arXiv subjects

Martin Eckstein

Publications and source records attributed to Martin Eckstein.

At least 109 records · Page 6Linked to original sources

arXiv2017

Ultrafast Electronic Band Gap Control in an Excitonic Insulator

We report on the nonequilibrium dynamics of the electronic structure of the layered semiconductor Ta$_2$NiSe$_5$ investigated by time- and angle-resolved photoelectron spectroscopy. We show that below the critical excitation density of $F_{C} = 0.2$ mJ cm$^{-2}$, the band gap $narrows$ transiently, while it is $enhanced$ above $F_{C}$. Hartree-Fock calculations reveal that this effect can be explained by the presence of the low-temperature excitonic insulator phase of Ta$_2$NiSe$_5$, whose order parameter is connected to the gap size. This work demonstrates the ability to manipulate the band gap of Ta$_2$NiSe$_5$ with light on the femtosecond time scale.

cond-mat.str-el↗

arXiv2017

Photo-induced enhancement of excitonic order

We study the dynamics of excitonic insulators coupled to phonons. Without phonon couplings, the linear response is given by the damped amplitude oscillations of the order parameter with frequency equal to the minimum band gap. A phonon coupling to the interband transfer integral induces two types of long-lived collective oscillations of the amplitude, one originating from the phonon dynamics and the other from the phase mode, which becomes massive. We show that even for small phonon coupling, a photo-induced enhancement of the exciton condensation and the gap can be realized. Using the Anderson pseudo-spin picture, we argue that the origin of the enhancement is a cooperative effect of the massive phase mode and the Hartree shift induced by the photo excitation. We also discuss how the enhancement of the order and the collective modes can be observed with time-resolved photo-emission spectroscopy.

cond-mat.str-el↗

arXiv2017

Nonequilibrium steady states and transient dynamics of conventional superconductors under phonon driving

We perform a systematic analysis of the influence of phonon driving on the superconducting Holstein model coupled to heat baths by studying both the transient dynamics and the nonequilibrium steady state (NESS) in the weak and strong electron-phonon coupling regimes. Our study is based on the nonequilibrium dynamical mean-field theory, and for the NESS we present a Floquet formulation adapted to electron-phonon systems. The analysis of the phonon propagator suggests that the effective attractive interaction can be strongly enhanced in a parametric resonant regime because of the Floquet side bands of phonons. While this may be expected to enhance the superconductivity (SC), our fully self-consistent calculations, which include the effects of heating and nonthermal distributions, show that the parametric phonon driving generically results in a suppression or complete melting of the SC order. In the strong coupling regime, the NESS always shows a suppression of the SC gap, the SC order parameter and the superfluid density as a result of the driving, and this tendency is most prominent at the parametric resonance. Using the real-time nonequilibrium DMFT formalism, we also study the dynamics towards the NESS, which shows that the heating effect dominates the transient dynamics, and SC is weakened by the external modulations, in particular at the parametric resonance. In the weak coupling regime, we find that the SC fluctuations above the transition temperature are generally weakened under the driving. The strongest suppression occurs again around the parametric resonances because of the efficient energy absorption.

cond-mat.supr-con↗

arXiv2017

Ultrafast doublon dynamics in photo-excited 1T-TaS$_2$

Strongly correlated systems exhibit intriguing properties caused by intertwined microscopic in- teractions that are hard to disentangle in equilibrium. Employing non-equilibrium time-resolved photoemission spectroscopy on the quasi-two-dimensional transition-metal dichalcogenide 1T-TaS$_2$, we identify a spectroscopic signature of double occupied sites (doublons) that are reflects fundamental Mott physics. Doublon-hole recombination is estimated to occur on time scales of one electronic hopping cycle $\hbar/J\approx$ 14 fs. Despite strong electron-phonon coupling the dynamics can be explained by purely electronic effects captured by the single band Hubbard model, where thermalization is fast in the small-gap regime. Qualitative agreement with the experimental results however requires the assumption of an intrinsic hole-doping. The sensitivity of the doublon dynamics on the doping level provides a way to control ultrafast processes in such strongly correlated materials.

cond-mat.str-el↗

arXiv2017

Probing the fluctuations of the optical properties in time-resolved spectroscopy

We show that, in optical pump-probe experiments on bulk samples, the statistical distribution of the intensity of ultrashort light pulses after the interaction with a nonequilibrium complex material can be used to measure the time-dependent noise of the current in the system. We illustrate the general arguments for a photo-excited Peierls material. The transient noise spectroscopy allows to measure to what extent electronic degrees of freedom dynamically obey the fluctuation-dissipation theorem, and how well they thermalize during the coherent lattice vibrations. The proposed statistical measurement developed here provides a new general framework to retrieve dynamical information on the excited distributions in nonequilibrium experiments which could be extended to other degrees of freedom of magnetic or vibrational origin.

cond-mat.str-el↗

arXiv2017

Nonequilibrium GW+EDMFT: Antiscreening and inverted populations from nonlocal correlations

We study the dynamics of screening in photo-doped Mott insulators with long-ranged interactions using a nonequilibrium implementation of the $GW$ plus extended dynamical mean field theory ($GW$+EDMFT) formalism. Our study demonstrates that the complex interplay of the injected carriers with bosonic degrees of freedom (charge fluctuations) can result in long-lived transient states with properties that are distinctly different from those of thermal equilibrium states. Systems with strong nonlocal interactions are found to exhibit a self-sustained population inversion of the doublons and holes. This population inversion leads to low-energy antiscreening which can be detected in time-resolved electron-energy loss spectra.

cond-mat.str-el↗

arXiv2017

Hund's coupling driven photo-carrier relaxation in the two-band Mott insulator

We study the relaxation dynamics of photo-carriers in the paramagnetic Mott insulating phase of the half-filled two-band Hubbard model. Using nonequilibrium dynamical mean field theory, we excite charge carriers across the Mott gap by a short hopping modulation, and simulate the evolution of the photo-doped population within the Hubbard bands. We observe an ultrafast charge-carrier relaxation driven by emission of local spin excitations with an inverse relaxation time proportional to the Hund's coupling. The photo-doping generates additional side-bands in the spectral function, and for strong Hund's coupling, the photo-doped population also splits into several resonances. The dynamics of the local many-body states reveals two effects, thermal blocking and kinetic freezing, which manifest themselves when the Hund's coupling becomes of the order of the temperature or the bandwidth, respectively. These effects, which are absent in the single-band Hubbard model, should be relevant for the interpretation of experiments on correlated materials with multiple active orbitals. In particular, the features revealed in the non-equilibrium energy distribution of the photo-carriers are experimentally accessible, and provide information on the role of the Hund's coupling in these materials.

cond-mat.str-el↗

arXiv2017

Two-channel Kondo physics in a periodically driven single-impurity Anderson model

We investigate a quantum dot (Anderson impurity) coupled to metallic leads, with a time-periodic voltage bias across the device. Using a time-dependent Schrieffer-Wolff transformation, we show that the Floquet Hamiltonian of the model can be mapped onto a two-channel Kondo model, in which the impurity is screened by separate conduction bands corresponding to parity-even and odd superpositions of the metallic leads. By changing the frequency and amplitude of the perturbation, one can tune the system to a quantum critical point with symmetric coupling of the impurity to both channels. For the understanding of the driven state, energy absorption from the drive must be considered: Although the absorption at the impurity is balanced by the energy flow into the conduction band, locally it leads to non-thermal distribution functions which can have a detrimental effect on the Kondo physics. However, a numerical simulation demonstrates that the absorption can be systematically suppressed at a fixed value of the induced couplings by increasing the frequency, so that the time-averaged dynamics in the driven one-channel Anderson model can be used to study the critical behavior of the two-channel model.

cond-mat.str-el↗

arXiv2017

Bypassing the energy-time uncertainty in time-resolved photoemission

The energy-time uncertainty is an intrinsic limit for time-resolved experiments imposing a tradeoff between the duration of the light pulses used in experiments and their frequency content. In standard time-resolved photoemission, this limitation maps directly onto a tradeoff between the time resolution of the experiment and the energy resolution that can be achieved on the electronic spectral function. Here we propose a protocol to disentangle the energy and time resolutions in photoemission. We demonstrate that dynamical information on all time scales can be retrieved from time-resolved photoemission experiments using suitably shaped light pulses of quantum or classical nature. As a paradigmatic example, we study the dynamical buildup of the Kondo peak, a narrow feature in the electronic response function arising from the screening of a magnetic impurity by the conduction electrons. After a quench, the electronic screening builds up on timescales shorter than the inverse width of the Kondo peak and we demonstrate that the proposed experimental scheme could be used to measure the intrinsic time scales of such electronic screening. The proposed approach provides an experimental framework to access the nonequilibrium response of collective electronic properties beyond the spectral uncertainty limit and will enable the direct measurement of phenomena such as excited Higgs modes and, possibly, the retarded interactions in superconducting systems.

cond-mat.str-el↗

arXiv2017

Designing spin and orbital exchange Hamiltonians with ultrashort electric field transients

We demonstrate how electric fields with arbitrary time profile can be used to control the time-dependent parameters of spin and orbital exchange Hamiltonians. Analytic expressions for the exchange constants are derived from a time-dependent Schrieffer-Wolff transformation, and the validity of the resulting effective Hamiltonian is verified for the case of a quarter-filled two-orbital Hubbard model, by comparing to the results of a full nonequilibrium dynamical mean-field theory simulation. The ability to manipulate Hamiltonians with arbitrary time-dependent fields, beyond the paradigm of Floquet engineering, opens the possibility to control intertwined spin and orbital order using laser or THz pulses which are tailored to minimize electronic excitations.

cond-mat.str-el↗

arXiv2016

Ultrafast switching of composite order in A$_3$C$_{60}$

We study the controlled manipulation of the Jahn-Teller metal state of fulleride compounds using nonequilibrium dynamical mean field theory. This anomalous metallic state is a spontaneous orbital-selective Mott phase, which is characterized by one metallic and two insulating orbitals. Using protocols based on transiently reduced hopping amplitudes or periodic electric fields, we demonstrate the possibility to switch orbitals between Mott insulating and metallic on a sub-picosecond timescale, and to rotate the order parameter between three equivalent states that can be distinguished by their anisotropic conductance. The Jahn-Teller metal phase of alkali-doped fullerides thus provides a promising platform for ultrafast persistent memory devices.

cond-mat.str-el↗

arXiv2016

Nonequilibrium Dynamical Cluster Approximation study of the Falicov-Kimball Model

We use a nonequilibrium implementation of the dynamical cluster approximation (DCA) to study the effect of short-range correlations on the dynamics of the two-dimensional Falicov-Kimball model after an interaction quench. As in the case of single-site dynamical mean field theory, thermalization is absent in DCA simulations, and for quenches across the metal-insulator boundary, nearest-neighbor charge correlations in the nonthermal steady state are found to be larger than in the thermal state with identical energy. We investigate to what extent it is possible to define an effective temperature of the trapped state after a quench. Based on the ratio between the lesser and retarded Green's function we conclude that a roughly thermal distribution is reached within the energy intervals corresponding to the momentum-patch dependent subbands of the spectral function. The effectively different chemical potentials of these distributions however lead to a very hot, or even negative, effective temperature in the energy intervals between these subbands.

cond-mat.str-el↗

arXiv2016

Interference stabilization of autoionizing states in molecular $N_2$ studied by time- and angular-resolved photoelectron spectroscopy

An autoionizing resonance in molecular N$_2$ is excited by an ultrashort XUV pulse and probed by a subsequent weak IR pulse, which ionizes the contributing Rydberg states. Time- and angular-resolved photoelectron spectra recorded with a velocity map imaging spectrometer reveal two electronic contributions with different angular distributions. One of them has an exponential decay rate of $20\pm5$ fs, while the other one is shorter than 10 fs. This observation is interpreted as a manifestation of interference stabilization involving the two overlapping discrete Rydberg states. A formalism of interference stabilization for molecular ionization is developed and applied to describe the autoionizing resonance. The results of calculations reveal, that the effect of the interference stabilization is facilitated by rotationally-induced couplings of electronic states with different symmetry.

physics.atom-ph↗

arXiv2016

Slow down of the electronic relaxation close to the Mott transition

We investigate the time-dependent reformation of the quasiparticle peak in a correlated metal near the Mott transition, after the system is quenched into a hot electron state and equilibrates with an environment which is colder than the Fermi-liquid crossover temperature. Close to the transition, we identify a purely electronic bottleneck timescale, which depends on the spectral weight around the Fermi energy in the bad metallic phase in a non-linear way. This timescale can be orders of magnitude larger than the bare electronic hopping time, so that a separation electronic and lattice timescales may break down. The results are obtained using nonequilibrium dynamical mean-field theory and a slave-rotor representation of the Anderson impurity model.

cond-mat.str-el↗

arXiv2016

Nonequilibrium self-energy functional approach to the dynamical Mott transition

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 observed. 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.

cond-mat.str-el↗

arXiv2016

Nonequilibrium variational-cluster approach to real-time dynamics in the Fermi-Hubbard model

The nonequilibrium 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 nonequilibrium 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.

cond-mat.str-el↗

arXiv2016

Photo-induced gap closure in an excitonic insulator

We study the dynamical phase transition out of an excitonic insulator phase after photo-excitation using a time-dependent extension of the selfconsistent GW method. We connect the evolution of the photoemission spectra to the dynamics of the excitonic order parameter and identify two dynamical phase transition points marked by a slowdown in the relaxation: one critical point is connected with the trapping in a nonthermal state with reduced exciton density and the second corresponds to the thermal phase transition. The transfer of kinetic energy from the photoexcited carriers to the exciton condensate is shown to be the main mechanism for the gap melting. We analyze the low energy dynamics of screening, which strongly depends on the presence of the excitonic gap, and argue that it is difficult to interpret the static component of the screened interaction as the effective interaction of some low energy model. Instead we propose a phenomenological measure for the effective interaction which indicates that screening has minor effects on the low energy dynamics.

cond-mat.str-el↗

arXiv2016

Alignment and characterization of the two-stage time delay compensating XUV monochromator

We present the design, implementation and alignment procedure for a two-stage time delay compensating monochromator. The setup spectrally filters the radiation of a high-order harmonic generation source providing wavelength-selected XUV pulses with a bandwidth of 300 to 600~meV in the photon energy range of 3 to 50~eV. XUV pulses as short as $12\pm3$~fs are demonstrated. Transmission of the 400~nm (3.1~eV) light facilitates precise alignment of the monochromator. This alignment strategy together with the stable mechanical design of the motorized beamline components enables us to automatically scan the XUV photon energ in pump-probe experiments that require XUV beam pointing stability. The performance of the beamline is demonstrated by the generation of IR-assisted sidebands in XUV photoionization of argon atoms.

physics.ins-det↗