe, but also uniquely control a variety of processes that range from fundamental dynamics in individual atoms and molecules, through phase transitions in solids to a wealth of interactions in biological materials. In this review, we are presenting an overview of two major directions in the generation of such radiation. Large-scale accelerator-based sources offer unprecedented pulse energies coupled with a wide tuning range and extreme repetition rates. Laser-based sources, on the other hand, are laboratory-scale instruments and thus are very attractive in their availability to the wide scientific community. The capabilities of different variants of these THz sources are evaluated and compared with each other. In addition, powerful techniques for the temporal characterization of THz pulses are discussed.

#### Interference in the angular distribution of photoelectrons in superimposed XUV and optical laser fields

*S. Düsterer, L Rading, P. Johnsson, A. Rouzée, A. Hundertmark, M. J. J. Vrakking, P. Radcliffe, M. Meyer, A. K. Kazansky, N. M. Kabachnik*

The angular distribution of photoelectrons ejected during the ionization of Ne atoms by extreme ultraviolet (XUV) free-electron laser radiation in the presence of an intense near infrared (NIR) dressing field was investigated experimentally and theoretically. A highly nonlinear process with absorption and emission of more than ten NIR photons results in the formation of numerous sidebands. The amplitude of the sidebands varies strongly with the emission angle and the angular distribution pattern reveals clear signatures of interferences between the different angular momenta for the outgoing electron in the multi-photon process. As a specific feature, the central photoelectron line is characterized at the highest NIR fields by an angular distribution, which is peaked perpendicularly to both the XUV and NIR polarization directions. Experimental results are reproduced by a theoretical model based on the strong field approximation.

#### Ultrafast X-ray pulse characterization at free-electron lasers

*I. Grguraš, A. R. Maier, C. Behrens, T. Mazza, T. J. Kelly, P. Radcliffe, S. Düsterer, A. K. Kazansky, N. M. Kabachnik, Th. Tschentscher, J. T. Costello, M. Meyer, M. C. Hoffmann, H. Schlarb, A. L. Cavalieri*

The ability to fully characterize ultrashort, ultra-intense X-ray pulses at free-electron lasers (FELs) will be crucial in experiments ranging from single-molecule imaging to extreme-timescale X-ray science. This issue is especially important at current-generation FELs, which are primarily based on self-amplified spontaneous emission and radiate with parameters that fluctuate strongly from pulse to pulse. Using single-cycle terahertz pulses from an optical laser, we have extended the streaking techniques of attosecond metrology to measure the temporal profile of individual FEL pulses with 5 fs full-width at half-maximum accuracy, as well as their arrival on a time base synchronized to the external laser to within 6 fs r.m.s. Optical laser-driven terahertz streaking can be utilized at any X-ray photon energy and is non-invasive, allowing it to be incorporated into any pump–probe experiment, eventually characterizing pulses before and after interaction with most sample environments.

#### Controlling core hole relaxation dynamics via intense optical fields

*T. Mazza, K. G. Papamihail, P. Radcliffe, W. B. Li, T. J. Kelly, J. T. Costello, S. Düsterer, P. Lambropoulos, M. Meyer*

The influence of an intense optical laser on the electronic relaxation of the 3d–5p resonance in atomic Kr has been studied experimentally and theoretically. The resonance profile undergoes a strong modification, observed as a shift and a broadening of the excitation spectrum, as a function of the optical intensity. The theoretical treatment of the process demonstrates the importance of strongly time-dependent dynamics as the origin of the observed phenomena resulting in the ponderomotive shift of the resonance position as well as a competition between resonant and normal Auger decay. The ionization of the excited 5p electron by the optical laser provides the possibility to change the ratio between singly and doubly charged final states by controlling the relaxation of the resonant core hole state via resonant or normal Auger decay.

#### Evidence for Chirped Auger-Electron Emission

*B. Schuette, S. Bauch, U. Fruehling, M. Wieland, M. Gensch, E. Ploenjes, T. Gaumnitz, A. Azima, M. Bonitz, M. Drescher*

Auger decay carries valuable information about the electronic structure and dynamics of atoms, molecules, and solids. Here we furnish evidence that under certain conditions Auger electrons are subject to an energetic chirp. The effect is disclosed in time-resolved streaking experiments on the Xe NOO and Kr MNN Auger decay using extreme-ultraviolet pulses from the free-electron laser in Hamburg as well as from a high-order harmonic laser source. The origin of this effect is found to be an exchange of energy between the Auger electron and an earlier emitted correlated photoelectron. The observed time-dependent spectral modulations are understood within an analytical model and confirmed by extensive computer simulations.

#### Light-field streaking for FELs

*U. Frühling*

Free-electron lasers provide intense femtosecond radiation pulses with wavelengths in the extreme ultraviolet to x-ray range. Due to the stochastic nature of the light generation scheme, based on self-amplified spontaneous emission, the duration and temporal profile fluctuate from shot to shot. The temporal profile can be measured in a single-shot experiment by light-field streaking, where an infrared light field is used to accelerate photoelectrons generated by the x-ray pulse. The photoelectron energy change depends on the phase of the infrared field at the time of ionization. This technique is extensively used in attosecond metrology where near-infrared streaking fields are employed for the temporal characterization of attosecond XUV pulses. Here, it is adapted for the analysis of pulse durations in the femtosecond range by choosing far-infrared (terahertz) streaking fields.

#### Time-and-energy-resolved measurement of Auger cascades following Kr 3d excitation by attosecond pulses

*A. J. Verhoef, A. V. Mitrofanov, X. T. Nguyen, M. Krikunova, S. Fritzsche, N. M. Kabachnik, M. Drescher, A Baltuška*

We show that attosecond metrology has evolved from proof-of-principle experiments to a level where complex processes can be resolved in time that cannot be accessed using any other existing technique. The cascaded Auger decay following ionization and excitation of the 3d-subshell in Kr with subfemtosecond 94 eV soft x-ray pulses has been energy- and time-resolved in an x-ray pump–infrared probe experiment. This Auger cascade reveals rich multi-electron dynamics, which despite the fact that there are many experimental and theoretical data available, is not yet fully understood. We present time-resolved data showing the sequence of the temporal dynamics in the cascaded Auger decay. The decay time of several groups of lines has been measured, including the lines at the low-energy part of the spectrum, which are predominantly produced by the second-step Auger transitions. Our experimental data reveal long lifetimes (up to 70 fs) of the subvalence excited ionic (intermediate) states in the cascaded resonant Auger decay. Extensive theoretical calculations within the multiconfiguration Dirac–Fock (MCDF) approach show that the observed long lifetime may be attributed to the second-step Auger decay of the resonantly excited 3d−1np states with n = 6,7. Furthermore, our experimental data show that the electrons with a kinetic energy around 25 eV (generally assigned as M4,5N1N1 1S0 normal Auger lines) have a component corresponding to the second-step Auger decay of the ion after resonant Auger transition 3d−1np → 4s2 4p3 4dnp → 4s2 4p4 with a lifetime of 26 ± 4 fs.

#### Electron wave packet sampling with laser-generated extreme ultraviolet and terahertz fields

*B. Schütte, U. Frühling, M. Wieland, A. Azima, M. Drescher*

We report on transferring the concept of light-field streaking with intense terahertz fields from free-electron lasers to the laboratory scale. Utilizing a commercial laser system, synchronized 300μm terahertz and 13nm extreme ultraviolet pulses are generated by optical rectification and high harmonic generation, respectively. The terahertz fields are sufficiently strong to support electron wave packet sampling with a few fs resolution. The capability of this approach is demonstrated by measuring the duration of electron pulses formed by direct photoemission from a neon gas target.

### Project A2

#### Weak-field few-femtosecond VUV photodissociation dynamics of water isotopologues

*A. Baumann, S. Bazzi, D. Rompotis, O. Schepp, A. Azima, M. Wieland, D. Popova-Gorelova, O. Vendrell, R. Santra, M. Drescher*

We present a joint experimental and theoretical study of the VUV-induced dynamics of H2O and its deuterated isotopologues in the first excited state (˜A1B1) utilizing a VUV-pump VUV-probe scheme combined with ab initio classical trajectory calculations. 16-fs VUV pulses centered at 161 nm created by fifth-order harmonic generation are employed for single-shot pump-probe measurements. Combined with a precise determination of the VUV pulses' temporal profile, they provide the necessary temporal resolution to elucidate sub-10-fs dissociation dynamics in the 1+1 photon ionization time window. Ionization with a single VUV photon complements established strong-field ionization schemes by disclosing the molecular dynamics under perturbative conditions. Kinetic isotope effects derived from the pump-probe experiment are found to be in agreement with our by ab initio classical trajectory calculations, taking into account photoionization cross sections for the ground and first excited state of the water cation.

#### Single-shot nonlinear spectroscopy in the vacuum-ultraviolet

*D. Rompotis, A. Baumann, O. Schepp, T. Maltezopoulos, M. Wieland, M. Drescher*

Time-resolved spectroscopy in the vacuum/extreme ultraviolet (VUV/XUV) spectral range promises to disclose ultrafast dynamics in all states of matter. Completing a measurement within a single shot eliminates the influence of experimental parameter fluctuations and enhances its statistical significance. We demonstrate a single-shot temporal metrology scheme operating in the vacuum/extreme-ultraviolet spectral range, combining few-femtosecond resolution in a wide temporal window with high detection efficiency. An anticollinear geometry encodes temporal delay information on the beam propagation coordinate. The spatial distribution of ions created in the common focus is captured with a mass/charge-state-selective ion imaging spectrometer, resulting in a single-shot pump–probe measurement. We demonstrate a proof-of-principle single-shot VUV-pump/VUV-probe experiment by investigating ultrafast dissociation dynamics of O2 excited at 162 nm. The experimental determination of the finite instrument response in the same apparatus enables robust deconvolution of the investigated dynamics well beyond the instrument’s intrinsic temporal resolution.

#### Attosecond interferometry with self-amplified spontaneous emission of a free-electron laser

*Usenko, A. Przystawik, M.A. Jakob, L.L. Lazzarino, G. Brenner, S. Toleikis, Ch. Haunhorst, D. Kip, T. Laarmann*

Light-phase-sensitive techniques, such as coherent multidimensional spectroscopy, are well-established in a broad spectral range, already spanning from radio-frequencies in nuclear magnetic resonance spectroscopy to visible and ultraviolet wavelengths in nonlinear optics with table-top lasers. In these cases, the ability to tailor the phases of electromagnetic waves with high precision is essential. Here we achieve phase control of extreme-ultraviolet pulses from a free-electron laser (FEL) on the attosecond timescale in a Michelson-type all-reflective interferometric autocorrelator. By varying the relative phase of the generated pulse replicas with sub-cycle precision we observe the field interference, that is, the light-wave oscillation with a period of 129 as. The successful transfer of a powerful optical method towards short-wavelength FEL science and technology paves the way towards utilization of advanced nonlinear methodologies even at partially coherent soft X-ray FEL sources that rely on self-amplified spontaneous emission.

#### Split-and-delay unit for FEL interferometry in the XUV spectral range

*S. Usenko, A. Przystawik, L.L. Lazzarino, M.A. Jakob, F. Jacobs, C. Becker, C. Haunhorst, D. Kip, and T. Laarmann*

In this work we present a reflective split-and-delay unit (SDU) developed for interferometric time-resolved experiments utilizing an (extreme ultraviolet) XUV pump–XUV probe scheme with focused free-electron laser beams. The developed SDU overcomes limitations for phase-resolved measurements inherent to conventional two-element split mirrors by a special design using two reflective lamellar gratings. The gratings produce a high-contrast interference signal controlled by the grating displacement in every diffraction order. The orders are separated in the focal plane of the focusing optics, which enables one to avoid phase averaging by spatially selective detection of a single interference state of the two light fields. Interferometry requires a precise relative phase control of the light fields, which presents a challenge at short wavelengths. In our setup the phase delay is determined by an in-vacuum white light interferometer (WLI) that monitors the surface profile of the SDU in real time and thus measures the delay for each laser shot. The precision of the WLI is 1 nm as determined by optical laser interferometry. In the presented experimental geometry it corresponds to a time delay accuracy of 3 as, which enables phase-resolved XUV pump–XUV probe experiments at free-electron laser (FEL) repetition rates up to 60 Hz.

#### Femtosecond dynamics of correlated many-body states in C60 fullerenes

*S. Usenko, M. Schüler, A. Azima, M. Jakob, L.L. Lazzarino, Y. Pavlyukh, A. Przystawik, M. Drescher, T. Laarmann, J. Berakdar*

Fullerene complexes may play a key role in the design of future molecular electronics and nanostructured devices with potential applications in light harvesting using organic solar cells. Charge and energy flow in these systems is mediated by many-body effects. We studied the structure and dynamics of laser-induced multi-electron excitations in isolated C60 by two-photon photoionization as a function of excitation wavelength using a tunable fs UV laser and developed a corresponding theoretical framework on the basis of ab initio calculations. The measured resonance line width gives direct information on the excited state lifetime. From the spectral deconvolution we derive a lower limit for purely electronic relaxation on the order of Tel=10+5-3 fs. Energy dissipation towards nuclear degrees of freedom is studied with time-resolved techniques. The evaluation of the nonlinear autocorrelation trace gives a characteristic time constant of Tvib=400+-100 fs for the exponential decay. In line with the experiment, the observed transient dynamics is explained theoretically by nonadiabatic (vibronic) couplings involving the correlated electronic, the nuclear degrees of freedom (accounting for the Herzberg–Teller coupling), and their interplay.

#### Tracing few-femtosecond photodissociation dynamics on molecular oxygen with a single-color pump-probe scheme in the VUV

*O. Schepp, A. Baumann, D. Rompotis, T. Gebert, A. Azima, M. Wieland, M. Drescher*

#### Efficient generation of below-threshold harmonics for high-fidelity multi-photon physics in the VUV spectral range

*D. Rompotis, T. Gebert, M. Wieland, F. Karimi, M. Drescher*

We demonstrate the generation of microjoule level, sub-20-fs, Ti:Sa fifth-harmonic pulses utilizing a loose-focusing geometry in a long Ar gas cell. The VUV pulses centered at 161.8 nm reach pulse energies of 1.1 μJ per pulse, while the corresponding pulse duration is measured with a second-order, fringe-resolved autocorrelation scheme to be 18±1 fs. Nonresonant, two-photon ionization of Kr and three-photon ionization of Ne verify the fifth-harmonic pulse high-intensity content and indicate the feasibility of multi-photon VUV pump-VUV probe studies of ultrafast atomic and molecular dynamics.

#### Ionisation dynamics of Xe nanoplasma formation studied with XUV fluorescence spectroscopy

*A. Przystawik, L. Schroedter, M. Müller, M. Adolph, C. Bostedt, L. Flückiger, T. Gorkhover, A. Kickermann, M. Krikunova, Nösel, T. Oelze, Y. Ovcharenko, D. Rupp, L. M. Sauppe, S. Schorb, S. Usenko, T. Möller, T. Laarmann*

Intense pulses from a short wavelength free-electron laser turn xenon nanoparticles into a high energy density nanoplasma within femtoseconds. Recently, the generation of multiply charged xenon ions during the initial phase of plasma evolution has been studied by energy-resolved XUV fluorescence detection as a function of cluster size and cluster composition [1]. In the present contribution we give a detailed analysis of the corresponding radiative transitions after resonant excitation of the 4d electron shell at intensities of 2 × 1012 − 2.45 × 1015 W cm−2. The evaluation of charge-state specific fluorescence yields as a function of FEL power density demonstrates that plasma effects such as ionization potential lowering, electron impact excitation, ionization, and energy redistribution govern the laser-induced non-equilibrium dynamics in xenon clusters.

#### Ionization dynamics of XUV excited clusters: the role of inelastic electron collisions

*M. Müller, L. Schroedter, T. Oelze, L. Nösel, A. Przystawik, A. Kickermann, M. Adolph, T. Gorkhover, L. Flückiger, M. Krikunova, M. Sauppe, Y. Ovcharenko, S. Schorb, C. Bostedt, D. Rupp, T. Laarmann, T. Möller*

We report on the ionization and nanoplasma dynamics of small xenon clusters irradiated by intense, short pulses of a short-wavelength free-electron laser. Fluorescence spectroscopy indicates that inelastic electron collisions play a prominent role in the formation of the highest charge states. From the spectral distribution an electron temperature of 27 eV is deduced which corresponds to the average excess energy of the Auger- and photoelectrons ionized from individual atoms but trapped in the cluster core. This suggests that fluorescence spectra reflect a very early stage within the nanoplasma dynamics and shows how a part of the kinetic energy of the plasma electrons trapped in the cluster potential is transferred to the ions.

#### Hidden Charge States in Soft-X-Ray Laser-Produced Nanoplasmas Revealed by Fluorescence Spectroscopy

*L. Schroedter, M. Müller, A. Kickermann, A. Przystawik, S. Toleikis, M. Adolph, L. Flückiger, T. Gorkhover, L. Nösel, M. Krikunova, T. Oelze, Y. Ovcharenko, D. Rupp, M. Sauppe, D. Wolter, S. Schorb, C. Bostedt, T. Möller, T. Laarmann*

Highly charged ions are formed in the center of composite clusters by strong free-electron laser pulses and they emit fluorescence on a femtosecond time scale before competing recombination leads to neutralization of the nanoplasma core. In contrast to mass spectrometry that detects remnants of the interaction, fluorescence in the extreme ultraviolet spectral range provides fingerprints of transient states of high energy density matter. Spectra from clusters consisting of a xenon core and a surrounding argon shell show that a small fraction of the fluorescence signal comes from multiply charged xenon ions in the cluster core. Initially, these ions are as highly charged as the ions in the outer shells of pure xenon clusters with charge states up to at least.

#### A high-harmonic generation source for seeding a free-electron laser at 38 nm

*T. Maltezopoulos, M. Mittenzwey, A. Azima, J. Bödewadt, H. Dachraoui, M. Rehders, C. Lechner, M. Schulz, M. Wieland, T. Laarmann, J. Roßbach, M. Drescher*

Direct seeding with a high-harmonic generation (HHG) source can improve the spectral, temporal, and coherence properties of a free-electron laser (FEL) and shall reduce intensity and arrival-time fluctuations. In the seeding experiment sFLASH at the extreme ultraviolet FEL in Hamburg FLASH, which operates in the self-amplified spontaneous emission mode (SASE), the 21st harmonic of an 800 nm laser is refocused into a dedicated seeding undulator. For seeding, the external light field has to overcome the noise level of SASE; therefore, an efficient coupling between seed pulse and electron bunch is mandatory. Thus, an HHG beam with a proper divergence, width, beam quality, Rayleigh length, pointing stability, single-shot pulse energy, and stability in the 21st harmonic is needed. Here, we present the setup of the HHG source that seeds sFLASH at 38.1 nm, the optimization procedures, and the necessary diagnostics.

#### Generation of Coherent 19- and 38-nm Radiation at a Free-Electron Laser Directly Seeded at 38 nm

*S. Ackermann, et al.*

Initiating the gain process in a free-electron laser (FEL) from an external highly coherent source of radiation is a promising way to improve the pulse properties such as temporal coherence and synchronization performance in time-resolved pump-probe experiments at FEL facilities, but this so-called “seeding” suffers from the lack of adequate sources at short wavelengths. We report on the first successful seeding at a wavelength as short as 38.2 nm, resulting in GW-level, coherent FEL radiation pulses at this wavelength as well as significant second harmonic emission at 19.1 nm. The external seed pulses are about 1 order of magnitude shorter compared to previous experiments allowing an ultimate time resolution for the investigation of dynamic processes enabling breakthroughs in ultrafast science with FELs. The seeding pulse is the 21st harmonic of an 800-nm, 15-fs (rms) laser pulse generated in an argon medium. Methods for finding the overlap of seed pulses with electron bunches in spatial, longitudinal, and spectral dimensions are discussed and results are presented. The experiment was conducted at FLASH, the FEL user facility at DESY in Hamburg, Germany.

#### Generation of the simplest rotational wave packet in a diatomic molecule: Tracing a two-level superposition in the time domain

*A. Przystawik, A. Kickermann, A. Al-Shemmary, S. Düsterer, A. M. Ellis, K. von Haeften, M. Harmand, S. Ramakrishna, H. Redlin, L. Schroedter, M. Schulz, T. Seideman, N. Stojanovic, J. Szekely, F. Tavella, S. Toleikis, T. Laarmann*

We introduce a time-domain approach to explore rotational dynamics caused by intramolecular coupling or the interaction with dissipative media. It pushes the time resolution toward the ultimate limit determined by the rotational period. Femtosecond pulses create a coherent superposition of two rotational states of carbon monoxide. The wave-packet motion is observed by subsequent Coulomb explosion, which results in a time-dependent asymmetry of spatial fragmentation patterns. The asymmetry oscillation prevails for at least 1 ns, covering more than 300 periods with no decoherence. Long time scans will allow weak perturbations of the order of ΔE/E=10−4 to be discerned. Our conclusions are confirmed by a fully quantum-mechanical model.

#### Michelson-type all-reflective interferometric autocorrelation in the VUV regime

*T. Gebert, D. Rompotis, M. Wieland, F. Karimi, A. Azima, M. Drescher*

We demonstrate second-order interferometric autocorrelation of a pulse in the vacuum-ultraviolet (VUV) spectral range using an optical arrangement equivalent to a Michelson interferometer. In an all-reflective design, wavefront splitting is realized with two moveable interdigitated reflective gratings forming a diffraction pattern with well separated orders and an intensity distribution depending on the precisely adjustable path-length difference. An imaging time-of-flight spectrometer is able to spatially select ions created by nonlinear two-photon absorption in the focus of the zeroth diffraction order. This arrangement is used to demonstrate interferometric autocorrelation in krypton with femtosecond VUV pulses at 160 nm wavelength. In addition to the pulse duration, which is already accessible with non-collinear intensity autocorrelation, the full interferometric contrast of the presented approach enables us to extract also information on temporal phases.

#### Moving the Frontier of Quantum Control into the Soft X-Ray Spectrum

*A. Aquila, M. Drescher, T. Laarmann, M. Barthelmeß, H. N. Chapman, S. Bajt*

The femtosecond nature of X-ray free electron laser (FEL) pulses opens up exciting research possibilities in time-resolved studies including femtosecond photoemission and diffraction. The recent developments of seeding X-ray FELs extend their capabilities by creating stable, temporally coherent, and repeatable pulses. This in turn opens the possibility of spectral engineering soft X-ray pulses to use as a probe for the control of quantum dynamics. We propose a method for extending coherent control pulse-shaping techniques to the soft X-ray spectral range by using a reflective geometry 4f pulse shaper. This method is based on recent developments in asymmetrically cut multilayer optic technology and piezoelectric substrates.

International Journal of Optics Volume 2011 (2011), Article ID 417075

### Project A3

#### Two-electron Processes in Multiple Ionization under Strong Soft X-ray Radiation

*M. Ilchen, T. Mazza, E. T. Karamatskos, D. Markellos, S. Bakhtiarzadeh, A. J. Rafipoor, T. J. Kelly, N. Walsh, J. T. Costello, P. O’Keeffe, N. Gerken, M. Martins, P. Lambropoulos, M. Meyer*

In a combined experimental and theoretical study we have investigated the ionization of atomic argon upon irradiation with intense soft-x-ray pulses of 105 eV photon energy from the free-electron laser FLASH. The measured ion yields show charge states up to Ar7+. The comparison with the theoretical study of the underlying photoionization dynamics highlights the importance of excited states in general and of processes governed by electron correlation in particular, namely, ionization with excitation and shake-off, processes usually inaccessible by measurements of ionic yields only. The Ar7+ yield shows a clear deviation from the predictions of the commonly used model of sequential ionization via single-electron processes and the observed signal can only be explained by taking into account the full multiplet structure of the involved configurations and by inclusion of two-electron processes. The competing process of two-photon ionization from the ground state of Ar6+ is calculated to be orders of magnitude smaller.

#### Sensitivity of nonlinear photoionization to resonance substructure in collective excitation

*T. Mazza, A. Karamatskou, M. Ilchen, S. Bakhtiarzadeh, A. J. Rafipoor, P. O’Keeffe, T. J. Kelly, N. Walsh, J. T. Costello, M. Meyer, R. Santra*

Collective behaviour is a characteristic feature in many-body systems, important for developments in fields such as magnetism, superconductivity, photonics and electronics. Recently, there has been increasing interest in the optically nonlinear response of collective excitations. Here we demonstrate how the nonlinear interaction of a many-body system with intense XUV radiation can be used as an effective probe for characterizing otherwise unresolved features of its collective response. Resonant photoionization of atomic xenon was chosen as a case study. The excellent agreement between experiment and theory strongly supports the prediction that two distinct poles underlie the giant dipole resonance. Our results pave the way towards a deeper understanding of collective behaviour in atoms, molecules and solid-state systems using nonlinear spectroscopic techniques enabled by modern short-wavelength light sources.

#### Observation of a Four-Electron Auger Process in Near-K-Edge Photoionization of Singly Charged Carbon Ions

*A. Müller, A. Borovik, Jr., T. Buhr, J. Hellhund, K. Holste, A. L. D. Kilcoyne, S. Klumpp, M. Martins, S. Ricz, J. Viefhaus, S. Schippers*

#### High resolution multi-photon spectroscopy by a tunable free-electron-laser light

*M. Zitnik, A. Mihelic, K. Bucar, M. Kavcic, J.-E. Rubensson, M. Svanquist, J. Söderström, R. Feifel, C. Sathe, Y. Ovcharenko, V. Lyamayev, T. Mazza, M. Meyer, M. Simon, L. Journel, J. Lüning, O. Plekan, M. Coreno, M. Devetta, M. Di Fraia, et. al*

Seeded free electron lasers theoretically have the intensity, tunability, and resolution required for multiphoton spectroscopy of atomic and molecular species. Using the seeded free electron laser FERMI and a novel detection scheme, we have revealed the two-photon excitation spectra of dipole-forbidden doubly excited states in helium. The spectral profiles of the lowest (−1,0)+1 Se1 and (0,1)0 De1 resonances display energy shifts in the meV range that depend on the pulse intensity. The results are explained by an effective two-level model based on calculated Rabi frequencies and decay rates.

#### Time-Dependent Multiphoton Ionization of Xenon in the Soft-X-Ray Regime

*N. Gerken, S. Klumpp, A. A. Sorokin, K. Tiedtke, M. Richter, V. Bürk, K. Mertens, P. Jurani, M. Martins*

The time-dependent multiphoton ionization of xenon atoms is studied with femtosecond pulses in the excitation range of the 4d giant resonance at the photon energy of 93 eV. Benefiting from a new operation mode of the free electron laser FLASH, the measurements are performed with varying pulse durations. A strong dependence of the ion charge distribution on the pulse duration allows the different multiphoton mechanisms behind the multiple photoionization of xenon to be disentangled up to a charge state of Xe10+. The results up to Xe8+ are well explained by sequences of single photon, multiphoton, and Auger processes, but higher charge state generation suggests the need for collective electron multiphoton excitations.

#### Non-dipole effects in the angular distribution of photoelectrons in sequential two-photon double ionization: argon and neon

*E. V. Gryzlova, A. N. Grum-Grzhimailo, S. I. Strakhova, M. Meyer*

As an extension to recent developments in the theory of non-dipole effects in nonlinear photoprocesses in the XUV/x-ray wavelength regime, the sequential two-photon double ionization of the 3p shell in atomic argon is studied theoretically and compared to similar processes in the 2p shell of neon. The calculations predict distinct non-dipole effects in the region of the Cooper minimum in argon at photon energies around 50 eV, where they are of similar importance as at photon energies of more than 500 eV. The non-dipole effects should therefore be clearly observable in experiments performed at the present x-ray free electron lasers.

### Project A4

#### Light-Induced Radical Formation and Isomerization of an Aromatic Thiol in Solution Followed by Time-Resolved X-ray Absorption Spectroscopy at the Sulfur K-Edge

*M. Ochmann, I. von Ahnen, A. A. Cordones, A. Hussain, J. H. Lee, K. Hong, K. Adamczyk, O. Vendrell , T. K. Kim , R. W. Schoenlein, N. Huse*

We applied time-resolved sulfur-1s absorption spectroscopy to a model aromatic thiol system as a promising method for tracking chemical reactions in solution. Sulfur-1s absorption spectroscopy allows tracking multiple sulfur species with a time resolution of ∼70 ps at synchrotron radiation facilities. Experimental transient spectra combined with high-level electronic structure theory allow identification of a radical and two thione isomers, which are generated upon illumination with 267 nm radiation. Moreover, the regioselectivity of the thione isomerization is explained by the resulting radical frontier orbitals. This work demonstrates the usefulness and potential of time-resolved sulfur-1s absorption spectroscopy for tracking multiple chemical reaction pathways and transient products of sulfur-containing molecules in solution.

#### Hydration shell effects in the relaxation dynamics of photoexcited Fe-II complexes in water

*P. Nalbach, A. J. A. Achner, M. Frey, M. Grosser, C. Bressler, M. Thorwart*

We study the relaxation dynamics of photoexcited Fe-II complexes dissolved in water and identify the relaxation pathway which the molecular complex follows in presence of a hydration shell of bound water at the interface between the complex and the solvent. Starting from a low-spin state, the photoexcited complex can reach the high-spin state via a cascade of different possible transitions involving electronic as well as vibrational relaxation processes. By numerically exact path integral calculations for the relaxational dynamics of a continuous solvent model, we find that the vibrational life times of the intermittent states are of the order of a few ps. Since the electronic rearrangement in the complex occurs on the time scale of about 100 fs, we find that the complex first rearranges itself in a high-spin and highly excited vibrational state, before it relaxes its energy to the solvent via vibrational relaxation transitions. By this, the relaxation pathway can be clearly identified. We find that the life time of the vibrational states increases with the size of the complex (within a spherical model), but decreases with the thickness of the hydration shell, indicating that the hydration shell acts as an additional source of fluctuations.

#### Solvation Dynamics Monitored by Combined X-Ray Spectroscopies and Scattering: Photoinduced Spin Transition in aqueous [Fe(bpy)3]2+

*C. Bressler, W. Gawelda, A. Galler, M. M. Nielsen, V. Sundström, G. Doumy, A. M. March, S. H. Southworth, L. Young, G. Vankó*

We have studied the photoinduced low spin (LS) to high spin (HS) conversion of aqueous Fe(bpy)3 with pulse-limited time resolution. In a combined setup permitting simultaneous X-ray diffuse scattering (XDS) and spectroscopic measurements at a MHz repetition rate we have unraveled the interplay between intramolecular dynamics and the intermolecular caging solvent response with 100 ps time resolution. On this time scale the ultrafast spin transition including intramolecular geometric structure changes as well as the concomitant bulk solvent heating process due to energy dissipation from the excited HS molecule are long completed. The heating is nevertheless observed to further increase due to the excess energy between HS and LS states released on a subnanosecond time scale. The analysis of the spectroscopic data allows precise determination of the excited population which efficiently reduces the number of free parameters in the XDS analysis, and both combined permit extraction of information about the structural dynamics of the first solvation shell.

#### Tracking excited-state charge and spin dynamics in iron coordination complexes

*W. Zhang, R. Alonso-Mori, U. Bergmann, C. Bressler, M. Chollet, A. Galler, W. Gawelda, R. G. Hadt, R. W. Hartsock1, T. Kroll, K. S. Kjær, K. Kubicˇek, H. T. Lemke, H. W. Liang, D. A. Meyer, M. M. Nielsen, C. Purser, J. S. Robinson, et. al*

Crucial to many light-driven processes in transition metal complexes is the absorption and dissipation of energy by 3d electrons1, 2, 3, 4. But a detailed understanding of such non-equilibrium excited-state dynamics and their interplay with structural changes is challenging: a multitude of excited states and possible transitions result in phenomena too complex to unravel when faced with the indirect sensitivity of optical spectroscopy to spin dynamics5 and the flux limitations of ultrafast X-ray sources6, 7. Such a situation exists for archetypal polypyridyl iron complexes, such as [Fe(2,2′-bipyridine)3]2+, where the excited-state charge and spin dynamics involved in the transition from a low- to a high-spin state (spin crossover) have long been a source of interest and controversy6, 7, 8, 9, 10, 11, 12, 13, 14, 15. Here we demonstrate that femtosecond resolution X-ray fluorescence spectroscopy, with its sensitivity to spin state, can elucidate the spin crossover dynamics of [Fe(2,2′-bipyridine)3]2+ on photoinduced metal-to-ligand charge transfer excitation. We are able to track the charge and spin dynamics, and establish the critical role of intermediate spin states in the crossover mechanism. We anticipate that these capabilities will make our method a valuable tool for mapping in unprecedented detail the fundamental electronic excited-state dynamics that underpin many useful light-triggered molecular phenomena involving 3d transition metal complexes.

#### Guest-Host Interactions Investigated by Time-Resolved X-Ray Spectroscopies and Scattering at MHz rates: Solvation Dynamics and Photoinduced Spin Transition in Aquesous [Fe(bipy]3]2+

*K. Haldrup, G. Vankó, W. Gawelda, A. Galler, G. Doumy, A. M. March, E. P. Kanter, A. Bordage, A. Dohn, T. B. van Driel, K. S. Kjaer, H. T. Lemke, S. E. Canton, J. Uhlig, V. Sundström, L. Young, S. Southworth, M. M. Nielsen, C. Bressler*

We have studied the photoinduced low spin (LS) to high spin (HS) conversion of [Fe(bipy)(3)](2+) in aqueous solution. In a laser pump/X-ray probe synchrotron setup permitting simultaneous, time-resolved X-ray diffuse scattering (XDS) and X-ray spectroscopic measurements at a 3.26 MHz repetition rate, we observed the interplay between intramolecular dynamics and the intermolecular caging solvent response with better than 100 ps time resolution. On this time scale, the initial ultrafast spin transition and the associated intramolecular geometric structure changes are long completed, as is the solvent heating due to the initial energy dissipation from the excited HS molecule. Combining information from X-ray emission spectroscopy and scattering, the excitation fraction as well as the temperature and density changes of the solvent can be closely followed on the subnanosecond time scale of the HS lifetime, allowing the detection of an ultrafast change in bulk solvent density. An analysis approach directly utilizing the spectroscopic data in the XDS analysis effectively reduces the number of free parameters, and both combined permit extraction of information about the ultrafast structural dynamics of the caging solvent, in particular, a decrease in the number of water molecules in the first solvation shell is inferred, as predicted by recent theoretical work.

### Project A5

#### Roadmap of ultrafast x-ray atomic and molecular physics

*L. Young, K. Ueda, M. Gühr, P. H. Bucksbaum, M. Simon, S. Mukamel, N. Rohringer, K. C. Prince, C. Masciovecchio, M. Meyer, A. Rudenko, D. Rolles, C. Bostedt, M. Fuchs, D. A. Reis, R. Santra, H. Kapteyn, M. Murnane, H. Ibrahim, F. Légaré, et. al.*

X-ray free-electron lasers (XFELs) and table-top sources of x-rays based upon high harmonic generation (HHG) have revolutionized the field of ultrafast x-ray atomic and molecular physics, largely due to an explosive growth in capabilities in the past decade. XFELs now provide unprecedented intensity (1020 W cm−2) of x-rays at wavelengths down to ~1 Ångstrom, and HHG provides unprecedented time resolution (~50 attoseconds) and a correspondingly large coherent bandwidth at longer wavelengths. For context, timescales can be referenced to the Bohr orbital period in hydrogen atom of 150 attoseconds and the hydrogen-molecule vibrational period of 8 femtoseconds; wavelength scales can be referenced to the chemically significant carbon K-edge at a photon energy of ~280 eV (44 Ångstroms) and the bond length in methane of ~1 Ångstrom. With these modern x-ray sources one now has the ability to focus on individual atoms, even when embedded in a complex molecule, and view electronic and nuclear motion on their intrinsic scales (attoseconds and Ångstroms). These sources have enabled coherent diffractive imaging, where one can image non-crystalline objects in three dimensions on ultrafast timescales, potentially with atomic resolution. The unprecedented intensity available with XFELs has opened new fields of multiphoton and nonlinear x-ray physics where behavior of matter under extreme conditions can be explored. The unprecedented time resolution and pulse synchronization provided by HHG sources has kindled fundamental investigations of time delays in photoionization, charge migration in molecules, and dynamics near conical intersections that are foundational to AMO physics and chemistry. This roadmap coincides with the year when three new XFEL facilities, operating at Ångstrom wavelengths, opened for users (European XFEL, Swiss-FEL and PAL-FEL in Korea) almost doubling the present worldwide number of XFELs, and documents the remarkable progress in HHG capabilities since its discovery roughly 30 years ago, showcasing experiments in AMO physics and other applications. Here we capture the perspectives of 17 leading groups and organize the contributions into four categories: ultrafast molecular dynamics, multidimensional x-ray spectroscopies; high-intensity x-ray phenomena; attosecond x-ray science.

#### State-resolved attosecond reversible and irreversible dynamics in strong optical fields

*M. Sabbar, H. Timmer, Y. Chen, A. K. Pymer, Z. Loh, S. G. Sayres, S. Pabst, R. Santra, S. R. Leone*

Strong-field ionization (SFI) is a key process for accessing real-time quantum dynamics of electrons on the attosecond timescale. The theoretical foundation of SFI was pioneered in the 1960s, and later refined by various analytical models. While asymptotic ionization rates predicted by these models have been tested to be in reasonable agreement for a wide range of laser parameters, predictions for SFI on the sub-laser-cycle timescale are either beyond the scope of the models or show strong qualitative deviations from full quantum-mechanical simulations. Here, using the unprecedented state specificity of attosecond transient absorption spectroscopy, we follow the real-time SFI process of the two valence spin–orbit states of xenon. The results reveal that the irreversible tunnelling contribution is accompanied by a reversible electronic population that exhibits an observable spin–orbit-dependent phase delay. A detailed theoretical analysis attributes this observation to transient ground-state polarization, an unexpected facet of SFI that cannot be captured by existing analytical models that focus exclusively on the production of asymptotic electron/ion yields.

#### Time-dependent configuration-interaction-singles calculation of the 5p-subshell two-photon ionization cross section in xenon

*A. Karamatskou and R. Santra*

The 5p two-photon ionization cross section of xenon in the photon-energy range below the one-photon ionization threshold is calculated within the time-dependent configuration-interaction-singles (TDCIS) method. The TDCIS calculations are compared to random-phase-approximation calculations [Wendin et al., J. Opt. Soc. Am. B 4, 833 (1987)] and are found to reproduce the energy positions of the intermediate Rydberg states reasonably well. The effect of interchannel coupling is also investigated and found to change the cross section of the 5p shell only slightly compared to the intrachannel case.

#### Stability of the time-dependent configuration-interaction-singles method in the attosecond and strong-field regimes: A study of basis sets and absorption methods

*S. Pabst, A. Sytcheva, O. Geffert, R. Santra*

We investigate the behavior of several spatial grid methods and complex absorbers for strong-field and attosecond scenarios when using the time-dependent configuration-interaction singles method to solve the multi-electron time-dependent Schrödinger equation for atoms. We compare the pseudospectral grid, finite-element, and finite-element-discrete-variable-representation (DVR) methods with each other and discuss their advantages and disadvantages. Additionally, we study the performances of complex absorbing potential (CAP) and smooth exterior complex scaling (SES) to absorb the outgoing electron. We find that SES performs generally better than CAP for calculating high-harmonic generation spectra and XUV photoelectron spectra. In both of these cases, the DVR and even more the FEM grid representations show more reliable results—especially when using SES. Both absorbers show drawbacks when calculating photoelectron spectra in the strong-field regime.

#### Maximizing hole coherence in ultrafast photoionization of argon with an optimization by sequential parametrization update

*R. Esteban Goetz, M. Merkel, A. Karamatskou, R. Santra, C. P. Koch*

Photoionization with attosecond pulses populates hole states in the photoion. Superpositions of hole states represent ideal candidates for time-dependent spectroscopy, for example via pump-probe studies. The challenge consists in identifying pulses that create coherent superpositions of hole states while satisfying practical constraints. Here, we employ quantum optimal control to maximize the degree of coherence between these hole states. To this end, we introduce a derivative-free optimization method with sequential parametrization update (SPA optimization). We demonstrate the versatility and computational efficiency of SPA optimization for photoionization in argon by maximizing the coherence between the 3s and 3p0 hole states using shaped attosecond pulses. We show that it is possible to maximize the hole coherence while simultaneously prescribing the ratio of the final hole state populations.

#### Quantum optimal control of photoelectron spectra and angular distributions

*R. E. Goetz, A. Karamatskou, R. Santra, C. P. Koch*

Photoelectron spectra and photoelectron angular distributions obtained in photoionization reveal important information on, e.g., charge transfer or hole coherence in the parent ion. Here we show that optimal control of the underlying quantum dynamics can be used to enhance desired features in the photoelectron spectra and angular distributions. To this end, we combine Krotov's method for optimal control theory with the time-dependent configuration interaction singles formalism and a splitting approach to calculate photoelectron spectra and angular distributions. The optimization target can account for specific desired properties in the photoelectron angular distribution alone, in the photoelectron spectrum, or in both. We demonstrate the method for hydrogen and then apply it to argon under strong XUV radiation, maximizing the difference of emission into the upper and lower hemispheres, in order to realize directed electron emission in the XUV regime.

#### Multielectron dynamics in the tunneling ionization of correlated quantum systems

*M. Hollstein and D. Pfannkuche*

The importance of multielectron dynamics during the tunneling ionization of a correlated quantum system is investigated. By comparison of the solution of the time-dependent Schrödinger equation with the time-dependent configuration-interaction singles approach, we demonstrate the importance of a multielectron description of the tunneling ionization process especially for weakly confined quantum systems. Within this context, we observe that adiabatic driving by an intense light field can even enhance the correlations between still trapped electrons.

#### Wave-packet propagation based calculation of above-threshold ionization in the x-ray regime

*M. Tilley, A. Karamatskou, R. Santra*

We investigate the multi-photon process of above-threshold ionization for the light elements hydrogen, carbon, nitrogen, and oxygen in the hard x-ray regime. Numerical challenges are discussed and by comparing Hartree–Fock–Slater calculations with configuration–interaction–singles results we justify the mean-field potential approach in this regime. We present a theoretical prediction of two-photon above-threshold-ionization cross sections for the mentioned elements. Moreover, we study how the importance of above-threshold ionization varies with intensity. We find that for carbon, at x-ray intensities around ${{10}^{23}}\ {\rm W}\;{\rm c}{{{\rm m}}^{-2}}$, two-photon above-threshold ionization of the K-shell electrons is as probable as one-photon ionization of the L-shell electrons.

#### Theoretical characterization of the collective resonance states underlying the xenon giant dipole resonance

*Yi-Jen Chen (陳怡蓁), Stefan Pabst, Antonia Karamatskou, Robin Santra*

We present a detailed theoretical characterization of the two fundamental collective resonances underlying the xenon giant dipole resonance (GDR). This is achieved consistently by two complementary methods implemented within the framework of the configuration-interaction singles (CIS) theory. The first method accesses the resonance states by diagonalizing the many-electron Hamiltonian using the smooth exterior complex scaling technique. The second method involves a different application of the Gabor analysis to wave-packet dynamics. We identify one resonance at an excitation energy of 74 eV with a lifetime of 27 as and the second at 107eV with a lifetime of 11as. Our work provides a deeper understanding of the nature of the resonances associated with the GDR: a group of close-lying intrachannel resonances splits into two far-separated resonances through interchannel couplings involving the 4d electrons. The CIS approach allows a transparent interpretation of the two resonances as new collective modes. Due to the strong entanglement between the excited electron and the ionic core, the resonance wave functions are not dominated by any single particle-hole state. This gives rise to plasma-like collective oscillations of the 4d shell as a whole.

#### Spin–orbit effects in atomic high-harmonic generation

*S. Pabst, R. Santra*

Spin–orbit interactions lead to small energy gaps between the outermost p1/2 and p3/2 shells of noble gas atoms. Strong-field pulses tunnel-ionize an electron out of either shell resulting in spin–orbit-driven hole motion. These hole dynamics affect the high-harmonic generation (HHG) yield. However, the spectral shape as well as the angular distribution of the HHG emission is not influenced by spin–orbit coupling. We demonstrate the spin–orbit effect on atomic krypton by solving the multi-electron Schrödinger equation with the time-dependent configuration-interaction singles approach. We also provide pulse parameters where this effect can be identified in experiments through an enhancement in the HHG yield as the wavelength of the strong-field pulse increases.

#### Controlling the 2p hole alignment in neon via the 2s-3p Fano resonance

*E. Heinrich-Josties, S. Pabst, R. Santra*

We study the state-resolved production of neon ion after resonant photoionization of Ne via the 2s-3p Fano resonance. We find that by tuning the photon energy across the Fano resonance, a surprisingly high control over the alignment of the final 2p hole along the polarization direction can be achieved. In this way, hole alignments can be created that are otherwise very hard to achieve. The mechanism responsible for this hole alignment is the destructive interference of the direct and indirect (via the autoionizing 2s−13p state) ionization pathways of 2p. By changing the photon energy, the strength of the interference varies and 2p hole alignments with ratios up to 19:1 between 2p0 and 2p±1 holes can be created—an effect normally only encountered in tunnel ionization using strong-field ir pulses. The inclusion of spin-orbit interaction does not change the qualitative feature and leads only to a reduction in the alignment by 2/3. Our study is based on a time-dependent configuration-interaction singles approach, which solves the multichannel time-dependent Schrödinger equation.

#### Calculation of photoelectron spectra within the time-dependent configuration-interaction singles scheme

*A. Karamatskou, S. Pabst, Y.-J. Chen, R. Santra*

We present an extension of the time-dependent configuration-interaction singles (TDCIS) method to the computation of the electron kinetic-energy spectrum in photoionization processes. Especially for strong and long ionizing light pulses, the detection of the photoelectron poses a computational challenge because propagating the outgoing photoelectron wave packet requires large grid sizes. Two different methods that allow for the extraction of the asymptotic photoelectron momentum are compared regarding their methodological and computational performance. The first method follows the scheme of Tong et al. [X. M. Tong, K. Hino, and N. Toshima, Phys. Rev. A 74, 031405(R) (2006)], where the photoelectron wave function is absorbed by a real splitting function. The second method following that presented by Tao and Scrinzi [L. Tao and A. Scrinzi, New J. Phys. 14, 013021 (2012)], measures the flux of the electron wave packet through a surface at a fixed radius. With both methods the full angle- and energy-resolved photoelectron spectrum is obtained. Combined with the TDCIS scheme, it is possible to analyze the dynamics of the outgoing electron in a channel-resolved way and, additionally, to study the dynamics of the bound electrons in the parent ion. As an application, one-photon and above-threshold ionization of argon following strong XUV irradiation are studied via energy- and angle-resolved photoelectron spectra.

#### Introducing many-body physics using atomic spectroscopy

*D. Krebs, S. Pabst, R. Santra*

Atoms constitute relatively simple many-body systems, making them suitable objects for developing an understanding of basic aspects of many-body physics. Photoabsorption spectroscopy is a prominent method to study the electronic structure of atoms and the inherent many-body interactions. In this article, the impact of many-body effects on well-known spectroscopic features, such as Rydberg series, Fano resonances, Cooper minima, and giant resonances, is studied and related many-body phenomena in other fields are outlined. To calculate photoabsorption cross sections, the time-dependent configuration interaction singles (TDCIS) model is employed. The conceptual clearness of TDCIS in combination with the compactness of atomic systems allows for a pedagogical introduction to many-body phenomena.

#### Strong-Field Many-Body Physics and the Giant Enhancement in the High-Harmonic Spectrum of Xenon

*S. Pabst, R. Santra*

We resolve an open question about the origin of the giant enhancement in the high-harmonic generation spectrum of atomic xenon around 100 eV. By solving the many-body time-dependent Schrödinger equation with all 4d, 5s, and 5p orbitals active, we truly demonstrate the enhancement results from the collective many-body excitation induced by the returning photoelectron via two-body interchannel interactions. Without the many-body interactions, which promote a 4d electron into the 5p vacancy created by strong-field ionization, no collective excitation and no enhancement in the high-harmonic generation spectrum exist.

#### Atomic and molecular dynamics triggered by ultrashort light pulses on the atto- to picosecond time scale

*S. Pabst*

Time-resolved investigations of ultrafast electronic and molecular dynamics were not possible until recently. The typical time scale of these processes is in the picosecond to attosecond realm. The tremendous technological progress in recent years made it possible to generate ultrashort pulses, which can be used to trigger, to watch, and to control atomic and molecular motion. This tutorial focuses on experimental and theoretical advances which are used to study the dynamics of electrons and molecules in the presence of ultrashort pulses. In the first part, the rotational dynamics of molecules, which happens on picosecond and femtosecond time scales, is reviewed. Well-aligned molecules are particularly suitable for angle-dependent investigations like x-ray diffraction or strong-field ionization experiments. In the second part, the ionization dynamics of atoms is studied. The characteristic time scale lies, here, in the attosecond to few-femtosecond regime. Although a one-particle picture has been successfully applied to many processes, many-body effects do constantly occur. After a broad overview of the main mechanisms and the most common tools in attosecond physics, examples of many-body dynamics in the attosecond world (e.g., in high-harmonic generation and attosecond transient absorption spectroscopy) are discussed.

#### Adiabaticity and diabaticity in strong-field ionization

*A. Karamatskou, S. Pabst, R. Santra*

If the photon energy is much less than the electron binding energy, ionization of an atom by a strong optical field is often described in terms of electron tunneling through the potential barrier resulting from the superposition of the atomic potential and the potential associated with the instantaneous electric component of the optical field. In the strict tunneling regime, the electron response to the optical field is said to be adiabatic, and nonadiabatic effects are assumed to be negligible. Here, we investigate to what degree this terminology is consistent with a language based on the so-called adiabatic representation. This representation is commonly used in various fields of physics. For electronically bound states, the adiabatic representation yields discrete potential-energy curves that are connected by nonadiabatic transitions. When applying the adiabatic representation to optical strong-field ionization, a conceptual challenge is that the eigenstates of the instantaneous Hamiltonian form a continuum; i.e., there are no discrete adiabatic states. This difficulty can be overcome by applying an analytic-continuation technique. In this way, we obtain a rigorous classification of adiabatic states and a clear characterization of (non)adiabatic and (non)diabatic ionization dynamics. Moreover, we distinguish two different regimes within tunneling ionization and explain the dependence of the ionization probability on the pulse envelope.

#### Real time tracing of valence-shell electronic coherences with attosecond transient absorption spectroscopy

*A. Wirth, R. Santra, E. Goulielmakis*

The chemical properties of atoms, molecules and of more complex systems such as clusters, nanoparticles or condensed matter systems are determined by valence electrons. Real-time control of these properties requires the capability of tracing as well as of driving valence electrons on their native temporal scale of motion, that is, within tens to thousands of attoseconds. Here we detail the technique of attosecond transient absorption spectroscopy. It combines the extreme sensitivity of core-level spectroscopy with the unprecedented temporal resolution offered by the tools of attosecond technology. We use the technique to demonstrate real-time tracing and complete characterization of coherent electron motion triggered by single, double or multiple ionization of atoms exposed to intense, few-cycle pulses. Our work opens the door to high fidelity, time-domain studies and control of electron dynamics in the microcosm.

#### Real time tracing of valence-shell electronic coherences with attosecond transient absorption spectroscopy

*A. Wirth, R. Santra, E. Goulielmakis*

The chemical properties of atoms, molecules and of more complex systems such as clusters, nanoparticles or condensed matter systems are determined by valence electrons. Real-time control of these properties requires the capability of tracing as well as of driving valence electrons on their native temporal scale of motion, that is, within tens to thousands of attoseconds. Here we detail the technique of attosecond transient absorption spectroscopy. It combines the extreme sensitivity of core-level spectroscopy with the unprecedented temporal resolution offered by the tools of attosecond technology. We use the technique to demonstrate real-time tracing and complete characterization of coherent electron motion triggered by single, double or multiple ionization of atoms exposed to intense, few-cycle pulses. Our work opens the door to high fidelity, time-domain studies and control of electron dynamics in the microcosm.

#### Theory of attosecond transient-absorption spectroscopy of krypton for overlapping pump and probe pulses

*S. Pabst, A. Sytcheva, A. Moulet, A. Wirth, E. Goulielmakis, R. Santra*

We present a fully ab initio calculations for attosecond transient absorption spectroscopy of atomic krypton with overlapping pump and probe pulses. Within the time-dependent configuration interaction singles (TDCIS) approach, we describe the pump step (strong-field ionization using a near-infrared pulse) as well as the probe step (resonant electron excitation using an extreme-ultraviolet pulse) from first principles. We extend our TDCIS model and account for the spin-orbit splitting of the occupied orbitals. We discuss the spectral features seen in a recent attosecond transient absorption experiment [ A. Wirth et al. Science 334 195 (2011)]. Our results support the concept that the transient absorption signal can be directly related to the instantaneous hole population even during the ionizing pump pulse. Furthermore, we find strong deformations in the absorption lines when the overlap of pump and probe pulses is maximum. These deformations can be described by relative phase shifts in the oscillating ionic dipole. We discuss possible mechanisms contributing to these phase shifts. Our finding suggests that the nonperturbative laser dressing of the entire N-electron wave function is the main contributor.

#### Impact of multichannel and multipole effects on the Cooper minimum in the high-order-harmonic spectrum of argon

*S. Pabst, L. Greenman, D. A. Mazziotti, R. Santra*

We investigate the relevance of multiple-orbital and multipole effects during high-harmonic generation (HHG). The time-dependent configuration interaction singles (TDCIS) approach is used to study the impact of the detailed description of the residual electron-ion interaction on the HHG spectrum. We find that the shape and position of the Cooper minimum in the HHG spectrum of argon changes significantly whether or not interchannel interactions are taken into account. The HHG yield can be underestimated by up to 2 orders of magnitude in the energy region of 30–50 eV. We show that the argument of low ionization probability is not sufficient to justify ignoring multiple-orbital contributions. Additionally, we find the HHG yield is sensitive to the nonspherical multipole character of the electron-ion interaction.

### Project A6

#### Observation of topological Bloch-state defects and their merging transition

*M. Tarnowski, M. Nuske, N. Fläschner, B. Rem, D. Vogel, L. Freystatzky, K. Sengstock, L. Mathey, C. Weitenberg*

Topological defects in Bloch bands, such as Dirac points in graphene, and their resulting Berry phases play an important role for the electronic dynamics in solid state crystals. Such defects can arise in systems with a two-atomic basis due to the momentum-dependent coupling of the two sublattice states, which gives rise to a pseudo-spin texture. The topological defects appear as vortices in the azimuthal phase of this pseudo-spin texture. Here, we demonstrate a complete measurement of the azimuthal phase in a hexagonal optical lattice

employing a versatile method based on time-of-flight imaging after off-resonant lattice modulation. Furthermore we map out the merging transition of the two Dirac points induced by beam imbalance. Our work paves the way to accessing geometric properties in general multi-band systems also with spin-orbit coupling and interactions.

Phys. Rev. Lett. 118, 240403 (2017)

https://arxiv.org/abs/1703.02813

#### Emulating molecular orbitals and electronic dynamics with ultracold atoms

*D.-S. Lühmann, C. Weitenberg, K. Sengstock*

In the recent years, ultracold atoms in optical lattices have proven their great value as quantum simulators for studying strongly-correlated phases and complex phenomena in solid-state systems. Here we reveal their potential as quantum simulators for molecular physics and propose a technique to image the three-dimensional molecular orbitals with high resolution. The outstanding tunability of ultracold atoms in terms of potential and interaction offer fully-adjustable model systems for gaining deep insight into the electronic structure of molecules. We study the orbitals of an artificial benzene molecule and discuss the effect of tunable interactions in its conjugated pi electron system with special regard to localization and spin order. The dynamical timescale of ultracold atom simulators are on the order milliseconds which allow for the time-resolved monitoring of a broad range of dynamical processes. As an example, we compute the hole dynamics in the conjugated pi system of the artificial benzene molecule.

## Project B

### Project B1

#### Trace phase detection and strain characterization from serial X-rayfree-electron laser crystallography of a Pr0.5 Ca0.5 MnO3 powder

*K. R. Beyerlein, C. Jooss, A. Barty, R. Bean, S. Boutet, S. S. Dhesi, R. Bruce Doak, M. Först, L. Galli, R. A. Kirian, J. Kozak, M. Lang, R. Mankowsky, A. Cavalleri, H. Chapman, et. al*

We report on the analysis of virtual powder-diffraction patterns from serial femtosecond crystallography (SFX) data collected at an X-ray free-electron laser. Different approaches to binning and normalizing these patterns are discussed with respect to the microstructural characteristics which each highlights. Analysis of SFX data from a powder of Pr0.5Ca0.5MnO3 in this way finds evidence of other trace phases in its microstructure which was not detectable in a standard powder-diffraction measurement. Furthermore, a comparison between two virtual powder pattern integration strategies is shown to yield different diffraction peak broadening, indicating sensitivity to different types of microstrain. This paper is a first step in developing new data analysis methods for microstructure characterization from serial crystallography data.

#### Driving Magnetic Order in a Manganite by Ultrafast Lattice Excitation

*M. Foerst, R.I. Tobey, S. Wall, H. Bromberger, V. Khanna, A.L. Cavalieri, Y.D. Chuang, W.S. Lee, R. Moore, W.F. Schlotter, J.J. Turner, O. Krupin, M. Trigo, H. Zheng, J.F. Mitchell, S.S. Dhesi, J.P. Hill, A. Cavalleri*

Femtosecond midinfrared pulses are used to directly excite the lattice of the single-layer manganite La0.5Sr1.5MnO4. Magnetic and orbital orders, as measured by femtosecond resonant soft x-ray diffraction with an x-ray free-electron laser, are reduced within a few picoseconds. This effect is interpreted as a displacive exchange quench, a prompt shift in the equilibrium value of the magnetic- and orbital-order parameters after the lattice has been distorted. Control of magnetism through ultrafast lattice excitation may be of use for high-speed optomagnetism.

#### Polaronic conductivity in the photoinduced phase of 1T-TaS2

*N. Dean, J. C. Petersen, D. Fausti, R. I. Tobey, S. Kaiser, L. V. Gasparov, H. Berger, A. Cavalleri*

The transient optical conductivity of photoexcited 1T-TaS2 is determined over a three-order-of-magnitude frequency range. Prompt collapse and recovery of the Mott gap is observed. However, we find important differences between this transient metallic state and that seen across the thermally driven insulator-metal transition. Suppressed low-frequency conductivity, Fano phonon line shapes, and a midinfrared absorption band point to polaronic transport. This is explained by noting that the photoinduced metallic state of 1T-TaS2 is one in which the Mott gap is melted but the lattice retains its low-temperature symmetry, a regime only accessible by photodoping.

#### Clocking the melting transition of charge and lattice order in 1T-TaS 2 with ultrafast extreme-ultraviolet angle-resolved photoemission spectroscopy

*J.C. Petersen, S. Kaiser, N. Dean, A. Simoncig, H. Y. Liu, A. L. Cavalieri, C. Cacho, I.C.E. Turcu, E. Springate, F. Frassetto, L. Poletto, S. S. Dhesi, H. Berger, A. Cavalleri*

We use time- and angle-resolved photoemission spectroscopy with sub-30-fs extreme-ultraviolet pulses to map the time- and momentum-dependent electronic structure of photoexcited 1T-TaS2. This compound is a two-dimensional Mott insulator with charge-density wave ordering. Charge order, evidenced by splitting between occupied subbands at the Brillouin zone boundary, melts well before the lattice responds. This challenges the view of a charge-density wave caused by electron-phonon coupling and Fermi-surface nesting alone, and suggests that electronic correlations play a key role in driving charge order.

#### Melting of antiferromagnetic order in La0.5Sr1.5MnO4 probed with ultrafast resonant soft X-ray diffraction

*H. Ehrke, R.I. Tobey, S. Wall, S. A. Cavill, M. Först, V. Khanna, Th. Garl, N. Stojanovic, D. Prabhakaran, A.T. Boothroyd, M. Gensch, A. Mirone, P. Reutler, A. Revcolevschi, S. S. Dhesi, A. Cavalleri*

We used ultrafast resonant soft x-ray diffraction to probe the picosecond dynamics of spin and orbital order in La0.5Sr1.5MnO4 after photoexcitation with a femtosecond pulse of 1.5 eV radiation. Complete melting of antiferromagnetic spin order is evidenced by the disappearance of a (1/4,1/4,1/2) diffraction peak. On the other hand, the (1/4,1/4,0) diffraction peak, reflecting orbital order, is only partially reduced. We interpret the results as evidence of destabilization in the short-range exchange pattern with no significant relaxation of the long-range Jahn-Teller distortions. Cluster calculations are used to analyze different possible magnetically ordered states in the long-lived metastable phase. Nonthermal coupling between light and magnetism emerges as a primary aspect of photoinduced phase transitions in manganites.

#### Bidirectional ultrafast electric field gating of interlayer transport in a cuprate superconductor

*A. Dienst, M. Hoffman, J. Petersen, S. Pyon, T. Takayama, H. Takagi, A. Cavalleri*

In cuprate superconductors, tunnelling between planes makes three-dimensional superconductive transport possible. However, the interlayer tunnelling amplitude is reduced when an order-parameter-phase gradient between planes is established. As such, interlayer superconductivity along the c-axis can be weakened if a strong electric field is applied along the c-axis. In this Letter, we use high-field single-cycle terahertz pulses to gate interlayer coupling in La1.84Sr0.16CuO4. We induce ultrafast oscillations between superconducting and resistive states and switch the plasmon response on and off, without reducing the density of Cooper pairs. In-plane superconductivity remains unperturbed, revealing a non-equilibrium state in which the dimensionality of the superconductivity is time-dependent. The gating frequency is determined by the electric field strength. Non-dissipative, bi-directional gating of superconductivity is of interest for device applications in ultrafast nanoelectronics and represents an example of how nonlinear terahertz physics can benefit nanoplasmonics and active metamaterials.

#### Nonlinear phononics as an ultrafast route to lattice control

*M. Foerst, Ch. Manzoni, S. Kaiser, Y. Tokura, Y. Tomioka, R. Merlin, A. Cavalleri*

Two types of coupling between electromagnetic radiation and a crystal lattice have so far been identified experimentally. The first is the direct coupling of light to infrared-active vibrations carrying an electric dipole. The second is indirect, involving electron–phonon coupling and occurring through excitation of the electronic system; stimulated Raman scattering1, 2, 3 is one example. A third path, ionic Raman scattering (IRS; refs 4, 5), was proposed 40 years ago. It was posited that excitation of an infrared-active phonon could serve as the intermediate state for Raman scattering, a process that relies on lattice anharmonicities rather than electron–phonon interactions6. Here, we report an experimental demonstration of IRS using femtosecond excitation and coherent detection of the lattice response. We show how this mechanism is relevant to ultrafast optical control in solids: a rectified phonon field can exert a directional force onto the crystal, inducing an abrupt displacement of the atoms from their equilibrium positions. IRS opens up a new direction for the optical control of solids in their electronic ground state7, 8, 9, different from carrier excitation.

#### Moving the Frontier of Quantum Control into the Soft X-Ray Spectrum

*A. Aquila, M. Drescher, T. Laarmann, M. Barthelmeß, H. N. Chapman, S. Bajt*

International Journal of Optics Volume 2011 (2011), Article ID 417075

### Project B2

#### The role of space charge in spin-resolved photoemission experiments

*A. Fognini, G. Salvatella, T.U. Michlmayr, C. Wetli, U. Ramsperger, T. Bähler, F. Sorgenfrei, M. Beye, A. Eschenlohr, N. Pontius, C. Stamm, F. Hieke, M. Dell‘Angela, S. de Jong, R. Kukreja, N. Gerasimova, V. Rybnikov, H. Redlin, J. Raabe, W. Wurth et.*

Spin-resolved photoemission is one of the most direct ways of measuring the magnetization of a ferromagnet. If all valence band electrons contribute, the measured average spin polarization is proportional to the magnetization. This is even the case if electronic excitations are present, and thus is of particular interest for studying the response of the magnetization to a pump laser pulse. Here, we demonstrate the feasibility of ultrafast spin-resolved photoemission using free electron laser (FEL) radiation and investigate the effect of space charge on the detected spin polarization. The sample is exposed to the radiation of the FEL FLASH in Hamburg. Surprisingly, the measured spin polarization depends on the fluence of the FEL radiation: a higher FEL fluence reduces the measured spin polarization. Space-charge simulations can explain this effect. These findings have consequences for future spin-polarized photoemission experiments using pulsed photon sources.

#### Ultrafast reduction of the total magnetization in iron

*A. Fognini, T. U. Michlmayr, G. Salvatella, C. Wetli, U. Ramsperger, T. Bähler, F.Sorgenfrei, M. Beye, A. Eschenlohr, N. Pontius, C. Stamm, F. Hieke, M. Dell'Angela, S. de Jong, R. Kukreja, N. Gerasimova, V. Rybnikov, H. Redlin, W. Wurth, et. al*

Surprisingly, if a ferromagnet is exposed to an ultrafast laser pulse, its apparent magnetization is reduced within less than a picosecond. Up to now, the total magnetization, i.e., the average spin polarization of the whole valence band, was not detectable on a sub-picosecond time scale. Here, we present experimental data, confirming the ultrafast reduction of the total magnetization. Soft x-ray pulses from the free electron laser in Hamburg (FLASH) extract polarized cascade photoelectrons from an iron layer excited by a femtosecond laser pulse. The spin polarization of the emitted electrons is detected by a Mott spin polarimeter.

#### Speed limit of the insulator metal-transition in magnetite

*S. de Jong, R. Kukreja, C. Trabant, N. Pontius, C.F. Chang, T. Kachel, M. Beye, F. Sorgenfrei, C. H. Back, B. Bräuer, W.F. Schlotter, J.J. Turner, O. Krupin, M. Doehler, D. Zhu, M.A. Hossain, W. Wurth, D. Fausti, F. Novelli, M. Esposito, et. al*

As the oldest known magnetic material, magnetite (Fe3O4) has fascinated mankind for millennia. As the first oxide in which a relationship between electrical conductivity and fluctuating/localized electronic order was shown, magnetite represents a model system for understanding correlated oxides in general. Nevertheless, the exact mechanism of the insulator–metal, or Verwey, transition has long remained inaccessible. Recently, three-Fe-site lattice distortions called trimerons were identified as the characteristic building blocks of the low-temperature insulating electronically ordered phase9. Here we investigate the Verwey transition with pump–probe X-ray diffraction and optical reflectivity techniques, and show how trimerons become mobile across the insulator–metal transition. We find this to be a two-step process. After an initial 300 fs destruction of individual trimerons, phase separation occurs on a 1.5±0.2 ps timescale to yield residual insulating and metallic regions. This work establishes the speed limit for switching in future oxide electronics.

### Project B3

#### Employing soft x-ray resonant magnetic scattering to study domain sizes and anisotropy in Co/Pd multilayers

*K. Bagschik, R. Frömter, J. Bach, B. Beyersdorff, L. Müller, S. Schleitzer, M. Hårdensson Berntsen, C. Weier, R. Adam, J. Viefhaus, C. M. Schneider, G. Grübel, H. P. Oepen*

It is demonstrated that the magnetic diffraction pattern of the isotropic disordered maze pattern is well described utilizing a gamma distribution of domain sizes in a one-dimensional model. From the analysis, the mean domain size and the shape parameter of the distribution are obtained. The model reveals an average domain size that is significantly different from the value that is determined from the peak position of the structure factor in reciprocal space. As a proof of principle, a wedge-shaped (CotÅ/Pd10Å)8 multilayer film, that covers the thickness range of the spin-reorientation transition, has been used. By means of soft x-ray resonant magnetic scattering (XRMS) and imaging techniques the thickness-driven evolution of the magnetic properties of the cobalt layers is explored. It is shown that minute changes of the domain pattern concerning domain size and geometry can be investigated and analyzed due to the high sensitivity and lateral resolution of the XRMS technique. The latter allows for the determination of the magnetic anisotropies of the cobalt layers within a thickness range of a few angstroms.

#### Spatial coherence determination from the Fourier analysis of a resonant soft X-ray magnetic speckle pattern

*K. Bagschik, R. Frömter, L. Müller, W. Roseker, J. Bach, P. Staeck, C. Thönnißen, S. Schleitzer, M. H. Berntsen, C. Weier, R. Adam, J. Viefhaus, C. M. Schneider, G. Grübel, H. P. Oepen*

We present a method to determine the two-dimensional spatial coherence of synchrotron radiation in the soft X-ray regime by analyzing the Fourier transform of the magnetic speckle pattern from a ferromagnetic film in a multidomain state. To corroborate the results, a Young’s double-pinhole experiment has been performed. The transverse coherence lengths in vertical and horizontal direction of both approaches are in a good agreement. The method presented here is simple and gives a direct access to the coherence properties of synchrotron radiation without nanostructured test objects.

#### Indirect excitation of ultrafast demagnetization

*B. Vodungbo, et.al.*

Does the excitation of ultrafast magnetization require direct interaction between the photons of the optical pump pulse and the magnetic layer? Here, we demonstrate unambiguously that this is not the case. For this we have studied the magnetization dynamics of a ferromagnetic cobalt/palladium multilayer capped by an IR-opaque aluminum layer. Upon excitation with an intense femtosecond-short IR laser pulse, the film exhibits the classical ultrafast demagnetization phenomenon although only a negligible number of IR photons penetrate the aluminum layer. In comparison with an uncapped cobalt/palladium reference film, the initial demagnetization of the capped film occurs with a delayed onset and at a slower rate. Both observations are qualitatively in line with energy transport from the aluminum layer into the underlying magnetic film by the excited, hot electrons of the aluminum film. Our data thus confirm recent theoretical predictions.

#### Characterization of spatial coherence of synchrotron radiation with non-redundant arrays of apertures

*P. Skopintsev, A. Singer, J. Bach, L. Müller, B. Beyersdorff, S. Schleitzer, O. Gorobtsov, A. Shabalin, R. P. Kurta, D. Dzhigaev, O. M. Yefanov, L. Glaser, A. Sakdinawat, G. Grübel, R. Frömter, H. P. Oepen, J. Viefhaus, I. A. Vartanyants*

A method to characterize the spatial coherence of soft X-ray radiation from a single diffraction pattern is presented. The technique is based on scattering from non-redundant arrays (NRAs) of slits and records the degree of spatial coherence at several relative separations from 1 to 15 µm, simultaneously. Using NRAs the spatial coherence of the X-ray beam at the XUV X-ray beamline P04 of the PETRA III synchrotron storage ring was measured as a function of different beam parameters. To verify the results obtained with the NRAs, additional Young's double-pinhole experiments were conducted and showed good agreement.

#### Imaging Ultrafast Demagnetization Dynamics after a Spatially Localized Optical Excitation

*C. von Korff Schmising, B. Pfau, M. Schneider, C. M. Günther, M. Giovannella, J. Perron, B. Vodungbo, L. Müller, F. Capotondi, E. Pedersoli, N. Mahne, J. Lüning, S. Eisebitt*

Ultrashort, coherent x-ray pulses of a free-electron laser are used to holographically image the magnetization dynamics within a magnetic domain pattern after creation of a localized excitation via an optical standing wave. We observe a spatially confined reduction of the magnetization within a couple of hundred femtoseconds followed by its slower recovery. Additionally, the experimental results show evidence of a spatial evolution of magnetization, which we attribute to ultrafast transport of nonequilibrium spin-polarized electrons for early times and to a fluence-dependent remagnetization rate for later times.

#### Endstation for ultrafast magnetic scattering experiments at the free-electron laser in Hamburg

*L. Müller, C. Gutt, S. Streit-Nierobisch, M. Walther, S. Schaffert, B. Pfau, J. Geilhufe, F. Büttner, S. Flewett, C. M. Günther, S. Eisebitt, A. Kobs, M. Hille, D. Stickler, R. Frömter, H. P. Oepen, J. Lüning, G. Grübel*

An endstation for pump–probe small-angle X-ray scattering (SAXS) experiments at the free-electron laser in Hamburg (FLASH) is presented. The endstation houses a solid-state absorber, optical incoupling for pump–probe experiments, time zero measurement, sample chamber, and detection unit. It can be used at all FLASH beamlines in the whole photon energy range offered by FLASH. The capabilities of the setup are demonstrated by showing the results of resonant magnetic SAXS measurements on cobalt-platinum multilayer samples grown on freestanding Si3N4 membranes and pump-laser-induced grid structures in multilayer samples.

#### Invited Article: Coherent imaging using seeded free-electron laser pulses with variable polarization: First results and research opportunities

*F. Capotondi, E. Pedersoli, N. Mahne, R. H. Menk, G. Passos, L. Raimondi, C. Svetina, G. Sandrin, M. Zangrando, M. Kiskinova, S. Bajt, M. Barthelmess, H. Fleckenstein, H. N. Chapman, J. Schulz, S. Schleitzer, L. Müller, C. Gutt, G. Grübel, et. al*

FERMI@Elettra, the first vacuum ultraviolet and soft X-ray free-electron laser (FEL) using by default a “seeded” scheme, became operational in 2011 and has been opened to users since December 2012. The parameters of the seeded FERMI FEL pulses and, in particular, the superior control of emitted radiation in terms of spectral purity and stability meet the stringent requirements for single-shot and resonant coherent diffraction imaging (CDI) experiments. The advantages of the intense seeded FERMI pulses with variable polarization have been demonstrated with the first experiments performed using the multipurpose experimental station operated at the diffraction and projection imaging (DiProI) beamline. The results reported here were obtained with fixed non-periodic targets during the commissioning period in 2012 using 20–32 nm wavelength range. They demonstrate that the performance of the FERMI FEL source and the experimental station meets the requirements of CDI, holography, and resonant magnetic scattering in both multi- and single-shot modes. Moreover, we present the first magnetic scattering experiments employing the fully circularly polarized FERMI pulses. The ongoing developments aim at pushing the lateral resolution by using shorter wavelengths provided by double-stage cascaded FERMI FEL-2 and probing ultrafast dynamic processes using different pump-probe schemes, including jitter-free seed laser pump or FEL-pump/FEL-probe with two color FEL pulses generated by the same electron bunch.

#### Breakdown of the X-Ray Resonant Magnetic Scattering Signal during Intense Pulses of Extreme Ultraviolet Free-Electron-Laser Radiation

*L. Müller, C. Gutt, B. Pfau, S. Schaffert, J. Geilhufe, F. Büttner, J. Mohanty, S. Flewett, R. Treusch, S. Düsterer, H. Redlin, A. Al-Shemmary, M. Hille, A. Kobs, R. Frömter, H. P. Oepen, B. Ziaja, N. Medvedev, S.-K. Son, R. Thiele, R. Santra, et. al.*

We present results of single-shot resonant magnetic scattering experiments of Co/Pt multilayer systems using 100 fs long ultraintense pulses from an extreme ultraviolet (XUV) free-electron laser. An x-ray-induced breakdown of the resonant magnetic scattering channel during the pulse duration is observed at fluences of 5 J/cm2. Simultaneously, the speckle contrast of the high-fluence scattering pattern is significantly reduced. We performed simulations of the nonequilibrium evolution of the Co/Pt multilayer system during the XUV pulse duration. We find that the electronic state of the sample is strongly perturbed during the first few femtoseconds of exposure leading to an ultrafast quenching of the resonant magnetic scattering mechanism.

#### Nanoscale spin reversal by non-local angular momentum transfer following ultrafast laser excitation in ferrimagnetic GdFeCo

*C. E. Graves, A. H. Reid, T. Wang, B. Wu, S. de Jong, K. Vahaplar, I. Radu, D. P. Bernstein, M. Messerschmidt, L. Müller, R. Coffee, M. Bionta, S. W. Epp, R. Hartmann, N. Kimmel, et. al.*

Ultrafast laser techniques have revealed extraordinary spin dynamics in magnetic materials that equilibrium descriptions of magnetism cannot explain. Particularly important for future applications is understanding non-equilibrium spin dynamics following laser excitation on the nanoscale, yet the limited spatial resolution of optical laser techniques has impeded such nanoscale studies. Here we present ultrafast diffraction experiments with an X-ray laser that probes the nanoscale spin dynamics following optical laser excitation in the ferrimagnetic alloy GdFeCo, which exhibits macroscopic all-optical switching. Our study reveals that GdFeCo displays nanoscale chemical and magnetic inhomogeneities that affect the spin dynamics. In particular, we observe Gd spin reversal in Gd-rich nanoregions within the first picosecond driven by the non-local transfer of angular momentum from larger adjacent Fe-rich nanoregions. These results suggest that a magnetic material’s microstructure can be engineered to control transient laser-excited spins, potentially allowing faster (~ 1 ps) spin reversal than in present technologies.

#### Ultrafast optical demagnetization manipulates nanoscale spin structure in domain walls

*B. Pfau, S. Schaffert, L. Müller, C. Gutt, A. Al-Shemmary, F. Büttner, R. Delaunay, S. Düsterer, S. Flewett, R. Frömter, J. Geilhufe, E. Guehrs, C.M. Günther, R. Hawaldar, M. Hille, N. Jaouen, A. Kobs, K. Li, J. Mohanty, H. Redlin et. al*

During ultrafast demagnetization of a magnetically ordered solid, angular momentum has to be transferred between the spins, electrons, and phonons in the system on femto- and picosecond timescales. Although the intrinsic spin-transfer mechanisms are intensely debated, additional extrinsic mechanisms arising due to nanoscale heterogeneity have only recently entered the discussion. Here we use femtosecond X-ray pulses from a free-electron laser to study thin film samples with magnetic domain patterns. We observe an infrared-pump-induced change of the spin structure within the domain walls on the sub-picosecond timescale. This domain-topography-dependent contribution connects the intrinsic demagnetization process in each domain with spin-transport processes across the domain walls, demonstrating the importance of spin-dependent electron transport between differently magnetized regions as an ultrafast demagnetization channel. This pathway exists independent from structural inhomogeneities such as chemical interfaces, and gives rise to an ultrafast spatially varying response to optical pump pulses.

#### Femtosecond Single-Shot Imaging of Nanoscale Ferromagnetic Order in Co/Pd Multilayers Using Resonant X-Ray Holography

*Tianhan Wang et al.*

### Project B4

#### Nonequilibrium self-energy functional approach to the dynamical Mott transition

*F. Hofmann, M. Eckstein, M. Potthoff*

The real-time dynamics of the Fermi-Hubbard model, driven out of equilibrium by quenching or ramping the interaction parameter, is studied within the framework of the nonequilibrium self-energy functional theory. A dynamical impurity approximation with a single auxiliary bath site is considered as a reference system and the time-dependent hybridization is optimized as prescribed by the variational principle. The dynamical two-site approximation turns out to be useful to study the real-time dynamics on short and intermediate time scales. Depending on the strength of the interaction in the final state, two qualitatively different response regimes are found. For both weak and strong couplings, qualitative agreement with previous results of nonequilibrium dynamical mean-field theory is found. The two regimes are sharply separated by a critical point at which the low-energy bath degree of freedom decouples in the course of time. We trace the dependence of the critical interaction of the dynamical Mott transition on the duration of the interaction ramp from sudden quenches to adiabatic dynamics, and therewith link the dynamical to the equilibrium Mott transition.

#### Non-equilibrium variational-cluster approach to real-time dynamics in the Fermi-Hubbard model

*Felix Hofmann, Martin Eckstein, Michael Potthoff*

The non-equilibrium variational-cluster approach is applied to study the real-time dynamics of the double occupancy in the one-dimensional Fermi-Hubbard model after different fast changes of hopping parameters. A simple reference system, consisting of isolated Hubbard dimers, is used to discuss different aspects of the numerical implementation of the approach in the general framework of non-equilibrium self-energy functional theory. Opposed to a direct solution of the Euler equation, its time derivative is found to serve as numerically tractable and stable conditional equation to fix the time-dependent variational parameters.

Journal of Physics: Conference Series, Volume 696, conference 1

#### Large-amplitude spin oscillations triggered by nonequilibrium strongly correlated t2g electrons

*M. Behrmann, F. Lechermann*

Laser-induced ultrafast (fs) magnetization experiments in antiferromagnets have recently attracted large attention, paving the road for inherently fast spin dynamics in the THz regime without invoking stray fields. The technical importance is emphasized by the rising new research field of antiferromagnetic (AFM) spintronics, where superexchange-dominated strongly correlated compounds provide an interesting materials playground. An intriguing question is whether the Coulomb interaction may be a key to control AFM order on ultrafast time scales. Therefore, we study (de)magnetization processes in a time-dependent multiorbital Hubbard model, focusing on t2g electrons in a wider doping range. Depending on filling, we reveal large-amplitude spin oscillations via interaction quenches from the antiferromagnetic or paramagnetic state. Nonequilibrium ultrafast spin-orientation effects in prominent correlated transition-metal oxides are therefrom predicted.

#### Fermi Condensation Near van Hove Singularities Within the Hubbard Model on the Triangular Lattice

*D. Yudin, D. Hirschmeier, H. Hafermann, O. Eriksson, A. I. Lichtenstein, M. I. Katsnelson*

The proximity of the Fermi surface to van Hove singularities drastically enhances interaction effects and leads to essentially new physics. In this work we address the formation of flat bands (“Fermi condensation”) within the Hubbard model on the triangular lattice and provide a detailed analysis from an analytical and numerical perspective. To describe the effect we consider both weak-coupling and strong-coupling approaches, namely the renormalization group and dual fermion methods. It is shown that the band flattening is driven by correlations and is well pronounced even at sufficiently high temperatures, of the order of 0.1–0.2 of the hopping parameter. The effect can therefore be probed in experiments with ultracold fermions in optical lattices.

#### Extended dynamic Mott transition in the two-band Hubbard model out of equilibrium

*M. Behrmann, M. Fabrizio, F. Lechermann*

#### Non-equilibrium magnetic interactions in strongly correlated systems

*A. Secchi, S. Brener, A. I. Lichtenstein, M. I. Katsnelson*

We formulate a low-energy theory for the magnetic interactions between electrons in the multi-band Hubbard model under non-equilibrium conditions determined by an external time-dependent electric field which simulates laser-induced spin dynamics. We derive expressions for dynamical exchange parameters in terms of non-equilibrium electronic Green functions and self-energies, which can be computed, e.g., with the methods of time-dependent dynamical mean-field theory. Moreover, we find that a correct description of the system requires, in addition to exchange, a new kind of magnetic interaction, that we name twist exchange, which formally resembles Dzyaloshinskii–Moriya coupling, but is not due to spin–orbit, and is actually due to an effective three-spin interaction. Our theory allows the evaluation of the related time-dependent parameters as well.

#### Competing orders in Na_xCoO_2 from strong correlations on a two-particle level

*L. Boehnke, F. Lechermann*

Based on dynamical mean-field theory with a continuous-time quantum Monte-Carlo impurity solver, static as well as dynamic spin and charge susceptibilites for the phase diagram of the sodium cobaltate system Na$_x$CoO$_2$ are discussed. The approach includes important vertex contributions to the q-dependent two-particle response functions by means of a local approximation to the irreducible vertex function in the particle-hole channel. A single-band Hubbard model suffices to reveal several charge- and spin-instability tendencies in accordance with experiment, including the stabilization of an effective kagome sublattice close to x=0.67, without invoking the doping-dependent Na-potential landscape. The in-plane antiferromagnetic-to-ferromagnetic crossover is additionally verified by means of the computed Korringa ratio. Moreover an intricate high-energy mode in the transverse spin susceptiblity is revealed, pointing towards a strong energy dependence of the effective intersite exchange.

Phys. Rev. B 85, 115128 (2012)

http://arxiv.org/abs/1012.5943

### Project B5

#### Non-collinear spin states in bottom-up fabricated atomic chains

*M. Steinbrecher, R. Rausch, Khai Ton That, J. Hermenau, A.A. Khajetoorians, M. Potthoff, R. Wiesendanger, J. Wiebe*

Non-collinear spin states with unique rotational sense, such as chiral spin-spirals, are recently heavily investigated because of advantages for future applications in spintronics and information technology and as potential hosts for Majorana Fermions when coupled to a superconductor. Tuning the properties of such spin states, e.g., the rotational period and sense, is a highly desirable yet difficult task. Here, we experimentally demonstrate the bottom-up assembly of a spin-spiral derived from a chain of iron atoms on a platinum substrate using the magnetic tip of a scanning tunneling microscope as a tool. We show that the spin-spiral is induced by the interplay of the Heisenberg and Dzyaloshinskii-Moriya components of the Ruderman-Kittel-Kasuya-Yosida interaction between the iron atoms. The relative strengths and signs of these two components can be adjusted by the interatomic iron distance, which enables tailoring of the rotational period and sense of the spin-spiral.

#### Anomalous spin precession under a geometrical torque

*C. Stahl, M. Potthoff*

Precession and relaxation predominantly characterize the real-time dynamics of a spin driven by a magnetic field and coupled to a large Fermi sea of conduction electrons. We demonstrate an anomalous precession with frequency higher than the Larmor frequency or with inverted orientation in the limit where the electronic motion adiabatically follows the spin dynamics. For a classical spin, the effect is traced back to a geometrical torque resulting from a finite spin Berry curvature.

#### Enforcing conservation laws in nonequilibrium cluster perturbation theory

*C. Gramsch, M. Potthoff*

Using the recently introduced time-local formulation of the nonequilibrium cluster perturbation theory (CPT), we construct a generalization of the approach such that macroscopic conservation laws are respected. This is achieved by exploiting the freedom for the choice of the starting point of the all-order perturbation theory in the intercluster hopping. The proposed conserving CPT is a self-consistent propagation scheme which respects the conservation of energy, particle number, and spin, which treats short-range correlations exactly up to the linear scale of the cluster, and which represents a mean-field-like approach on length scales beyond the cluster size. Using Green's functions, conservation laws are formulated as local constraints on the local spin-dependent particle and the doublon density. We consider them as conditional equations to self-consistently fix the time-dependent intracluster one-particle parameters. Thanks to the intrinsic causality of the CPT, this can be set up as a step-by-step time propagation scheme with a computational effort scaling linearly with the maximum propagation time and exponentially in the cluster size. As a proof of concept, we consider the dynamics of the two-dimensional, particle-hole-symmetric Hubbard model following a weak interaction quench by simply employing two-site clusters only. Conservation laws are satisfied by construction. We demonstrate that enforcing them has strong impact on the dynamics. While the doublon density is strongly oscillating within plain CPT, a monotonic relaxation is observed within the conserving CPT.

#### Filling-dependent doublon dynamics in the one-dimensional Hubbard model

*R. Rausch and M. Potthoff*

The fate of a local two-hole doublon excitation in the one-dimensional Fermi-Hubbard model is systematically studied for strong Hubbard interaction U in the entire filling range using the density-matrix renormalization group (DMRG) and the Bethe ansatz. For strong U, two holes at the same site form a compound object whose decay is impeded by the lack of phase space. Still, a partial decay is possible on an extremely short time scale where phase-space arguments do not yet apply. We argue that the initial decay and the resulting intermediate state are relevant for experiments performed with ultracold atoms loaded into an optical lattice as well as for (time-resolved) CVV Auger-electron spectroscopy. The detailed discussion comprises the mixed ballistic-diffusive real-time propagation of the doublon through the lattice, its partial decay on the short time scale as a function of filling and interaction strength, as well as the analysis of the decay products, which are metastable on the intermediate time scale that is numerically accessible and which show up in the two-hole excitation (Auger) spectrum. The ambivalent role of singly occupied sites is key to understanding the doublon physics; for high fillings, ground-state configurations with single occupancies are recognized to strongly relax the kinematic constraints and to open up decay channels. For fillings close to half-filling, however, their presence actually blocks the doublon decay. Finally, the analysis of the continua in the two-hole spectrum excludes a picture where the doublon decays into unbound electron holes for generic fillings, different from the limiting case of the completely filled band. We demonstrate that the decay products as well as the doublon propagation should rather be understood in terms of Bethe ansatz eigenstates.

#### Inertia effects in the real-time dynamics of a quantum spin coupled to a Fermi sea

*M. Sayad, R. Rausch, M. Potthoff*

Spin dynamics in the Kondo impurity model, initiated by suddenly switching the direction of a local magnetic field, is studied by means of the time-dependent density-matrix renormalization group. Quantum effects are identified by systematic computations for different spin quantum numbers S and by comparing with tight-binding spin-dynamics theory for the classical-spin Kondo model. We demonstrate that, besides the conventional precessional motion and relaxation, the quantum-spin dynamics shows nutation, similar to a spinning top. Opposed to semiclassical theory, however, the nutation is efficiently damped on an extremely short time scale. The effect is explained in the large-S limit as quantum dephasing of the eigenmodes in an emergent two-spin model that is weakly entangled with the bulk of the system. We argue that, apart from the Kondo effect, the damping of nutational motion is essentially the only characteristics of the quantum nature of the spin. Qualitative agreement between quantum and semiclassical spin dynamics is found down to S=1/2.

#### One-step theory of two-photon photoemission

*J. Braun, R. Rausch, M. Potthoff, H. Ebert*

A theoretical frame for two-photon photoemission is derived from the general theory of pump-probe photoemission, assuming that not only the probe but also the pump pulse is sufficiently weak. This allows us to use a perturbative approach to compute the lesser Green function within the Keldysh formalism. Two-photon photoemission spectroscopy is a widely used analytical tool to study nonequilibrium phenomena in solid materials. Our theoretical approach aims at a material-specific, realistic, and quantitative description of the time-dependent spectrum based on a picture of effectively independent electrons as described by the local-density approximation in band-structure theory. To this end we follow Pendry's one-step theory of the photoemission process as close as possible and heavily make use of concepts of relativistic multiple-scattering theory, such as the representation of the final state by a time-reversed low-energy electron diffraction state. The formalism allows for a quantitative calculation of the time-dependent photocurrent for moderately correlated systems like simple metals or more complex compounds like topological insulators. An application to the Ag(100) surface is discussed in detail.

#### Relaxation of a classical spin coupled to a strongly correlated electron system

*13.09.2016 00:00 M. Sayad, R. Rausch, M. Potthoff*

A classical spin which is antiferromagnetically coupled to a system of strongly correlated conduction electrons is shown to exhibit unconventional real-time dynamics which cannot be described by Gilbert damping. Depending on the strength of the local Coulomb interaction U, the two main electronic dissipation channels, namely transport of excitations via correlated hopping and via excitations of correlation-induced magnetic moments, become active on largely different time scales. We demonstrate that correlations can lead to a strongly suppressed relaxation which so far has been observed in purely electronic systems only and which is governed here by proximity to the divergent magnetic time scale in the infinite-U limit.

#### Time-dependent Mott transition in the periodic Anderson model with nonlocal hybridization

*F. Hofmann, M. Potthoff*

The time-dependent Mott transition in a periodic Anderson model with off-site, nearest-neighbor hybridization is studied within the framework of nonequilibrium self-energy functional theory. Using the two-site dynamical-impurity approximation, we compute the real-time dynamics of the optimal variational parameter and of different observables initiated by sudden quenches of the Hubbard-U and identify the critical interaction. The time-dependent transition is orbital selective, i.e., in the final state, reached in the long-time limit after the quench to the critical interaction, the Mott gap opens in the spectral function of the localized orbitals only. We discuss the dependence of the critical interaction and of the final-state effective temperature on the hybridization strength and point out the various similarities between the nonequilibrium and the equilibrium Mott transition. It is shown that these can also be smoothly connected to each other by increasing the duration of a U-ramp from a sudden quench to a quasi-static process. The physics found for the model with off-site hybridization is compared with the dynamical Mott transition in the single-orbital Hubbard model and with the dynamical crossover found for the real-time dynamics of the conventional Anderson lattice with on-site hybridization.

#### Multiplons in the two-hole excitation spectra of the one-dimensional Hubbard model

*R. Rausch, M. Potthoff*

Using the density-matrix renormalization group in combination with the Chebyshev polynomial expansion technique, we study the two-hole excitation spectrum of the one-dimensional Hubbard model in the entire filling range from the completely occupied band (n = 2) down to half-filling (n = 1). For strong interactions, the spectra reveal multiplon physics, i.e., relevant final states are characterized by two (doublon), three (triplon), four (quadruplon) and more holes, potentially forming stable compound objects or resonances with finite lifetime. These give rise to several satellites in the spectra with largely different spectral weights as well as to different two-hole, doublon–hole, two-doublon etc continua. The complex multiplon phenomenology is analyzed by interpreting not only local and k-resolved two-hole spectra but also three- and four-hole spectra for the Hubbard model and by referring to effective low-energy models. In addition, a filter-operator technique is presented and applied which allows to extract specific information on the final states at a given excitation energy. While multiplons composed of an odd number of holes do neither form stable compounds nor well-defined resonances unless a nearest-neighbor density interaction V is added to the Hamiltonian, the doublon and the quadruplon are well-defined resonances. The k-resolved four-hole spectrum at n = 2 represents an interesting special case where a completely stable quadruplon turns into a resonance by merging with the doublon–doublon continuum at a critical wave vector. For all fillings with $n\gt 1$, the doublon lifetime is strongly k-dependent and is even infinite at the Brillouin zone edges as demonstrated by k-resolved two-hole spectra. This can be traced back to the 'hidden' charge-SU(2) symmetry of the model which is explicitly broken off half-filling and gives rise to a massive collective excitation, even for arbitrary higher-dimensional but bipartite lattices.

#### Lehmann representation of the nonequilibrium self-energy

*C. Gramsch, M. Potthoff*

It is shown that the nonequilibrium self-energy of an interacting lattice-fermion model has a unique Lehmann representation. Based on the construction of a suitable noninteracting effective medium, we provide an explicit and numerically practicable scheme to construct the Lehmann representation for the self-energy, given the Lehmann representation of the single-particle nonequilibrium Green's function. This is of particular importance for an efficient numerical solution of Dyson's equation in the context of approximations where the self-energy is obtained from a reference system with a small Hilbert space. As compared to conventional techniques to solve Dyson's equation on the Keldysh contour, the effective-medium approach allows us to reach a maximum propagation time, which can be several orders of magnitude longer. This is demonstrated explicitly by choosing the nonequilibrium cluster-perturbation theory as a simple approach to study the long-time dynamics of an inhomogeneous initial state after a quantum quench in the Hubbard model on a 10×10 square lattice. We demonstrate that the violation of conservation laws is moderate for weak Hubbard interaction and that the cluster approach is able to describe prethermalization physics.

#### Spin dynamics and relaxation in the classical-spin Kondo-impurity model beyond the Landau-Lifschitz-Gilbert equation

*M. Sayad, M. Potthoff*

The real-time dynamics of a classical spin in an external magnetic field and local exchange coupled to an extended one-dimensional system of non-interacting conduction electrons is studied numerically. Retardation effects in the coupled electron-spin dynamics are shown to be the source for the relaxation of the spin in the magnetic field. Total energy and spin is conserved in the non-adiabatic process. Approaching the new local ground state is therefore accompanied by the emission of dispersive wave packets of excitations carrying energy and spin and propagating through the lattice with Fermi velocity. While the spin dynamics in the regime of strong exchange coupling J is rather complex and governed by an emergent new time scale, the motion of the spin for weak J is regular and qualitatively well described by the Landau–Lifschitz–Gilbert (LLG) equation. Quantitatively, however, the full quantum–classical hybrid dynamics differs from the LLG approach. This is understood as a breakdown of weak-coupling perturbation theory in J in the course of time. Furthermore, it is shown that the concept of the Gilbert damping parameter is ill-defined for the case of a one-dimensional system.

#### Crossover from conventional to inverse indirect magnetic exchange in the depleted Anderson lattice

*M. W. Aulbach, I. Titvinidze, M. Potthoff*

We investigate the finite-temperature properties of an Anderson lattice with regularly depleted impurities. The physics of this model is ruled by two different magnetic exchange mechanisms: conventional Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction at weak hybridization strength V and an inverse indirect magnetic exchange (IIME) at strong V, both favoring a ferromagnetic ground state. The stability of ferromagnetic order against thermal fluctuations is systematically studied by static mean-field theory for an effective low-energy spin-only model emerging perturbatively in the strong-coupling limit as well as by dynamical mean-field theory for the full model. The Curie temperature is found at a maximum for a half-filled conduction band and at intermediate hybridization strengths in the crossover regime between RKKY and IIME.

#### One-step theory of pump-probe photoemission

*J. Braun, R. Rausch, M. Potthoff, J. Minár, H. Ebert*

#### Cooperation of different exchange mechanisms in confined magnetic systems

*A. Schwabe, M. Hänsel, M. Potthoff*

The diluted Kondo lattice model is investigated at strong antiferromagnetic local exchange couplings J, where almost-local Kondo clouds drastically restrict the motion of conduction electrons, giving rise to the possibility of quantum localization of conduction electrons for certain geometries of impurity spins. This localization may lead to the formation of local magnetic moments in the conduction-electron system, and the inverse indirect magnetic exchange (IIME) provided by virtual excitations of the Kondo singlets couples those local moments to the remaining electrons. Exemplarily, we study the one-dimensional two-impurity Kondo model with impurity spins near the chain ends, which supports the formation of conduction-electron magnetic moments at the edges of the chain for sufficiently strong J. Employing degenerate perturbation theory as well as analyzing spin gaps numerically by means of the density-matrix renormalization group, it is shown that the low-energy physics of the model can be well captured within an effective antiferromagnetic Ruderman–Kittel–Kasuya–Yosida-like two-spin model (“RKKY from IIME”) or within an effective central-spin model, depending on edge-spin distance and system size.

#### Nonequilibrium self-energy functional theory

*F. Hofmann, M. Eckstein, E. Arrigoni, M. Potthoff*

The self-energy functional theory (SFT) is generalized to describe the real-time dynamics of correlated lattice-fermion models far from thermal equilibrium. This is achieved by starting from a reformulation of the original equilibrium theory in terms of double-time Green's functions on the Keldysh-Matsubara contour. With the help of a generalized Luttinger-Ward functional, we construct a functional Ω̂[Σ] which is stationary at the physical (nonequilibrium) self-energy Σ and which yields the grand potential of the initial thermal state Ω at the physical point. Nonperturbative approximations can be defined by specifying a reference system that serves to generate trial self-energies. These self-energies are varied by varying the reference system's one-particle parameters on the Keldysh-Matsubara contour. In the case of thermal equilibrium, this approach reduces to the conventional SFT. Contrary to the equilibrium theory, however, “unphysical” variations, i.e., variations that are different on the upper and the lower branches of the Keldysh contour, must be considered to fix the time dependence of the optimal physical parameters via the variational principle. Functional derivatives in the nonequilibrium SFT Euler equation are carried out analytically to derive conditional equations for the variational parameters that are accessible to a numerical evaluation via a time-propagation scheme. Approximations constructed by means of the nonequilibrium SFT are shown to be inherently causal, internally consistent, and to respect macroscopic conservation laws resulting from gauge symmetries of the Hamiltonian. This comprises the nonequilibrium dynamical mean-field theory but also dynamical-impurity and variational-cluster approximations that are specified by reference systems with a finite number of degrees of freedom. In this way, nonperturbative and consistent approximations can be set up, the numerical evaluation of which is accessible to an exact-diagonalization approach.

#### Dynamical symmetry between spin and charge excitations studied by a plaquette mean-field approach in two dimensions

*P. Jurgenowski, M. Potthoff*

The real-time dynamics of local occupation numbers in a Hubbard model on a 6×6 square lattice is studied by means of the nonequilibrium generalization of the cluster-perturbation theory. The cluster approach is adapted to studies of two-dimensional lattice systems by using concepts of multiple-scattering theory and a component decomposition of the nonequilibrium Green's function on the Keldysh-Matsubara contour. We consider “classical” initial states formed as tensor products of states on 2×2 plaquettes and trace the effects of the interplaquette hopping in the final-state dynamics. Two different initially excited states are considered on an individual plaquette, a fully polarized staggered spin state (Néel) and a fully polarized charge-density wave (CDW). The final-state dynamics is constrained by a dynamical symmetry; i.e., the time-evolution operator and certain observables are invariant under an antiunitary transformation composed of time reversal, an asymmetric particle-hole, and a staggered sign transformation. We find an interesting interrelation between this dynamical symmetry and the separation of energy and time scales: In the case of a global excitation with all plaquettes excited, the initial Néel and the initial CDW states are linked by the transformation. This prevents an efficient relaxation of the CDW state on the short time scale governing the dynamics of charge degrees of freedom. Contrarily, the CDW state is found to relax much faster than the Néel state in the case of a local excitation on a single plaquette where the symmetry relation between the two states is broken by the coupling to the environment.

#### Inverse indirect magnetic exchange

*A. Schwabe, I. Titvinidze, M. Potthoff*

Magnetic moments strongly coupled to the spins of conduction electrons in a nanostructure can confine the conduction-electron motion due to scattering at almost localized Kondo singlets. We study the resulting local-moment formation in the conduction-electron system and the magnetic exchange coupling mediated by the Kondo singlets. Its distance dependence is oscillatory and induces robust ferro- or antiferromagnetic order in multi-impurity systems.

#### Doublon dynamics in the extended Fermi-Hubbard model

*F. Hofmann, M. Potthoff*

#### Krylov-space approach to the equilibrium and nonequilibrium single-particle Green's function

*M. Balzer, N. Gdaniec, M.Potthoff*

#### Nonequilibrium cluster perturbation theory

*M. Balzer, M. Potthoff*

## Project C

### Project C1

#### Twisted superfluid phase in the extended one-dimensional Bose-Hubbard

* D.-S. Lühmann*

#### Breaking inversion symmetry in a state-dependent honeycomb lattice: Artificial graphene with tunable band gap

* M. Weinberg, C. Staarmann, C. Ölschläger, J. Simonet, K. Sengstock*

Here, we present the application of a novel method for controlling the geometry of a state-dependent honeycomb lattice: The energy offset between the two sublattices of the honeycomb structure can be adjusted by rotating the atomic quantization axis. This enables us to continuously tune between a homogeneous graphene-like honeycomb lattice and a triangular lattice and to open an energy gap at the characteristic Dirac points. We probe the symmetry of the lattice with microwave spectroscopy techniques and investigate the behavior of atoms excited to the second energy band. We find a striking influence of the energy gap at the Dirac cones onto the lifetimes of atoms in the excited band.

#### Symmetry-broken momentum distributions induced by matter-wave diffraction during time-of-flight expansion of ultracold atoms

* M. Weinberg, O. Jürgensen, C. Ölschläger, D.-S. Lühmann, K. Sengstock, J. Simonet*

We study several effects which lead to symmetry-broken momentum distributions of quantum gases released from optical lattices. In particular, we demonstrate that interaction within the first milliseconds of the time-of-flight expansion can strongly alter the measurement of the initial atomic momentum distribution. For bosonic mixtures in state-dependent lattices, inter-species scattering processes lead to a symmetry breaking in momentum space. The underlying mechanism is identified to be diffraction of the matter wave from the total density lattice, which gives rise to a timedependent interaction potential. Our findings are of fundamental relevance for the interpretation of time-of-flight measurements and for the study of exotic quantum phases such as the twisted superfluid. Beyond that, the observed matter-wave diraction can also be used as an interferometric probe. In addition, we report on diffraction from the state-dependent standing light field, which leads to the same symmetry-broken momentum distributions, even for single component condensates.

#### Twisted complex superfluids in optical lattices

*O. Jürgensen, K. Sengstock, D.-S. Lühmann*

We show that correlated pair tunneling drives a phase transition to a twisted superfluid with a complex order parameter. This unconventional superfluid phase spontaneously breaks the time-reversal symmetry and is characterized by a twisting of the complex phase angle between adjacent lattice sites. We discuss the entire phase diagram of the extended Bose--Hubbard model for a honeycomb optical lattice showing a multitude of quantum phases including twisted superfluids, pair superfluids, supersolids and twisted supersolids. Furthermore, we show that the nearest-neighbor interactions breaks the inversion symmetry of the lattice and gives rise to dimerized density-wave insulators, where particles are delocalized on dimers. For two components, we find twisted superfluid phases with strong correlations between the species already for surprisingly small pair-tunneling amplitudes. Interestingly, this ground state shows an infinite degeneracy ranging continuously from a supersolid to a twisted superfluid.

#### Multiphoton interband excitations of quantum gases in driven optical lattices

* M. Weinberg, C. Ölschläger, C. Sträter, S. Prelle, A. Eckardt, K. Sengstock, J. Simonet*

We report on the observation of multiphoton absorption processes for quantum gases in shaken light crystals. Periodic inertial forcing, induced by a spatial motion of the lattice potential, drives multiphoton interband excitations of up to the 9th order. The occurrence of such excitation features is systematically investigated with respect to the potential depth and the driving amplitude. Ab initio calculations of resonance positions as well as numerical evaluation of their strengths exhibit a good agreement with experimental data. In addition our findings set the stage for reaching novel phases of quantum matter by tailoring appropriate driving schemes.

#### Beyond-mean-field study of a binary bosonic mixture in a state-dependent honeycomb lattice

* L. Cao, S. Krönke, J. Stockhofe, J. Simonet, K. Sengstock, D.-S. Lühmann and P. Schmelcher*

We investigate a binary mixture of bosonic atoms loaded into a state-dependent honeycomb lattice. For this system, the emergence of a so-called twisted-superfluid ground state was experimentally observed in Soltan-Panahi et al. [Nat. Phys. 8, 71 (2012)]. Theoretically, the origin of this effect is not understood. We perform numerical simulations of an extended single-band Bose-Hubbard model adapted to the experimental parameters employing the multilayer multiconfiguration time-dependent Hartree method for Bosons. Our results confirm the overall applicability of mean-field theory in the relevant parameter range, within the extended single-band Bose-Hubbard model. Beyond this, we provide a detailed analysis of correlation effects correcting the mean-field result. These have the potential to induce asymmetries in single shot time-of-flight measurements, but we find no indication of the patterns characteristic of the twisted superfluid. We comment on the restrictions of our model and possible extensions.

#### Dimerized Mott insulators in hexagonal optical lattices

*O. Jürgensen, D.-S. Lühmann*

We study bosonic atoms in optical honeycomb lattices with anisotropic tunneling and find dimerized Mott insulator (MI) phases with fractional filling. These incompressible insulating phases are characterized by an interaction-driven localization of particles in respect to the individual dimers and large local particle-number fluctuations within the dimers. We calculate the ground-state phase diagrams and the excitation spectra using an accurate cluster mean-field method. The cluster treatment enables us to probe the fundamental excitations of the dimerized MI where the excitation gap is dominated by the intra-dimer tunneling amplitude. This allows the distinction from normal Mott insulating phases gapped by the on-site interaction. In addition, we present analytical results for the phase diagram derived by a higher-order strong-coupling perturbative expansion approach. By computing finite lattices with large diameters the influence of a harmonic confinement is discussed in detail. It is shown that a large fraction of atoms forms the dimerized MI under experimental conditions. The necessary anisotropic tunneling can be realized either by periodic driving of the optical lattice or by engineering directly a dimerized lattice potential. The dimers can be mapped to their antisymmetric states creating a lattice with coupled p-orbitals.

#### Spin Orbit Coupling in Periodically Driven Optical Lattices

* J. Struck, J. Simonet, K. Sengstock*

We propose a novel experimental scheme for the emulation of spin-orbit coupling for ultracold, neutral atoms trapped in a one-dimensional lattice. This scheme does not involve near-resonant laser fields, avoiding the heating processes connected to the spontaneous emission of photons.

A time dependent magnetic field gradient periodically drives the atoms, which can lead to complex valued tunnel matrix elements, equivalent to a gauge dependent shift of the dispersion relation for a 1D lattice. For opposite spin states, the dispersion relations are shifted in opposite direction due to the inverted drive for both states. An additional radio-frequency coupling between the spin states leads to a mixing of the spin dispersion relations and a spin-orbit gap in the band structure.

Phys. Rev. A 90, 031601(R) (2014)

http://arxiv.org/abs/1407.1953

#### Quantum phases in tunable state-dependent hexagonal optical lattices

* D.-S. Lühmann, O. Jürgensen, M. Weinberg, J. Simonet, P. Soltan-Panahi, K. Sengstock*

We study the ground-state properties of ultracold bosonic atoms in a state-dependent graphene-like honeycomb optical lattice, where the degeneracy between the two triangular sublattices A and B can be lifted. We discuss the various geometries accessible with this lattice setup and present a novel scheme to control the energy offset with external magnetic fields. The competition of the on-site interaction with the offset energy leads to Mott phases characterized by population imbalances between the sublattices. For the definition of an optimal Hubbard model, we demonstrate a scheme that allows for the efficient computation of Wannier functions. Using a cluster mean-field method, we compute the phase diagrams and provide a universal representation for arbitrary energy offsets. We find good agreement with the experimental data for the superfluid to Mott insulator transition.

#### Tunable gauge potential for spinless particles in driven lattices

*J. Simonet, J. Struck, M. Weinberg, C. Ölschläger, P. Hauke, A. Eckardt, M. Lewenstein, K. Sengstock, P. Windpassinger*

We present a universal method to create a tunable, artificial vector gauge potential for neutral particles trapped in an optical lattice. A suitable periodic shaking of the lattice allows to engineer a Peierls phase for the hopping parameters. This scheme thus allows one to address the atomic internal degrees of freedom independently. We experimentally demonstrate the realisation of such artificial potentials in a 1D lattice, which generate ground state superfluids at arbitrary non-zero quasimomentum [4].

This scheme offers fascinating possibilities to emulate synthetic magnetic fields in 2D lattices. In a triangular lattice, continuously tunable staggered fluxes are realised. Spontaneous symmetry breaking has recently been observed for a π-flux [23]. With the presented scheme, we are now able to study the influence of a small symmetry breaking perturbation.

#### Engineering Ising-XY spin models in a triangular lattice using tunable artificial gauge fields

*J. Struck, M. Weinberg, C. Ölschläger, P. Windpassinger, J. Simonet, K. Sengstock, R. Höppner, P. Hauke, A. Eckardt, M. Lewenstein, L. Mathey*

#### Cluster Gutzwiller method for bosonic lattice systems

*D.-S. Lühmann*

A versatile and numerically inexpensive method is presented allowing the accurate calculation of phase diagrams for bosonic lattice models. By treating clusters within the Gutzwiller theory, a surprisingly good description of quantum fluctuations beyond the mean-field theory is achieved approaching quantum Monte Carlo predictions for large clusters. Applying this powerful method to the Bose-Hubbard model, we demonstrate that it yields precise results for the superfluid to Mott-insulator transition in square, honeycomb, and cubic lattices. Due to the exact treatment within a cluster, the method can be effortlessly adapted to more complicated Hamiltonians in the fast progressing field of optical lattice experiments. This includes state- and site-dependent superlattices, large confined atomic systems, and disordered potentials, as well as various types of extended Hubbard models. Furthermore, the approach allows an excellent treatment of systems with arbitrary filling factors. We discuss the perspectives that allow for the computation of large, spatially varying lattices, low-lying excitations, and time evolution.

#### Non-Abelian gauge fields and topological insulators in shaken optical lattices

*P. Hauke, O. Tielemann, A. Celi, C. Ölschläger, J. Simonet, J. Struck, M. Weinberg, P. Windpassinger, K. Sengstock, M. Lewenstein, A. Eckardt*

Time-periodic driving offers a low-demanding method to generate artificial gauge fields in optical lattices. We demonstrate that it is a powerful and versatile tool for engineering two-dimensional lattice systems: We show how to tune frustration and how to create and control band touching points like Dirac cones in the shaken kagom\'e lattice. We propose the realization of a topological or a quantum spin Hall insulator in a shaken spin-dependent hexagonal lattice. We describe how strong artificial magnetic fields can be achieved for example in a square lattice by employing superlattice modulation. Finally, exemplified on a shaken spin-dependent square lattice, we develop a method to create strong non-Abelian gauge fields.

Phys. Rev. Lett. 109, 145301 (2012)

http://www.arxiv.org/abs/1205.1398

#### Tunable gauge potential for neutral and spinless particles in driven lattices

* J. Struck, C. Ölschläger, M. Weinberg, P. Hauke, J. Simonet, A. Eckardt, M. Lewenstein, K. Sengstock, P. Windpassinger*

We present a universal method to create a tunable, artificial vector gauge potential for neutral particles trapped in an optical lattice. The necessary Peierls phase of the hopping parameters between neighboring lattice sites is generated by applying a suitable periodic inertial force such that the method does not rely on any internal structure of the particles. We experimentally demonstrate the realization of such artificial potentials, which generate ground state superfluids at arbitrary non-zero quasi-momentum. We furthermore investigate possible implementations of this scheme to create tuneable magnetic fluxes, going towards model systems for strong-field physics.

#### Quantum phase transition to unconventional multi-orbital superfluidity in optical lattices

* P. Soltan-Panahi, D.-S. Lühmann, J. Struck, P. Windpassinger, K. Sengstock*

Orbital physics plays a significant role for a vast number of important phenomena in complex condensed matter systems such as high-Tc superconductivity and unconventional magnetism. In contrast, phenomena in superfluids - especially in ultracold quantum gases - are commonly well described by the lowest orbital and a real order parameter. Here, we report on the observation of a novel multi-orbital superfluid phase with a complex order parameter in binary spin mixtures. In this unconventional superfluid, the local phase angle of the complex order parameter is continuously twisted between neighboring lattice sites. The nature of this twisted superfluid quantum phase is an interaction-induced admixture of the p-orbital favored by the graphene-like band structure of the hexagonal optical lattice used in the experiment. We observe a second-order quantum phase transition between the normal superfluid (NSF) and the twisted superfluid phase (TSF) which is accompanied by a symmetry breaking in momentum space. The experimental results are consistent with calculated phase diagrams and reveal fundamentally new aspects of orbital superfluidity in quantum gas mixtures. Our studies might bridge the gap between conventional superfluidity and complex phenomena of orbital physics.

Nature Physics 8, 71–75 (2012)

http://arxiv.org/abs/1104.3456v1

#### Quantum Simulation of Frustrated Classical Magnetism in Triangular Optical Lattices

* J. Struck, C. Ölschläger, R. Le Targat, P. Soltan-Panahi, A. Eckardt, M. Lewenstein, P. Windpassinger, K. Sengstock*

Magnetism plays a key role in modern technology and stimulates research in several branches of condensed matter physics. Although the theory of classical magnetism is well developed, the demonstration of a widely tunable experimental system has remained an elusive goal. We present the realization of a large-scale simulator for classical magnetism on a triangular lattice by exploiting the particular properties of a quantum system. We use the motional degrees of freedom of atoms trapped in an optical lattice to simulate a large variety of magnetic phases: ferromagnetic, antiferromagnetic, and even frustrated spin configurations. A rich phase diagram is revealed with different types of phase transitions. Our results provide a route to study highly debated phases like spin-liquids as well as the dynamics of quantum phase transitions.

### Project C2

#### Orbital optical lattices with bosons

*T. Kock, C. Hippler, A. Ewerbeck, and A. Hemmerich*

This article provides a synopsis of our recent experimental work exploring Bose-Einstein condensation in metastable higher Bloch bands of optical lattices. Bipartite lattice geometries have allowed us to implement appropriate band structures, which meet three basic requirements: the existence of metastable excited states sufficiently protected from collisional band relaxation, a mechanism to excite the atoms initially prepared in the lowest band with moderate entropy increase, and the possibility of cross-dimensional tunneling dynamics, necessary to establish coherence along all lattice axes. A variety of bands can be selectively populated and a subsequent thermalisation process leads to the formation of a condensate in the lowest energy state of the chosen band. As examples the 2nd, 4th and 7th bands in a bipartite square lattice are discussed. The geometry of the 2nd and 7th band can be tuned such that two inequivalent energetically degenerate energy minima arise at the X±-points at the edge of the 1st Brillouin zone. In this case even a small interaction energy is sufficient to lock the phase between the two condensation points such that a complex-valued chiral superfluid order parameter can emerge, which breaks time reversal symmetry. In the 4th band a condensate can be formed at the Gamma-point in the center of the 1st Brillouin zone, which can be used to explore topologically protected band touching points. The new techniques to access orbital degrees of freedom in higher bands greatly extend the class of many-body scenarios that can be explored with bosons in optical lattices.

J. Phys. B: At. Mol. Opt. Phys. 49, 042001 (2016)

http://arxiv.org/abs/1601.00500

#### Observation of chiral superfluid order by matter wave interference

* T. Kock, M. Ölschläger, A. Ewerbeck, W.-M. Huang, L. Mathey, A. Hemmerich*

The breaking of time reversal symmetry via the spontaneous formation of chiral order is ubiquitous in nature. Here, we present an unambiguous demonstration of this phenomenon for atoms Bose-Einstein condensed in the second Bloch band of an optical lattice. As a key tool we use a matter wave interference technique, which lets us directly observe the phase properties of the superfluid order parameter and allows us to reconstruct the spatial geometry of certain low energy excitations, associated with the formation of domains of different chirality. Our work marks a new era of optical lattices where orbital degrees of freedom play an essential role for the formation of exotic quantum matter, similarly as in electronic systems.

Physical Review Letters 114, 115301 (2015)

http://arxiv.org/abs/1411.3483

#### Controlling coherence via tuning of the population imbalance in a bipartite optical lattice

* M. Di Liberto, T. Comparin , T. Kock, M. Ölschäger, A. Hemmerich, C. Morais Smith*

The control of transport properties is a key tool at the basis of many technologically relevant effects in condensed matter. The clean and precisely controlled environment of ultracold atoms in optical lattices allows one to prepare simplified but instructive models, which can help to better understand the underlying physical mechanisms. We show that by tuning a structural deformation of the unit cell in a bipartite optical lattice, one can induce a phase transition from a superfluid into various Mott insulating phases forming a shell structure in the superimposed harmonic trap. The Mott shells are identified via characteristic features in the visibility of Bragg maxima in momentum spectra. The experimental findings are explained by Gutzwiller mean-field and quantum Monte Carlo calculations. Our system bears similarities with the loss of coherence in cuprate superconductors, known to be associated with the doping induced buckling of the oxygen octahedra surrounding the copper sites.

#### Proposed formation and dynamical signature of a chiral Bose liquid in an optical lattice

* X. Li, A. Paramekanti, A. Hemmerich, W. Vincent Liu*

Recent experiments on p-orbital atomic bosons have suggested the emergence of a spectacular ultracold superfluid with staggered orbital currents in optical lattices. This raises fundamental questions concerning the effects of thermal fluctuations as well as possible ways of directly observing such chiral order. Here we show via Monte Carlo simulations that thermal fluctuations destroy this superfluid in an unexpected two-step process, unveiling an intermediate normal phase with spontaneously broken time-reversal symmetry, dubbed a ‘chiral Bose liquid’. For integer fillings (n≥2) in the chiral Mott regime, thermal fluctuations are captured by an effective orbital Ising model, and Onsager’s powerful exact solution is adopted to determine the transition from this intermediate liquid to the para- orbital normal phase at high temperature. A lattice quench is designed to convert the staggered angular momentum, previously thought by experts difficult to directly probe, into coherent orbital oscillations, providing a time-resolved dynamical signature of chiral order.

Nature Communications 5, 3205 (2014)

http://arxiv.org/abs/1309.0523

#### Interaction-induced chiral px ± i py superfluid order of bosons in an optical lattice

*M. Ölschläger, T. Kock, G. Wirth, A. Ewerbeck, C. Morais Smith, A. Hemmerich*

The study of superconductivity with unconventional order is complicated in condensed matter systems by their immense complexity. Optical lattices with their exceptional precision and control allow one to emulate superfluidity avoiding many of the complications of condensed matter. A promising approach to realize unconventional superfluid order is to employ orbital degrees of freedom in higher Bloch bands. In recent work, indications were found that bosons condensed in the second band of an optical chequerboard lattice might exhibit px ± i py order. Here we present experiments, which provide strong evidence for the emergence of px ± i py order driven by the interaction in the local p-orbitals. We compare our observations with a multi-band Hubbard model and find excellent quantitative agreement.

New Journal of Physics 15, 083041 (2013)

http://arxiv.org/abs/1305.1177

#### Topologically induced avoided band crossing in an optical chequerboard lattice

* M. Ölschläger, G. Wirth, T. Kock, A. Hemmerich*

We report on the condensation of bosons in the 4th band of an optical chequerboard lattice providing a topologically induced avoided band crossing involving the second, third, and fourth bands. When the condensate is slowly tuned through the avoided crossing, accelerated band relaxation arises and the zero momentum approximately C4-invariant condensate wave function acquires finite momentum order and reduced C2 symmetry. For faster tuning Landau-Zener oscillations between different superfluid orders arise, which are used to characterize the avoided crossing.

Physical Review Letters, 108, 075302 (2012)

http://lanl.arxiv.org/abs/1110.3716

#### Topological semimetal in a fermionic optical lattice

* K. Sun, W. V. Liu, A. Hemmerich, S. Das Sarma*

Optical lattices have an important role in advancing our understanding of correlated quantum matter. The recent implementation of orbital degrees of freedom in chequerboard and hexagonal3 optical lattices opens up a new avenue towards discovering novel quantum states of matter that have no prior analogues in solid-state electronic materials. Here, we predict that an exotic topological semimetal emerges as a parity-protected gapless state in the orbital bands of a two-dimensional fermionic optical lattice. This new quantum state is characterized by a parabolic band-degeneracy point with Berry flux 2 Pi, in sharp contrast to the Pi-flux of Dirac points as in graphene.We showthat the appearance of this topological liquid is universal for all latticeswith D4 point-group symmetry, as long as orbitals with opposite parities hybridize strongly with each other and the band degeneracy is protected by odd parity. Turning on inter-particle repulsive interactions, the system undergoes a phase transition to a topological insulator whose experimental signature includes chiral gapless domain-wall modes, reminiscent of quantumHall edge states.

#### Unconventional Superfluid Order in the F Band of a Bipartite Optical Square Lattice

* M. Ölschläger, G. Wirth, A. Hemmerich*

We report on the first observation of bosons condensed into the energy minima of an F band of a bipartite square optical lattice. Momentum spectra indicate that a truly complex-valued staggered angular momentum superfluid order is established. The corresponding wave function is composed of alternating local F_(2x^3-3x)±iF_(2y^3-3y) orbits and local S orbits residing in the deep and shallow wells of the lattice, which are arranged as the black and white areas of a checkerboard. A pattern of staggered vortical currents arises, which breaks time-reversal symmetry and the translational symmetry of the lattice potential. We have measured the populations of higher order Bragg peaks in the momentum spectra for varying relative depths of the shallow and deep lattice wells and find remarkable agreement with band calculations.

#### Evidence for orbital superfluidity in the P-band of a bipartite optical square lattice

*G. Wirth, M. Ölschläger, A. Hemmerich*

The successful emulation of the Hubbard model in optical lattices has stimulated extensive efforts to extend their scope to also capture more complex, incompletely understood scenarios of many-body physics. A promising approach is to consider higher bands, where the orbital degree of freedom gives rise to a structural diversity that is directly relevant, for example, for the physics of strongly correlated electronic matter. Here we report evidence for the formation of a superfluid in the P-band of a bipartite optical square lattice with S-orbits and P-orbits arranged in a chequerboard pattern. The observed momentum spectra feature cross-dimensional coherence with a lifetime of nearly 20 ms. Depending on the value of a small adjustable anisotropy of the lattice, our findings are explained either by real-valued striped superfluid order parameters with different orientations Px±Py, or by a complex-valued Px±iPy order parameter, which breaks time-reversal symmetry.

Nature Physics 7, 147 (2011), featured in News & Views ibid.

#### Competing Superconducting States for Ultracold Atoms in Optical Lattices with Artificial Staggered Magnetic Field

* L.-K. Lim, A. Lazarides, A. Hemmerich, C. Morais Smith*

Abstract: We study superconductivity in an ultracold Bose-Fermi mixture loaded into a square optical lattice subjected to a staggered flux. While the bosons form a superfluid at very low temperature and weak interaction, the interacting fermions experience an additional long-ranged attractive interaction mediated by phonons in the bosonic superfluid. This leads us to consider a generalized Hubbard model with on-site and nearest-neighbor attractive interactions, which give rise to two competing superconducting channels. We use the Bardeen-Cooper-Schrieffer theory to determine the regimes where distinct superconducting ground states are stabilized, and find that the non-local pairing channel favors a superconducting ground state which breaks both the gauge and the lattice symmetries, thus realizing unconventional superconductivity. Furthermore, the particular structure of the single-particle spectrum leads to unexpected consequences, for example, a dome-shaped superconducting region in the temperature versus filing fraction phase diagram, with a normal phase that comprises much richer physics than a Fermi-liquid. Notably, the relevant temperature regime and coupling strength is readily accessible in state of the art experiments with ultracold trapped atoms.

#### Strongly interacting two-dimensional Dirac fermions

* L.-K. Lim, A. Lazarides, A. Hemmerich, C. Morais Smith*

We show how strongly interacting two-dimensional Dirac fermions can be realized with ultracold atoms in a two-dimensional optical square lattice with an experimentally realistic, inherent gauge field, which breaks time reversal and inversion symmetries. We find remarkable phenomena in a temperature range around a tenth of the Fermi temperature, accessible with present experimental techniques: at zero chemical potential, besides a conventional s-wave superconducting phase, unconventional superconductivity with non-local bond pairing arises. In a temperature vs. doping phase diagram, the unconventional superconducting phase exhibits a dome structure, reminiscent of the phase diagram for high-temperature superconductors and heavy fermions.

### Project C3

#### Dynamics of Ultracold Quantum Gases in the Dissipative Fermi-Hubbard Model

* K. Sponselee, L. Freystatzky, B. Abeln, M. Diem, B. Hundt, A. Kochanke, T. Ponath, B. Santra, L. Mathey, K. Sengstock and C. Becker*

Abstract. We employ metastable ultracold 173-Yb atoms to study dynamics in the 1D dissipative Fermi-Hubbard model experimentally and theoretically, and observe a complete inhibition of two-body losses after initial fast transient dynamics. We attribute the suppression of particle loss to the dynamical generation of a highly entangled Dicke state. For several lattice depths and for two- and six-spin component mixtures we find very similar dynamics, showing that the creation of strongly correlated states is a robust and universal phenomenon. This offers interesting opportunities for precision measurements.

#### Relaxation dynamics of a closed high-spin Fermi system far from equilibrium

* U. Ebling, J. S. Krauser, N. Fläschner, K. Sengstock, C. Becker, M. Lewenstein, A. Eckardt*

A fundamental question in many-body physics is how closed quantum systems reach equilibrium. We address this question experimentally and theoretically in an ultracold high-spin Fermi gas where we find a complex interplay between internal and motional degrees of freedom. The fermions are initially prepared far from equilibrium with only a few spin states occupied. The subsequent dynamics leading to redistribution among all spin states is observed experimentally and simulated theoretically using a kinetic Boltzmann equation with full spin coherence. The latter is derived microscopically and provides good agreement with experimental data without any free parameters. We identify several collisional processes, which occur on different time scales. By varying density and magnetic field, we control the relaxation dynamics and are able to continuously tune the character of a subset of spin states from an open to a closed system.

Phys. Rev. X 4, 021011 (2014)

http://arxiv.org/abs/1312.6704

#### Detecting quadrupole interactions in ultracold Fermi gases

*M. Lahrz, M. Lemeshko, K. Sengstock, C. Becker, L. Mathey*

#### Creation of Quantum-Degenerate Gases of Ytterbium in a Compact 2D-/3D-MOT Setup

*S. Dörscher, A. Thobe, B. Hundt, A. Kochanke, R. Le Targat, P. Windpassinger, C. Becker, K. Sengstock*

*The following article has been accepted by Review of Scientific Instruments. After it is published, it will be found at http://rsi.aip.org*

We report on the first experimental setup based on a 2D-/3D-MOT scheme to create both Bose-Einstein condensates and degenerate Fermi gases of several ytterbium isotopes. Our setup does not require a Zeeman slower and offers the flexibility to simultaneously produce ultracold samples of other atomic species. Furthermore, the extraordinary optical access favors future experiments in optical lattices. A 2D-MOT on the strong 1S0-1P1 transition captures ytterbium directly from a dispenser of atoms and loads a 3D-MOT on the narrow 1S0-3P1 intercombination transition. Subsequently, atoms are transferred to a crossed optical dipole trap and cooled evaporatively to quantum degeneracy.

Review of Scientific Instruments 84, 043109

http://arxiv.org/abs/1303.1105

#### Intrinsic Photoconductivity of Ultracold Fermions in Optical Lattices

* J. Heinze, J. S. Krauser, N. Fläschner, B. Hundt, S. Götze, A. Itin, L. Mathey, K. Sengstock, C. Becker*

We report on the first experimental observation of a persistent alternating photocurrent in an ultracold gas of fermionic atoms in an optical lattice. The dynamics is induced and sustained by an external harmonic confinement. We find a counterintuitively momentum-dependent oscillation frequency for excited particles and a fast decay of holes which we attribute to spatial trapping. Lifetime measurements reveal a significant enhancement of particle-hole recombination with increasing interactions.

Phys. Rev. Lett. 110, 085302 (2013)

http://arxiv.org/abs/1208.4020

### Project C4

#### Detecting Friedel oscillations in ultracold Fermi gases

* Keno Riechers, Klaus Hueck, Niclas Luick, Thomas Lompe, Henning Moritz*

Investigating Friedel oscillations in ultracold gases would complement the studies performed on solid state samples with scanning-tunneling microscopes. In atomic quantum gases interactions and external potentials can be tuned freely and the inherently slower dynamics allow to access non-equilibrium dynamics following a potential or interaction quench. Here, we examine how Friedel oscillations can be observed in current ultracold gas experiments under realistic conditions. To this aim we numerically calculate the amplitude of the Friedel oscillations which a potential barrier provokes in a 1D Fermi gas and compare it to the expected atomic and photonic shot noise in a density measurement. We find that to detect Friedel oscillations the signal from several thousand one-dimensional systems has to be averaged. However, as up to 100 parallel one-dimensional systems can be prepared in a single run with present experiments, averaging over about 100 images is sufficient.

Eur. Phys. J. D 71, 232 (2017)

http://lanl.arxiv.org/abs/1704.06626

#### Two-Dimensional Homogeneous Fermi Gases

* Klaus Hueck, Niclas Luick, Lennart Sobirey, Jonas Siegl, Thomas Lompe, Henning Moritz*

We report on the experimental realization of homogeneous two-dimensional (2D) Fermi gases trapped in a box potential. In contrast to harmonically trapped gases, these homogeneous 2D systems are ideally suited to probe local as well as non-local properties of strongly interacting many-body systems. As a first measurement, we use a local probe to extract the equation of state (EOS) of a non-interacting Fermi gas. We then perform matter wave focusing to extract its momentum distribution and directly observe Pauli blocking in a near unity occupation of momentum states. Finally, we measure the momentum distribution of strongly interacting homogeneous 2D gases in the crossover between attractively interacting fermions and deeply-bound bosonic molecules.

PRL 120, 060402 (2018).

http://lanl.arxiv.org/abs/1704.06315

#### Calibrating High Intensity Absorption Imaging of Ultracold Atoms

* Klaus Hueck, Niclas Luick, Lennart Sobirey, Jonas Siegl, Thomas Lompe, Henning Moritz, Logan W. Clark, Cheng Chin*

Absorption imaging of ultracold atoms is the foundation for quantitative extraction of information from experiments with ultracold atoms. Due to the limited exposure time available in these systems, the signal-to-noise ratio is largest for high intensity absorption imaging where the intensity of the imaging light is on the order of the saturation intensity. In this case, the absolute value of the intensity of the imaging light enters as an additional parameter making it more sensitive to systematic errors. Here, we present a novel and robust technique to determine the imaging intensity in units of the effective saturation intensity to better than 5%. We do this

by measuring the momentum transferred to the atoms by the imaging light while varying its intensity. We further utilize the method to quantify the purity of the polarization of the imaging light and to determine the correct

imaging detuning.

Opt. Express 25, 8670-8679 (2017)

https://arxiv.org/abs/1702.01943

#### Suppression of kHz-Frequency Switching Noise in Digital Micro-Mirror Devices

* Klaus Hueck, Anton Mazurenko, Niclas Luick, Thomas Lompe, Henning Moritz*

igh resolution digital micro-mirror devices (DMD) make it possible to produce nearly arbitrary light fields with high accuracy, reproducibility and low optical aberrations. However, using these devices to trap and manipulate ultracold atomic systems for e.g. quantum simulation is often complicated by the presence of kHz-frequency switching noise. Here we demonstrate a simple hardware extension that solves this problem and makes it possible to produce truly static light fields. This modification leads to a 47 fold increase in the time that we can hold ultracold 6Li atoms in a dipole potential created with the DMD. Finally, we provide reliable and user friendly APIs written in Matlab and Python to control the DMD.

Rev. Sci. Instrum. 88, 016103 (2017)

https://arxiv.org/abs/1611.03397

#### Sudden and slow quenches into the antiferromagnetic phase of ultracold fermions

*M. Ojekhile, R. Höppner, H. Moritz, L. Mathey*

#### Probing superfluidity of Bose-Einstein condensates via laser stirring

*Vijay Pal Singh, Wolf Weimer, Kai Morgener, Jonas Siegl, Klaus Hueck, Niclas Luick, Henning Moritz, Ludwig Mathey*

We investigate the superfluid behavior of a Bose-Einstein condensate of 6Li molecules. In the experiment by Weimer et al., Phys. Rev. Lett. 114, 095301 (2015) a condensate is stirred by a weak, red-detuned laser beam along a circular path around the trap center. The rate of induced heating increases steeply above a velocity vc, which we define as the critical velocity. Below this velocity, the moving beam creates almost no heating. In this paper, we demonstrate a quantitative understanding of the critical velocity. Using both numerical and analytical methods, we identify the non-zero temperature, the circular motion of the stirrer, and the density profile of the cloud as key factors influencing the magnitude of vc. A direct comparison to the experimental data shows excellent agreement.

Phys. Rev. A 93, 023634 (2016)

http://lanl.arxiv.org/abs/1509.02168

#### The critical velocity in the BEC-BCS crossover

* W. Weimer, K. Morgener, V. P. Singh, J. Siegl, K. Hueck, N. Luick, L. Mathey, H. Moritz*

We map out the critical velocity in the crossover from Bose-Einstein condensation (BEC) to Bardeen-Cooper-Schrieffer superfluidity with ultracold 6Li gases. A small attractive potential is dragged along lines of constant column density. The rate of the induced heating increases steeply above a critical velocity vc. In the same samples, we measure the speed of sound vs by exciting density waves and compare the results to the measured values of vc. We perform numerical simulations in the BEC regime and find very good agreement, validating the approach. In the strongly correlated regime, where theoretical predictions only exist for the speed of sound, our measurements of vc provide a testing ground for theoretical approaches.

Phys. Rev. Lett. 114, 095301 (2015)

http://arxiv.org/abs/1408.5239

#### Interferometric Measurement of Local Spin-Fluctuations in a Quantum Gas

* J. Meineke, J.-P. Brantut, D. Stadler, T. Mueller, H. Moritz, T. Esslinger*

Ultracold gases provide a controlled environment that is ideal for studying many intriguing phenomena associated with quantum correlated systems. Current efforts are directed towards the identification of magnetic properties, as well as the creation and detection of exotic quantum phases. In this context, a mapping of the spin polarization of the atoms to the state of a single-mode light beam has been proposed. Here we introduce a quantum-limited interferometer that realizes such an atom–light interface with high spatial resolution. We measure the probability distribution of the local spin polarization in a trapped Fermi gas, showing a reduction of spin fluctuations by up to 4.6(3) dB below shot noise in weakly interacting Fermi gases, and by 9.4(8) dB for strong interactions. We deduce the magnetic susceptibility as a function of temperature and discuss our measurements in terms of an entanglement witness.

The subtle interplay between quantum-statistics and interactions is at the origin of many intriguing quantum phenomena connected to superfluidity and quantum magnetism. The controlled setting of ultracold quantum gases is well suited to study such quantum correlated systems. Current efforts are directed towards the identification of their magnetic properties, as well as the creation and detection of exotic quantum phases. In this context, it has been proposed to map the spin-polarization of the atoms to the state of a single-mode light beam. Here we introduce a quantum-limited interferometer realizing such an atom-light interface with high spatial resolution. We measure the probability distribution of the local spin-polarization in a trapped Fermi gas showing a reduction of spin-fluctuations by up to 4.6(3) dB below shot-noise in weakly interacting Fermi gases and by 9.4(8) dB for strong interactions. We deduce the magnetic susceptibility as a function of temperature and discuss our measurements in terms of an entanglement witness.

Nature Physics 8, 454 (2012)

http://xxx.lanl.gov/abs/1202.5250

#### High-resolution imaging and manipulation of ultracold fermions

* B. Zimmermann, T. Mueller, J. Meineke, T. Esslinger, H. Moritz*

We report on the local probing and manipulation of an ultracold Fermi gas on the length scale of one micrometer, i.e. of the order of the Fermi wavelength. The essential tool of our experimental setup is a pair of identical, high-resolution microscope objectives. One of the microscope objectives allows local imaging of the trapped Fermi gas of 6Li atoms with a maximum resolution of 660 nm, while the other enables the generation of arbitrary optical dipole potentials on the same length scale. Employing a 2D acousto-optical deflector, we demonstrate the formation of several trapping geometries including a tightly focussed single optical dipole trap, a 4x4-site two-dimensional optical lattice and a 8-site ring lattice configuration. Furthermore, we show the ability to load and detect a small number of atoms in these trapping potentials. A site separation of down to one micrometer in combination with the low mass of 6Li results in tunneling rates which are sufficiently large for the implementation of Hubbard-models with the designed geometries.

#### Local observation of antibunching in a trapped Fermi gas

* T. Müller, B. Zimmermann, J. Meineke, J.-P. Brantut, T. Esslinger, H. Moritz*

For a viewpoint written by Chris Westbrook for "Physics", follow this link.

Local density fluctuations and density profiles of a Fermi gas are measured in situ and analyzed. In the quantum degenerate regime, the weakly interacting 6Li gas shows a suppression of the density fluctuations compared to the nondegenerate case, where atomic shot noise is observed. This manifestation of antibunching is a direct result of the Pauli principle and constitutes a local probe of quantum degeneracy. We analyze our data using the predictions of the fluctuation-dissipation theorem and the local density approximation, demonstrating a fluctuation-based temperature measurement.

Phys. Rev. Lett. 105, 040401 (2010)

http://lanl.arxiv.prg/abs/1005.0302

#### A Mott insulator of fermionic atoms in an optical lattice

* R. Jördens, N. Strohmaier, K. Günter, H. Moritz, T. Esslinger*

Strong interactions between electrons in a solid material can lead to surprising properties. A prime example is the Mott insulator, in which suppression of conductivity occurs as a result of interactions rather than a filled Bloch band. Proximity to the Mott insulating phase in fermionic systems is the origin of many intriguing phenomena in condensed matter physics, most notably high-temperature superconductivity. The Hubbard model, which encompasses the essential physics of the Mott insulator, also applies to quantum gases trapped in an optical lattice. It is therefore now possible to access this regime with tools developed in atomic physics. However, an atomic Mott insulator has so far been realized only with a gas of bosons7, which lack the rich and peculiar nature of fermions. Here we report the formation of a Mott insulator of a repulsively interacting two-component Fermi gas in an optical lattice. It is identified by three features: a drastic suppression of doubly occupied lattice sites, a strong reduction of the compressibility inferred from the response of double occupancy to an increase in atom number, and the appearance of a gapped mode in the excitation spectrum. Direct control of the interaction strength allows us to compare the Mott insulating regime and the non-interacting regime without changing tunnel-coupling or confinement. Our results pave the way for further studies of the Mott insulator, including spin-ordering and ultimately the question of d-wave superfluidity.

### Project C5

#### Topological Varma superfluid in optical lattices

* M. Di Liberto, A. Hemmerich, and C. Morais Smith*

Topological states of matter are peculiar quantum phases showing different edge and bulk transport properties connected by the bulk-boundary correspondence. While non-interacting fermionic topological insulators are well established by now and have been classified according to a ten-fold scheme, the possible realisation of topological states for bosons has not been much explored yet. Furthermore, the role of interactions is far from being understood. Here, we show that a topological state of matter exclusively driven by interactions may occur in the p-band of a Lieb optical lattice filled with ultracold bosons. The single-particle spectrum of the system displays a remarkable parabolic band-touching point, with both bands exhibiting non-negative curvature. Although the system is neither topological at the single-particle level, nor for the interacting ground state, on-site interactions induce an anomalous Hall effect for the excitations, carrying a non-zero Chern number. Our work introduces an experimentally realistic strategy for the formation of interaction-driven topological states of bosons.

Physical Review Letters 117, 163001 (2016)

https://arxiv.org/abs/1604.06055

#### In-situ observation of optomechanical Bloch oscillations in an optical cavity

*H. Keßler, J. Klinder, B. Prasanna Venkatesh, Ch. Georges, A. Hemmerich*

It is shown experimentally that a Bose-Einstein condensate inside an optical cavity, operating in the regime of strong cooperative coupling, responds to an external force by an optomechanical Bloch oscillation, which can be directly observed in the light leaking out of the cavity. Previous theoretical work predicts that the frequency of this oscillation matches with that of conventional Bloch oscillations such that its in-situ monitoring may help to increase the data acquisition speed in precision force measurements.

New Journal of Physics 18, 102001 (2016)

https://arxiv.org/abs/1606.08386

#### Observation of a superradiant Mott insulator in the Dicke-Hubbard model

* J. Klinder, H. Keßler, M. Reza Bakhtiari, M. Thorwart, and A. Hemmerich*

It is well known that the bosonic Hubbard model possesses a Mott insulator phase. Likewise, it is known that the Dicke model exhibits a self-organized superradiant phase. By implementing an optical lattice inside of a high finesse optical cavity both models are merged such that an extended Hubbard model with cavity-mediated infinite range interactions arises. In addition to a normal superfluid phase, two superradiant phases are found, one of them coherent and hence superfluid and one incoherent Mott insulating.

Physical Review Letters 115, 230403 (2015)

http://arxiv.org/abs/1511.00850

#### Nonequilibrium phase transition of interacting bosons in an intra-cavity optical lattice

* M. R. Bakhtiari, A. Hemmerich, H. Ritsch, M. Thorwart*

We investigate the nonlinear light-matter interaction of a Bose-Einstein condensate trapped in an external periodic potential inside an optical cavity, which is weakly coupled to the vacuum radiation modes and driven by a transverse pump field. Based on a generalized Bose-Hubbard model, which incorporates a single cavity mode, we include the collective back action of the atoms on the cavity light field and determine the nonequilibrium quantum phases within the non-perturbative bosonic dynamical mean-field theory. With the system parameters adapted to recent experiments, we find a quantum phase transition from a normal phase to a self-organized superfluid phase, which is related to the Hepp-Lieb-Dicke phase transition. For even stronger pumping, a self-organized Mott insulator phase arises.

Physical Review Letters 114, 123601 (2015)

http://arxiv.org/abs/1410.5735

#### Steering matter wave superradiance with an ultra-narrowband optical cavity

* H. Keßler, J. Klinder, M. Wolke, A. Hemmerich*

A superfluid atomic gas is prepared inside an optical resonator with an ultra-narrow band width on the order of the single photon recoil energy. When a monochromatic off-resonant laser beam irradiates the atoms, above a critical intensity the cavity emits superradiant light pulses with a duration on the order of its photon storage time. The atoms are collectively scattered into coherent superpositions of discrete momentum states, which can be precisely controlled by adjusting the cavity resonance frequency. With appropriate pulse sequences the entire atomic sample can be collectively accelerated or decelerated by multiples of two recoil momenta. The instability boundary for the onset of matter wave superradiance is recorded and its main features are explained by a mean field model.

Physical Review Letters 113, 070404 (2014)

http://arxiv.org/abs/1407.4954

#### Optomechanical atom-cavity interaction in the sub-recoil regime

* H. Keßler, J. Klinder, M. Wolke, A. Hemmerich*

We study the optomechanical interaction of a Bose-Einstein condensate with a single longitudinal mode of an ultra-high finesse standing wave optical resonator. As a unique feature the resonator combines three extreme regimes, previously not realized together, i.e., strong cooperative coupling, cavity dominated scattering with a Purcell factor far above unity, and sub-recoil resolution provided by a cavity damping rate smaller than four times the single photon recoil frequency. We present experimental observations in good agreement with a two-mode model predicting highly non-linear dynamics with signatures as bistability, hysteresis, persistent oscillations, and superradiant back-scattering instabilities.

New Journal of Physics 16, 053008 (2014)

http://arxiv.org/abs/1403.3545

#### Cavity cooling below the recoil limit

* M. Wolke, J. Klinner, H. Keßler, A. Hemmerich*

Conventional laser cooling relies on repeated electronic excitations by near-resonant light, which constrains its area of application to a selected number of atomic species prepared at moderate particle densities. Optical cavities with sufficiently large Purcell factors allow for laser cooling schemes avoiding these limitations. Here, we report on an atom-cavity system, combining a Purcell factor above 40 with a cavity bandwidth below the recoil frequency associated with the kinetic energy transfer in a single photon scattering event. This lets us access a yet unexplored regime of atom-cavity interactions, in which the atomic motion can be manipulated by targeted dissipation with sub-recoil resolution. We demonstrate cavity-induced heating of a Bose-Einstein condensate and subsequent cooling at particle densities and temperatures incompatible with conventional laser cooling.

#### Normal-Mode-Splitting and Mechanical Effects of an Optical Lattice in a Ring Cavity

* J. Klinner, M. Lindholdt, B. Nagorny, A. Hemmerich*

A novel regime of atom-cavity physics is explored, arising when large atom samples dispersively interact with high-finesse optical cavities. A stable far-detuned optical lattice of several million rubidium atoms is formed inside an optical ring resonator by coupling equal amounts of laser light to each propagation direction of a longitudinal cavity mode. An adjacent longitudinal mode, detuned by about 3 GHz, is used to perform probe transmission spectroscopy of the system. The atom-cavity coupling for the lattice beams and the probe is dispersive and dissipation results only from the finite photon-storage time. The observation of two well-resolved normal modes demonstrates the regime of strong cooperative coupling. The details of the normal mode spectrum reveal mechanical effects associated with the retroaction of the probe upon the optical lattice.

### Project C6

#### Symmetry effects on the spin switching of adatoms

* C. Hübner, B. Baxevanis, A. A. Khajetoorians, D. Pfannkuche*

Highly symmetric magnetic environments have been suggested to stabilize the magnetic information stored in magnetic adatoms on a surface. Utilized as memory devices such systems are subjected to electron tunneling and external magnetic fields. We analyze theoretically how such perturbations affect the switching probability of a single quantum spin for two characteristic symmetries encountered in recent experiments and suggest a third one that exhibits robust protection against surface-induced spin flips. Further we illuminate how the switching of an adatom spin exhibits characteristic behavior with respect to low energy excitations from which the symmetry of the system can be inferred.

#### Isospin correlations in two-partite hexagonal optical lattices

* M. Prada, E.-M. Richter, D. Pfannkuche*

Two-component mixtures in optical lattices reveal a rich variety of different phases. We employ an exact diagonalization method to obtain the relevant correlation functions in hexagonal optical lattices which characterize those phases. We relate the occupation difference of the two species to the magnetic polarization. “Iso” -magnetic correlations disclose the nature of the system, which can be of easy-axis type, bearing phase segregation, or of easy-plane type, corresponding to super-counter-fluidity. In the latter case, the correlations reveal easy-plane segregation, involving a highly entangled state. We identify striking correlated supersolid phases appearing within the superfluid limit.

#### Doublon Relaxation in the Bose-Hubbard Model

*A. L. Chudnovskiy, D. M. Gangardt, A. Kamenev*

### Project C7

#### Entanglement Induced Interactions in Binary Mixtures

*J. Chen, J.M. Schurer and P. Schmelcher*

We establish a conceptual framework for the identification and the characterization of induced interactions in binary mixtures and reveal their intricate relation to entanglement between the components or species of the mixture. Exploiting an expansion in terms of the strength of the entanglement among the two species enables us to deduce an effective single-species description. In this way, we naturally incorporate the mutual feedback of the species and obtain induced interactions for both species which are effectively present among the particles of same type. Importantly, our approach incorporates few-body and inhomogeneous systems extending the scope of induced interactions where two particles interact via a bosonic bath-type environment. Employing the example of a one-dimensional ultracold Bose-Fermi mixture, we obtain induced Bose-Bose and Fermi-Fermi interactions with short-range attraction and long-range repulsion. With this, we show how beyond species mean-field physics visible in the two-body correlation functions can be understood via the induced interactions.

#### Bosonic quantum dynamics following a linear interaction quench in finite optical lattices of unit filling

*S.I. Mistakidis, G.M. Koutentakis and P. Schmelcher*

The nonequilibrium ultracold bosonic quantum dynamics in finite optical lattices of unit filling following a linear interaction quench from a superfluid to a Mott insulator state and vice versa is investigated. The resulting dynamical response consists of various inter and intraband tunneling modes. We find that the competition between the quench rate and the interparticle repulsion leads to a resonant dynamical response, at moderate ramp times, being related to avoided crossings in the many-body eigenspectrum with varying interaction strength. Crossing the regime of weak to strong interactions several transport pathways are excited. The higher-band excitation dynamics is shown to obey an exponential decay possessing two distinct time scales with varying ramp time. Studying the crossover from shallow to deep lattices we find that for a diabatic quench the excited band fraction decreases, while approaching the adiabatic limit it exhibits a non-linear behavior for increasing height of the potential barrier. The inverse ramping process from strong to weak interactions leads to a melting of the Mott insulator and possesses negligible higher-band excitations which follow an exponential decay for decreasing quench rate. Finally, independently of the direction that the phase boundary is crossed, we observe a significant enhancement of the excited to higher-band fraction for increasing system size.

#### Many-body expansion dynamics of a Bose-Fermi mixture confined in an optical lattice

*P. Siegl, S.I. Mistakidis and P. Schmelcher*

We unravel the correlated nonequilibrium dynamics of a mass balanced Bose-Fermi mixture in a one-dimensional optical lattice upon quenching an imposed harmonic trap from strong to weak confinement. Regarding the system's ground state, the competition between the inter- and intraspecies interaction strength gives rise to the immiscible and miscible phases characterized by negligible and complete overlap of the constituting atomic clouds, respectively. The resulting dynamical response depends strongly on the initial phase and consists of an expansion of each cloud and an interwell tunneling dynamics. For varying quench amplitude and referring to a fixed phase, a multitude of response regimes is unveiled, being richer within the immiscible phase, which are described by distinct expansion strengths and tunneling channels.

#### Correlation effects in the quench-induced phase separation dynamics of a two species ultracold quantum gas

*S.I. Mistakidis, G.C. Katsimiga, P.G. Kevrekidis and P. Schmelcher*

We explore the quench dynamics of a binary Bose–Einstein condensate crossing the miscibility–immiscibility threshold and vice versa, both within and in particular beyond the mean-field approximation. Increasing the interspecies repulsion leads to the filamentation of the density of each species, involving shorter wavenumbers and longer spatial scales in the many-body (MB) approach. These filaments appear to be strongly correlated and exhibit domain-wall structures. Following the reverse quench process multiple dark–antidark solitary waves are spontaneously generated and subsequently found to decay in the MB scenario. We simulate single-shot images to connect our findings to possible experimental realizations. Finally, the growth rate of the variance of a sample of single-shots probes the degree of entanglement inherent in the system.

#### Correlation induced localization of lattice trapped bosons coupled to a Bose–Einstein condensate

*K. Keiler, S. Krönke and P. Schmelcher*

We investigate the ground state properties of a lattice trapped bosonic system coupled to a Lieb–Liniger type gas. Our main goal is the description and in depth exploration and analysis of the two-species many-body quantum system including all relevant correlations beyond the standard mean-field approach. To achieve this, we use the multi-configuration time-dependent Hartree method for mixtures (ML-MCTDHX). Increasing the lattice depth and the interspecies interaction strength, the wave function undergoes a transition from an uncorrelated to a highly correlated state, which manifests itself in the localization of the lattice atoms in the latter regime. For small interspecies couplings, we identify the process responsible for this cross-over in a single-particle-like picture. Moreover, we give a full characterization of the wave function's structure in both regimes, using Bloch and Wannier states of the lowest band, and we find an order parameter, which can be exploited as a corresponding experimental signature. To deepen the understanding, we use an effective Hamiltonian approach, which introduces an induced interaction and is valid for small interspecies interaction. We finally compare the ansatz of the effective Hamiltonian with the results of the ML-MCTDHX simulations.

#### Quantum dynamics of two trapped bosons following infinite interaction quenches

*L.M.A. Kehrberger, V.J. Bolsinger and P. Schmelcher*

We investigate the quantum dynamics of two identical bosons in a one-dimensional harmonic trap following an interaction quench from zero to infinite interaction strength and vice versa. For both quench scenarios, closed analytical expressions for the temporal evolution of the wave function as well as the Loschmidt echo are found and the dynamics of the momentum density as well as the reduced single-particle density matrix are analyzed. We observe a crossover of these quantities between bosonic, “symmetrized” fermionic, and fermionic properties. Furthermore, several combined quenches are analyzed as well.

#### Quantum dynamical response of ultracold few-boson ensembles in finite optical lattices to multiple interaction quenches

*J. Neuhaus-Steinmetz, S. Mistakidis and P. Schmelcher*

The correlated nonequilibrium quantum dynamics following a multiple interaction quench protocol for few-bosonic ensembles confined in finite optical lattices is investigated. The quenches give rise to an interwell tunneling and excite the cradle and a breathing mode. Several tunneling pathways open during the time interval of increased interactions, while only a few occur when the system is quenched back to its original interaction strength. The cradle mode, however, persists during and in between the quenches, while the breathing mode possesses distinct frequencies. The occupation of excited bands is explored in detail revealing a monotonic behavior with increasing quench amplitude and a nonlinear dependence on the duration of the application of the quenched interaction strength. Finally, a periodic population transfer between momenta for quenches of increasing interaction is observed, with a power-law frequency dependence on the quench amplitude. Our results open the possibility to dynamically manipulate various excited modes of the bosonic system.

#### Collective excitations of dipolar gases based on local tunneling in superlattices

*L. Cao, S.I. Mistakidis, X. Deng and P. Schmelcher*

The collective dynamics of a dipolar fermionic quantum gas confined in a one-dimensional double-well superlattice is explored. The fermionic gas resides in a paramagnetic-like ground state in the weak interaction regime, upon which a new type of collective dynamics is found when applying a local perturbation. This dynamics is composed of the local tunneling of fermions in separate supercells, and is a pure quantum effect, with no classical counterpart. Due to the presence of the dipolar interactions the local tunneling transports through the entire superlattice, giving rise to a collective dynamics. A well-defined momentum-energy dispersion relation is identified in the ab-initio simulations demonstrating the phonon-like behavior. The phonon-like characteristic is also confirmed by an analytical description of the dynamics within a semiclassical picture.

#### Mode coupling of interaction quenched ultracold few-boson ensembles in periodically driven lattices

*S.I. Mistakidis and P. Schmelcher*

The out-of-equilibrium dynamics of interaction quenched finite ultracold bosonic ensembles in periodically driven one-dimensional optical lattices is investigated. It is shown that periodic driving enforces the bosons in the outer wells of the finite lattice to exhibit out-of-phase dipolelike modes, while in the central well the atomic cloud experiences a local breathing mode. The dynamical behavior is investigated with varying driving frequencies, revealing resonantlike behavior of the intrawell dynamics. An interaction quench in the periodically driven lattice gives rise to admixtures of different excitations in the outer wells, enhanced breathing in the center, and amplification of the tunneling dynamics. We then observe multiple resonances between the inter- and the intrawell dynamics at different quench amplitudes, with the position of the resonances being tunable via the driving frequency. Our results pave the way for future investigations of the use of combined driving protocols in order to excite different inter- and intrawell modes and to subsequently control them.

#### Quench-induced resonant tunneling mechanisms of bosons in an optical lattice with harmonic confinement

*G.M. Koutentakis, S.I. Mistakidis and P. Schmelcher*

The nonequilibrium dynamics of small boson ensembles in a one-dimensional optical lattice is explored upon a sudden quench of an additional harmonic trap from strong to weak confinement. We find that the competition between the initial localization and the repulsive interaction leads to a resonant response of the system for intermediate quench amplitudes, corresponding to avoided crossings in the many-body eigenspectrum with varying final trap frequency. In particular, we show that these avoided crossings can be utilized to prepare the system in a desired state. The dynamical response is shown to depend on both the interaction strength as well as the number of atoms manifesting the many-body nature of the tunneling dynamics.

#### Resonant quantum dynamics of few ultracold bosons in periodically driven finite lattices

* S.I. Mistakidis, T. Wulf, A. Negretti and P. Schmelcher*

The out-of-equilibrium dynamics of finite ultracold bosonic ensembles in periodically driven one-dimensional optical lattices is investigated. Our study reveals that the driving enforces the bosons in different wells to oscillate in-phase and to exhibit a dipole-like mode. A wide range from weak-to-strong driving frequencies is covered and a resonance-like behavior of the intra-well dynamics is discussed. In the proximity of the resonance a rich intraband excitation spectrum is observed. The single particle excitation mechanisms are studied in the framework of Floquet theory elucidating the role of the driving frequency. The impact of the interatomic repulsive interactions is examined in detail yielding a strong influence on the tunneling period and the excitation probabilities. Finally, the dependence of the resonance upon a variation of the tunable parameters of the optical lattice is examined. Our analysis is based on the ab initio multi-configuration time-dependent Hartree method for bosons.

#### Two-body correlations and natural-orbital tomography in ultracold bosonic systems of definite parity

* S. Krönke and P. Schmelcher*

The relationship between natural orbitals, one-body coherences, and two-body correlations is explored for bosonic many-body systems of definite parity with two occupied single-particle states. We show that the strength of local two-body correlations at the parity-symmetry center characterizes the number-state distribution and controls the structure of nonlocal two-body correlations. A recipe for the experimental reconstruction of the natural-orbital densities and quantum depletion is derived. These insights into the structure of the many-body wave function are applied to the predicted quantum-fluctuation-induced decay of dark solitons.

#### Magnetic Kink States Emulated with Dipolar Superlattice Gases

* X. Yin, L. Cao. P. Schmelcher*

We propose an effective Ising spin chain constructed with dipolar quantum gases confined in a one-dimensional optical superlattice. Mapping the motional degree of freedom of a single particle in the lattice onto a pseudo-spin results in an effective Ising type chain dressed with transverse and longitudinal magnetic fields. The ground state of this effective Ising chain changes from a paramagnetic to a single-kink state as the dipolar interaction increases. Particularly in the single-kink state this effective chain permits emulations of magnetic kink effects. Being realizable with current experimental techniques, this effective Ising chain presents a unique platform for emulations of Ising physics and enriches the toolbox for quantum emulation of spin models by ultracold quantum gases.

#### Correlated quantum dynamics of a single atom collisionally coupled to an ultracold finite bosonic ensemble

* S. Krönke, J. Knörzer and P. Schmelcher*

We explore the correlated quantum dynamics of a single atom, regarded as an open system, with a spatio-temporally localized coupling to a finite bosonic environment. The single atom, initially prepared in a coherent state of low energy, oscillates in a one-dimensional harmonic trap and thereby periodically penetrates an interacting ensemble of NA bosons held in a displaced trap. We show that the inter-species energy transfer accelerates with increasing NA and becomes less complete at the same time. System-environment correlations prove to be significant except for times when the excess energy distribution among the subsystems is highly imbalanced. These correlations result in incoherent energy transfer processes, which accelerate the early energy donation of the single atom and stochastically favour certain energy transfer channels, depending on the instantaneous direction of transfer. Concerning the subsystem states, the energy transfer is mediated by non-coherent states of the single atom and manifests itself in singlet and doublet excitations in the finite bosonic environment. These comprehensive insights into the non-equilibrium quantum dynamics of an open system are gained by ab initio simulations of the total system with the recently developed multi-layer multi-configuration time-dependent Hartree method for bosons.

#### Beyond-mean-field study of a binary bosonic mixture in a state-dependent honeycomb lattice

* L. Cao, S. Krönke, J. Stockhofe, J. Simonet, K. Sengstock, D.-S. Lühmann and P. Schmelcher*

We investigate a binary mixture of bosonic atoms loaded into a state-dependent honeycomb lattice. For this system, the emergence of a so-called twisted-superfluid ground state was experimentally observed in Soltan-Panahi et al. [Nat. Phys. 8, 71 (2012)]. Theoretically, the origin of this effect is not understood. We perform numerical simulations of an extended single-band Bose-Hubbard model adapted to the experimental parameters employing the multilayer multiconfiguration time-dependent Hartree method for Bosons. Our results confirm the overall applicability of mean-field theory in the relevant parameter range, within the extended single-band Bose-Hubbard model. Beyond this, we provide a detailed analysis of correlation effects correcting the mean-field result. These have the potential to induce asymmetries in single shot time-of-flight measurements, but we find no indication of the patterns characteristic of the twisted superfluid. We comment on the restrictions of our model and possible extensions.

#### Negative-quench-induced excitation dynamics for ultracold bosons in one-dimensional lattices

* S.I. Mistakidis, L. Cao and P. Schmelcher*

The nonequilibrium dynamics following a quench of strongly repulsive bosonic ensembles in one-dimensional finite lattices is investigated by employing interaction quenches and/or a ramp of the lattice potential. Both sudden and time-dependent quenches are analyzed in detail. For the case of interaction quenches we address the transition from the strong repulsive to the weakly interacting regime, suppressing in this manner the heating of the system. The excitation modes such as the cradle process and the local breathing mode are examined via local density observables. In particular, the cradle mode is inherently related to the initial delocalization and, following a negative interaction quench, can be excited only for incommensurate setups with filling larger than unity. Alternatively, a negative quench of the lattice depth which favors the spatial delocalization is used to access the cradle mode for setups with filling smaller than unity. Our results shed light on possible schemes to control the cradle and the breathing modes. Finally, employing the notion of fidelity we study the dynamical response of the system after a diabatic or adiabatic parameter modulation for short and long evolution times. The evolution of the system is obtained numerically using the ab initio multilayer multiconfiguration time-dependent Hartree method for bosons, which permits us to follow nonequilibrium dynamics including the corresponding investigation of higher-band effects.

#### Interaction quench induced multimode dynamics of finite atomic ensembles

*S. Mistakidis, L. Cao, P. Schmelcher*

The correlated non-equilibrium dynamics of few-boson systems in one-dimensional finite lattices is investigated. Starting from weak interactions we perform a sudden interaction quench and employ the numerically exact multi-layer multi-configuration time-dependent Hartree method for bosons to obtain the resulting quantum dynamics. Focusing on the low-lying modes of the finite lattice we observe the emergence of density-wave tunneling, breathing and cradle-like processes. In particular, the tunneling induced by the quench leads to a 'global' density-wave oscillation. The resulting breathing and cradle modes are inherent to the local intrawell dynamics and connected to excited-band states. Moreover, the interaction quenches couple the density-wave and the cradle modes allowing for resonance phenomena. These are associated with an avoided-crossing in the respective frequency spectrum and lead to a beating dynamics for the cradle. Finally, complementing the numerical studies, an effective Hamiltonian in terms of the relevant Fock states is derived for the description of the spectral properties and the related resonant dynamics.

#### Quantum breathing dynamics of ultracold bosons in one-dimensional harmonic traps: Unraveling the pathway from few- to many-body systems

* R. Schmitz, S. Krönke, L. Cao, P. Schmelcher*

Following a “bottom-up approach” in understanding many-particle effects and dynamics we provide a systematic ab initio study of the dependence of the breathing dynamics of ultracold bosons in a one-dimensional (1D) harmonic trap on the number of bosons ranging from few to many. To this end, we employ the multilayer multiconfiguration time-dependent Hartree method for bosons (ML-MCTDHB) which has been developed very recently [ Krönke, Cao, Vendrell and Schmelcher New J. Phys. 15 063018 (2013)]. The beating behavior for two bosons is found numerically and consequently explained by an analytical approach. Drawing on this, we show how to compute the complete breathing mode spectrum in this case. We examine how the two-mode breathing behavior of two bosons evolves to the single-frequency behavior of the many-particle limit when adding more particles. In the limit of many particles, we numerically study the dependence of the breathing mode frequency on both the interaction strength as well as on the particle number. We provide an estimate for the parameter region where the mean-field description provides a valid approximation.

#### The multi-layer multi-configuration time-dependent Hartree method for bosons: Theory, implementation, and applications

* L. Cao, S. Krönke, O. Vendrell, P. Schmelcher*

We develop the multi-layer multi-configuration time-dependent Hartree method for bosons (ML-MCTDHB), a variational numerically exact ab initio method for studying the quantum dynamics and stationary properties of general bosonic systems. ML-MCTDHB takes advantage of the permutation symmetry of identical bosons, which allows for investigations of the quantum dynamics from few to many-body systems. Moreover, the multi-layer feature enables ML-MCTDHB to describe mixed bosonic systems consisting of arbitrary many species. Multi-dimensional as well as mixed-dimensional systems can be accurately and efficiently simulated via the multi-layer expansion scheme. We provide a detailed account of the underlying theory and the corresponding implementation. We also demonstrate the superior performance by applying the method to the tunneling dynamics of bosonic ensembles in a one-dimensional double well potential, where a single-species bosonic ensemble of various correlation strengths and a weakly interacting two-species bosonic ensemble are considered.

#### Non-equilibrium quantum dynamics of ultra-cold atomic mixtures: the multi-layer multi-configuration time-dependent Hartree method for bosons

* S. Krönke, L. Cao, O. Vendrell, P. Schmelcher*

We develop and apply the multi-layer multi-configuration time-dependent Hartree method for bosons, which represents an ab initio method for investigating the non-equilibrium quantum dynamics of multi-species bosonic systems. Its multi-layer feature allows for tailoring the wave function ansatz to describe intra- and inter-species correlations accurately and efficiently. To demonstrate the beneficial scaling and efficiency of the method, we explored the correlated tunneling dynamics of two species with repulsive intra- and inter-species interactions, to which a third species with vanishing intra-species interaction was weakly coupled. The population imbalances of the first two species can feature a temporal equilibration and their time evolution significantly depends on the coupling to the third species. Bosons of the first and second species exhibit a bunching tendency, whose strength can be influenced by their coupling to the third species.

#### Two-component few-fermion mixtures in a one-dimensional trap: Numerical versus analytical approach

*I. Brouzos, P. Schmelcher*

We explore a few-fermion mixture consisting of two components that are repulsively interacting and confined in a one-dimensional harmonic trap. Different scenarios of population imbalance ranging from the completely imbalanced case where the physics of a single impurity in the Fermi sea is discussed to the partially imbalanced and equal population configurations are investigated. For the numerical calculations the multiconfigurational time-dependent Hartree method is employed, extending its application to few-fermion systems. Apart from numerical calculations we generalize our ansatz for a correlated pair wave function proposed recently [ I. Brouzos and P. Schmelcher Phys. Rev. Lett. 108 045301 (2012)] for bosons to mixtures of fermions. From weak to strong coupling between the components the energies, the densities and the correlation properties of one-dimensional systems change vastly with an upper limit set by fermionization where for infinite repulsion all fermions can be mapped to identical ones. The numerical and analytical treatments are in good agreement with respect to the description of this crossover. We show that for equal populations each pair of different component atoms splits into two single peaks in the density while for partial imbalance additional peaks and plateaus arise for very strong interaction strengths. The case of a single-impurity atom shows rich behavior of the energy and density as we approach fermionization and is directly connected to recent experiments [ G. Zürn et al. Phys. Rev. Lett. 108 075303 (2012)].

#### Controlled Excitation and Resonant Acceleration of Ultracold Few-Boson Systems by Driven Interactions in a Harmonic Trap

*I. Brouzos, P. Schmelcher*

### Project C8

#### Hydration shell effects in the relaxation dynamics of photoexcited Fe-II complexes in water

*P. Nalbach, A. J. A. Achner, M. Frey, M. Grosser, C. Bressler, M. Thorwart*

We study the relaxation dynamics of photoexcited Fe-II complexes dissolved in water and identify the relaxation pathway which the molecular complex follows in presence of a hydration shell of bound water at the interface between the complex and the solvent. Starting from a low-spin state, the photoexcited complex can reach the high-spin state via a cascade of different possible transitions involving electronic as well as vibrational relaxation processes. By numerically exact path integral calculations for the relaxational dynamics of a continuous solvent model, we find that the vibrational life times of the intermittent states are of the order of a few ps. Since the electronic rearrangement in the complex occurs on the time scale of about 100 fs, we find that the complex first rearranges itself in a high-spin and highly excited vibrational state, before it relaxes its energy to the solvent via vibrational relaxation transitions. By this, the relaxation pathway can be clearly identified. We find that the life time of the vibrational states increases with the size of the complex (within a spherical model), but decreases with the thickness of the hydration shell, indicating that the hydration shell acts as an additional source of fluctuations.

#### Photon-assisted confinement-induced resonances for ultracold atoms

*V. Leyton, M. Roghani, V. Peano, M. Thorwart*

We solve the two-particle s-wave scattering for an ultracold-atom gas confined in a quasi-one-dimensional trapping potential which is periodically modulated. The interaction between the atoms is included via Fermi’s pseudopotential. For a modulated isotropic transverse harmonic confinement, the atomic center of mass and relative degrees of freedom decouple and an exact solution is possible. The modulation opens additional photon-assisted resonant scattering channels. Applying the Bethe-Peierls boundary condition, we obtain the general scattering solution of the time-dependent Floquet-Schrödinger equation which is universal at low energies. The effective one-dimensional scattering length can be controlled by the external driving.

#### Quantification of non-Markovian effects in the Fenna-Matthews-Olson complex

*C. Mujica-Martinez, P. Nalbach, M. Thorwart*

The excitation energy transfer dynamics in the Fenna-Matthews-Olson complex is quantified in terms of a non-Markovianity measure based on the time evolution of the trace distance of two quantum states. We use a system description derived from experiments and different environmental fluctuation spectral functions, which are obtained either from experimental data or from molecular dynamics simulations. These exhibit, in all cases, a nontrivial structure with several peaks attributed to vibrational modes of the pigment-protein complex. Such a structured environmental spectrum can, in principle, give rise to strong non-Markovian effects. We present numerically exact real-time path-integral calculations for the transfer dynamics and find, in all cases, a monotonic decrease of the trace distance with increasing time which renders a Markovian description valid.

#### Nonequilibrium quantum fluctuation relations for harmonic systems in nonthermal environments

*D. Pagel, P. Nalbach, A. Alvermann, H. Fehske, M. Thorwart*

We formulate exact generalized nonequilibrium fluctuation relations for the quantum mechanical harmonic oscillator coupled to multiple harmonic baths. Each of the different baths is prepared in its own individual (in general nonthermal) state. Starting from the exact solution for the oscillator dynamics we study fluctuations of the oscillator position as well as of the energy current through the oscillator under general nonequilibrium conditions. In particular, we formulate a fluctuation–dissipation relation for the oscillator position autocorrelation function that generalizes the standard result for the case of a single bath at thermal equilibrium. Moreover, we show that the generating function for the position operator fulfils a generalized Gallavotti–Cohen-like relation. For the energy transfer through the oscillator, we determine the average energy current together with the current fluctuations. Finally, we discuss the generalization of the cumulant generating function for the energy transfer to nonthermal bath preparations.

#### Crossover from coherent to incoherent quantum dynamics due to sub-Ohmic dephasing

*P. Nalbach, M. Thorwart*

We report exact results for the influence of purely sub-Ohmic dephasing on the dynamics of a quantum two-level system. From response functions, we determine a crossover coupling strength between oscillatory coherent and overdamped dynamics. Surprisingly, we find no overdamping even at arbitrary large dephasing for spectra with spectral exponent.

#### Organic pi-conjugated copolymers as molecular charge qubits

*C. A. Mujica-Martinez, P. Nalbach, M. Thorwart*

We propose a design for molecular charge qubits based on π-conjugated block copolymers and determine their electronic structure as well as their vibrational active modes. By tuning the length of the oligomers, the tunnel coupling in the charge qubit and its decoherence properties due to molecular vibrations can be chemically engineered. Coherent oscillations result with quality factors of up to 104 at room temperature. In turn, the molecular vibrational spectrum induces strong non-Markovian electronic effects which support the survival of quantum coherence.

#### Noise-Induced Förster Resonant Energy Transfer between Orthogonal Dipoles in Photoexcited Molecules

* P. Nalbach, I. Pugliesi, H. Langhals, M. Thorwart*

#### Quantum noise properties of multiphoton transitions in driven nonlinear resonators

*V. Leyton, V. Peano, M. Thorwart*

We investigate the quantum noise properties of a weakly nonlinear Duffing resonator in the deep quantum regime, where only a few quanta are excited. This regime is dominated by the appearance of coherent multiphoton resonances in the nonlinear response of the resonator to the modulation. We determine simple expressions for the photon noise spectrum and find that the multiphoton resonances also induce a multiple peak structure in that spectrum. When the corresponding multiphoton Rabi oscillations are underdamped, zero-temperature quantum fluctuations determine comparable populations of all quasienergy states which belong to a resonant multiphoton doublet. Most interestingly, the quantum fluctuations probe the multiphoton transitions by inducing several peaks in the noise spectrum of the resonator observables. In particular, the noise of the photon number contains complete information about the multiphoton states and their stationary populations via pairs of nearly symmetric peaks at opposite frequencies. Their widths are determined by the damping of the Rabi oscillations and their heights are proportional to the stationary nonequilibrium populations. A finite detuning from a multiphoton resonance generates a quasielastic noise peak at zero frequency. In addition, we relate the stationary populations of the quasienergy states with an effective quantum temperature and discuss the role of a finite temperature.

### Project C9

#### Theory of enhanced interlayer tunneling in optically driven high Tc superconductors

*J. Okamoto, A. Cavalleri, L. Mathey*

Motivated by recent pump-probe experiments indicating enhanced coherent c-axis transport in underdoped YBCO, we study Josephson junctions periodically driven by optical pulses. We propose a mechanism for this observation by demonstrating that a parametrically driven Josephson junction shows an enhanced imaginary part of the low-frequency conductivity when the driving frequency is above the plasma frequency, implying an effectively enhanced Josephson coupling. We generalize this analysis to a bilayer system of Josephson junctions modeling YBCO. Again, the Josephson coupling is enhanced when the pump frequency is blue-detuned to either of the two plasma frequencies of the material. We show that the emergent driven state is a genuine, non-equilibrium superconducting state, in which equilibrium relations between the Josephson coupling, current fluctuations, and the critical current no longer hold.

#### Designing exotic many-body states of atomic spin and motion in photonic crystals

*M. T. Manzoni, L. Mathey, D. E. Chang*

Cold atoms coupled to photonic crystals constitute an exciting platform for exploring quantum many-body physics. Here we investigate the strong coupling between atomic internal ("spin") degrees of freedom and motion, which arises from spin-dependent forces associated with the exchange of guided photons. We show that this system can realize a remarkable and extreme limit of quantum spin-orbital systems, where both the direct spin exchange between neighboring sites and the kinetic energy of the orbital motion vanish. We find that this previously unexplored system has a rich phase diagram of emergent orders, including spatially dimerized spin-entangled pairs, a fluid of composite particles comprised of joint spin-phonon excitations, phonon-induced Neel ordering, and a fractional magnetization plateau associated with trimer formation.

#### Magnus expansion approach to parametric oscillator systems in a thermal bath

*B. Zhu, T. Rexin, L. Mathey*

We develop a Magnus formalism for periodically driven systems which provides an expansion both in the driving term and the inverse driving frequency, applicable to isolated and dissipative systems. We derive explicit formulas for a driving term with a cosine dependence on time, up to fourth order. We apply these to the steady state of a classical parametric oscillator coupled to a thermal bath, which we solve numerically for comparison. Beyond dynamical stabilization at second order, we find that the higher orders further renormalize the oscillator frequency, and additionally create a weakly renormalized effective temperature. The renormalized oscillator frequency is quantitatively accurate almost up to the parametric instability, as we confirm numerically. Additionally, a cut-off dependent term is generated, which indicates the break-down of the hierarchy of time scales of the system, as a precursor to the instability. Finally, we apply this formalism to a parametrically driven chain, as an example for the control of the dispersion of a many-body system.

arXiv:1604.01010

http://arxiv.org/abs/1604.01010

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#### Sudden-quench dynamics of Bardeen-Cooper-Schrieffer states in deep optical lattices

*Marlon Nuske, L. Mathey, Eite Tiesinga*

We determine the exact dynamics of an initial Bardeen-Cooper-Schrieffer (BCS) state of ultracold atoms in a deep hexagonal optical lattice. The dynamical evolution is triggered by a quench of the lattice potential such that the interaction strength Uf is much larger than the hopping amplitude Jf. The quench initiates collective oscillations with frequency ∣∣Uf|/2π in the momentum occupation numbers and imprints an oscillating phase with the same frequency on the BCS order parameter Δ. The oscillation frequency of Δ is not reproduced by treating the time evolution in mean-field theory. In our theory, the momentum noise (i.e., density-density) correlation functions oscillate at frequency ∣∣Uf|/2π as well as at its second harmonic. For a very deep lattice, with zero tunneling energy, the oscillations of momentum occupation numbers are undamped. Nonzero tunneling after the quench leads to dephasing of the different momentum modes and a subsequent damping of the oscillations. The damping occurs even for a finite-temperature initial BCS state, but not for a noninteracting Fermi gas. Furthermore, damping is stronger for larger order parameter and may therefore be used as a signature of the BCS state. Finally, our theory shows that the noise correlation functions in a honeycomb lattice will develop strong anticorrelations near the Dirac point.

#### Noise correlations of two-dimensional Bose gases

*V. P. Singh, L. Mathey*

We analyze density-density correlations of expanding clouds of weakly interacting two-dimensional Bose gases below and above the Berezinskii-Kosterlitz-Thouless transition, with particular focus on short-time expansions. During time-of-flight expansion, phase fluctuations of the trapped system translate into density fluctuations, in addition to the density fluctuations that exist in situ. We calculate the correlations of these fluctuations both in real space and in momentum space and derive analytic expressions in momentum space. Below the transition, the correlation functions show an oscillatory behavior, controlled by the scaling exponent of the quasicondensed phase, due to constructive interference. We argue that this can be used to extract the scaling exponent of the quasicondensate experimentally. Above the transition, the interference is rapidly suppressed when the atoms travel an average distance beyond the correlation length. This can be used to distinguish the two phases qualitatively.

#### Quantum Phases of quadrupolar Fermi gases in optical lattices

*S. G. Bhongale, L. Mathey, E. Zhao, S. F. Yelin, M. Lemeshko*

We introduce a new platform for quantum simulation of many-body systems based on non-spherical particles with zero dipole moment but possessing a significant value of the electric quadrupole moment. Considering a quadrupolar quantum gas trapped in a 2D optical lattice, we show that the peculiar symmetry and broad tunability of the quadrupole-quadrupole interactions results in a rich phase diagram encompassing unconventional BCS and charge density wave phases, and paves the way to create topological superfluid ground states of px + i py symmetry. Quadrupolar species, such as metastable alkaline-earth atoms and homonuclear molecules, are stable against chemical reactions and collapse and are readily available in experiment at high densities.

Phys. Rev. Lett. 110, 155301 (2013)

http://arxiv.org/abs/1211.3317

#### Unconventional Spin Density Waves in Dipolar Fermi Gases

*S. G. Bhongale, L. Mathey, S. Tsai, C. W. Clark, E. Zhao*

The conventional spin density wave (SDW) phase (Overhauser, 1962), as found in antiferromagnetic metal for example (Fawcett 1988), can be described as a condensate of particle-hole pairs with zero angular momentum, $\ell=0$, analogous to a condensate of particle-particle pairs in conventional superconductors. While many unconventional superconductors with Cooper pairs of finite $\ell$ have been discovered, their counterparts, density waves with non-zero angular momenta, have only been hypothesized in two-dimensional electron systems (Nayak, 2000). Using an unbiased functional renormalization group analysis, we here show that spin-triplet particle-hole condensates with $\ell=1$ emerge generically in dipolar Fermi gases of atoms (Lu, Burdick, and Lev, 2012) or molecules (Ospelkaus et al., 2008; Wu et al.) on optical lattice. The order parameter of these exotic SDWs is a vector quantity in spin space, and, moreover, is defined on lattice bonds rather than on lattice sites. We determine the rich quantum phase diagram of dipolar fermions at half-filling as a function of the dipolar orientation, and discuss how these SDWs arise amidst competition with superfluid and charge density wave phases.

Phys. Rev. A 87, 043604 (2012)

http://arxiv.org/abs/1209.2671

#### Decay of a superfluid current of ultra-cold atoms in a toroidal trap

*Amy C. Mathey, Charles W. Clark, L. Mathey*

Using a numerical implementation of the truncated Wigner approximation, we simulate the experiment reported by Ramanathan et al. in Phys. Rev. Lett. 106, 130401 (2011), in which a Bose-Einstein condensate is created in a toroidal trap and set into rotation via a Gauss-Laguerre beam. A potential barrier is then placed in the trap to study the decay of the superflow. We find that the current decays via thermally activated phase slips, which can also be visualized as vortices crossing the barrier region in radial direction. Adopting the notion of critical velocity used in the experiment, we determine it to be lower than the local speed of sound at the barrier. This result is in agreement with the experimental findings, but in contradiction to the predictions of the Gross-Pitaevskii equation. This emphasizes the importance of thermal fluctuations in the experiment.