We establish the nonequilibrium thermal phases of a voltage driven antiferromagnetic Mott insulator in three dimensions, realised at steady state under a voltage bias. Starting from the Keldysh action for the half filled Hubbard model we derive an effective Langevin equation for the `slow' magnetic variables. The coupling of electrons to these degrees of freedom determine the transport properties. At low temperature we find a voltage-driven discontinuous insulator-metal transition, along with hysteresis. We map the suppression of the Néel temperature $T_N$ and pseudogap temperature $T_{pg}$ with increasing voltage, and discover that the biased Mott insulator has a finite temperature insulator-metal transition. The low temperature results resolve an experimental puzzle about hysteresis, and the thermal results make testable predictions on spectra and nonlinear transport.
We present a formalism based on nonequilibrium dynamical mean field theory (DMFT) which allows to compute the time-resolved X-ray absorption spectrum (XAS) of photo-excited solids. By applying this formalism to the photo-doped half-filled and quarter-filled two-orbital Hubbard models in the Mott insulating regime we clarify how the time-resolved XAS signal reflects the nonequilibrium population of different local states. Apart from the missing broadening associated with continuum excitations, the atomic XAS spectrum computed with the nonthermal state populations provides a good approximation t…
We define, compute and analyze the nonequilibrium differential optical conductivity of the one-dimensional extended Hubbard model at half-filling after applying a pump pulse, using the time-dependent density matrix renormalization group method. The melting of the Mott insulator is accompanied by a suppression of the local magnetic moment and ensuing photogeneration of doublon-holon pairs. The differential optical conductivity reveals $(i)$ mid-gap states related to parity-forbidden optical states, and $(ii)$ strong renormalization and hybridization of the excitonic resonance and the absorption…
Suppression of rectification at metal--Mott-insulator interfaces, which is previously shown by numerical solutions to the time-dependent Schrödinger equation and experiments on real devices, is reinvestigated theoretically by nonequilibrium Green's functions. The one-dimensional Hubbard model is used for a Mott insulator. The effects of attached metallic electrodes are incorporated into the self-energy. A scalar potential originating from work-function differences and satisfying the Poisson equation is added to the model. For the electron density, we decompose it into three parts. One is obtai…
We study real-time dynamics of a charge carrier introduced into undoped Mott insulator propagating under a constant electric field F on the t-J ladder and square lattice. We calculate quasistationary current. In both systems adiabatic regime is observed followed by the positive differential resistivity (PDR) at moderate fields where carrier mobility is determined. Quantitative differences between ladder and 2-dimensional (2D) system emerge when at large fields both systems enter negative differential resistivity (NDR) regime. In the ladder system Bloch-like oscillations prevail, while in 2D th…
Electronic properties of heterostructures in which a finite number of Mott-insulator layers are sandwiched by semi-infinite metallic leads are investigated by using the dynamical-mean-field method combined with the Keldysh Green's function technique to account for the finite bias voltage between the leads. Current across the junction is computed as a function of bias voltage. Electron spectral functions in the interacting region are shown to evolve by an applied bias voltage. This effect is measurable by photoemission spectroscopy and scanning tunneling microscopy. Further predictions are made…
Competition between ordered phases, and their associated phase transitions, are significant in the study of strongly correlated systems. Here we examine one aspect, the nonequilibrium dynamics of a photoexcited Mott-Peierls system, using an effective Peierls-Hubbard model and exact diagonalization. Near a transition where spin and charge become strongly intertwined, we observe anti-phase dynamics and a coupling-strength-dependent suppression or enhancement in the static structure factors. The renormalized bosonic excitations coupled to a particular photoexcited electron can be extracted, which…
We use time-evolution techniques for (infinite) matrix-product-states to calculate, directly in the thermodynamic limit, the time-dependent photoemission spectra and dynamic structure factors of the half-filled Hubbard chain after pulse irradiation. These quantities exhibit clear signatures of the photoinduced phase transition from insulator to metal that occurs because of the formation of so-called $η$ pairs. In addition, the spin dynamic structure factor loses spectral weight in the whole momentum space, reflecting the suppression of antiferromagnetic correlations due to the buildup of $η$-p…
We develop a method for extracting the steady nonequilibrium current from studies of driven isolated systems, applying it to the model of one-dimensional Mott insulator at high temperatures. While in the nonintegrable model the nonequilibrium conditions can be accounted by internal heating, the integrability leads to a strongly nonlinear dc response with vanishingly small dc conductivity in the linear--response regime. The finding is consistent with equilibrium results for dc limit of the optical conductivity determined in the presence of a weak and decreasing perturbation.
Photo-induced metallic states in a Mott insulator are studied for the half-filled, one-dimensional Hubbard model with the time-dependent density matrix renormalization group. An irradiation of strong AC field is found to create a linear dispersion in the optical spectrum (current-current correlation) in the nonequilibrium steady state reminiscent of the Tomonaga-Luttinger liquid for the doped Mott insulator in equilibrium. The spin spectrum in nonequilibrium retains the des Cloizeaux-Pearson mode with the spin velocity differing from the charge velocity. The mechanism of the photocarrier-dopin…
We study the current response of an AC driven dissipative Mott insulator system, a normal quantum dot array, using an analytical Keldysh field theory approach. Deep in the Mott insulator regime, the nonequilibrium steady state (NESS) response resembles a resistively shunted Josephson array, with a nonequilibrium Mott insulating to conductor transition as the drive frequency Ω is increased. The diamagnetic component of the NESS in the conducting phase is anomalous, implying negative inductance, strikingly reminiscent of the η-pairing phase of a Josephson array with negative phase stiffness. How…
We extend the nonequilibrium dynamical mean field (DMFT) formalism to inhomogeneous systems by adapting the "real-space" DMFT method to Keldysh Green's functions. Solving the coupled impurity problems using strong-coupling perturbation theory, we apply the formalism to homogeneous and inhomogeneous layered systems with strong local interactions and up to 39 layers. We study the diffusion of doublons and holes created by photo-excitation in a Mott insulating system, the time-dependent build-up of the polarization and the current induced by a linear voltage bias across a multi-layer structure, a…
Photo-excited strongly correlated systems can exhibit intriguing non-thermal phases, but the theoretical investigation of them poses significant challenges. In this work, we introduce a generalized Gibbs ensemble type description for long-lived photo-doped states in Mott insulators. This framework enables systematic studies of photo-induced phases based on equilibrium methods, as demonstrated here for the one-dimensional extended Hubbard model. We determine the nonequilibrium phase diagram, which features $η$-pairing and charge density wave phases in a wide doping range, and reveal physical pr…
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…
Photodoped states are widely observed in laser-excited Mott insulators, in which charge excitations are quickly created and can exist beyond the duration of the external driving. Despite the fruitful experimental explorations, theoretical studies on the microscopic models face the challenge to simultaneously deal with exponentially separated time scales, especially in multi-band systems, where the long-time behaviors are often well beyond the reach of state-of-the-art numerical tools. Here, we address this difficulty by introducing a steady-state description of photodoped Mott insulators using…
We study the nonequilibrium dynamics of photoexcited electrons in the narrow-gap Mott insulator VO$_2$. The initial stages of relaxation are treated using a quantum Boltzmann equation methodology, which reveals a rapid ($\sim$ femtosecond time scale) relaxation to a pseudothermal state characterized by a few parameters that vary slowly in time. The long-time limit is then studied by a Hartree-Fock methodology, which reveals the possibility of nonequilibrium excitation to a new metastable $M_1$ metal phase that is qualitatively consistent with a recent experiment. The general physical picture o…
Understanding strongly correlated systems driven out of equilibrium is a challenging task necessitating the simultaneous treatment of quantum mechanics,dynamical constraints and strong interactions. A Mott insulator subjected to a uniform and static electric field is prototypical, raising key questions such as the fate of Bloch oscillations with increasing correlation strength, the approach to a steady state DC transport regime and the role of dissipation in it, and electric field driven phase transitions. We develop here an effective large-N Keldysh field theory for studying nonequilibrium tr…
We investigate the effect of nonlocal interactions on the photo-doped Mott insulating state of the two-dimensional Hubbard model using a nonequilibrium generalization of the dynamical cluster approximation. In particular, we compare the situation where the excitonic states are lying within the continuum of doublon-holon excitations to a set-up where the excitons appear within the Mott gap. In the first case, the creation of nearest-neighbor doublon-holon pairs by excitations across the Mott gap results in enhanced excitonic correlations, but these excitons quickly decay into uncorrelated doubl…
We present a systematic study of the nonequilibrium steady states (NESS) in Mott insulators driven by DC or AC electric fields, based on the Floquet dynamical mean-field theory. The results are analyzed using a generalized tunneling formula for the current, which is reminiscent of the Meir-Wingreen formula and provides insights into the relevant physical processes. In the DC case, the spectrum of the NESSs exhibits Wannier-Stark (WS) states associated with the lower and upper Hubbard bands. In addition, there emerge WS sidebands from many-body states. Using the tunneling formula, we demonstrat…
Nonequilibrium dynamics in correlated materials has attracted attention due to the possibility of characterizing, tuning, and creating complex ordered states. To understand the photoinduced microscopic dynamics, especially the linkage under realistic pump conditions between transient states and remnant elementary excitations, we performed nonperturbative simulations of various time-resolved spectroscopies. We used the Mott antiferromagnetic insulator as a model platform. The transient dynamics of multi-particle excitations can be attributed to the interplay between Floquet virtual states and a…
We use a self-consistent strong-coupling expansion for the self-energy (perturbation theory in the hopping) to describe the nonequilibrium dynamics of strongly correlated lattice fermions. We study the three-dimensional homogeneous Fermi-Hubbard model driven by an external electric field showing that the damping of the ensuing Bloch oscillations depends on the direction of the field, and that for a broad range of field strengths, a long-lived transient prethermalized state emerges. This long-lived transient regime implies that thermal equilibrium may be out of reach of the time scales accessib…
We use a nonequilibrium implementation of extended dynamical mean field theory to study the effect of dynamical screening in photo-excited Mott insulators. The insertion of doublons and holes adds low-energy screening modes and leads to a reduction of the Mott gap. The coupling to low-energy bosonic modes further- more opens new relaxation channels and significantly speeds up the thermalization process. We also consider the effect of the energy distribution of the doped carriers on the screening.
In this work, we explore the possibility of emergent nonequilibrium steady states arising from the electric-field-driven Mott insulator via the Keldysh-Floquet dynamical mean field theory (DMFT), which can determine the fully-interacting, nonequilibrium steady-state Green's functions with the noninteracting counterparts as an input to the DMFT self-consistency loop. Unlike the retarded component, obtaining the lesser Green's function for the noninteracting system presents an important obstacle since the thermalization of the noninteracting system still requires a precise understanding of the d…
We study a model for photovoltaic energy collection consisting of a Mott insulating layer in presence of acoustic phonons, coupled to two wide-band fermion leads at different chemical potentials and driven into a nonequilibrium steady state by a periodic electric field. We treat electron correlations with nonequilibrium dynamical mean-field theory (DMFT) using the so-called auxiliary master equation approach as impurity solver and include dissipation by acoustic phonons via the Migdal approximation. For a small hybridization to the leads, we obtain a peak in the photocurrent as a function of t…
Inspired by the physics of rare earth nickelates, we study the photoemission (PES) and resonant inelastic X-ray scattering (RIXS) spectra of a correlated electron system with two types of insulating sublattices. Sublattice A is characterized by a hybridization gap and a low-spin state, while sublattice B features a Mott gap and a local magnetic moment. We show how the coupling of these two qualitatively different insulating states affects the dynamics of photo-induced charge carriers and how the nonequilibrium states manifest themselves in the PES and RIXS signals. In particular, we find that …
Using nonequilibrium dynamical mean-field theory, we compute the time evolution of the current in a Mott insulator after a strong electric field is turned on. We observe the formation of a quasistationary state in which the current is almost time-independent although the system is constantly excited. At moderately strong fields this state is stable for quite long times. The stationary current exhibits a threshold behavior as a function of the field, in which the threshold increases with the Coulomb interaction and vanishes as the metal-insulator transition is approached.
To study excitonic effects on high-harmonic generation (HHG) in Mott insulators, we investigate pumped nonequilibrium dynamics in the one-dimensional extended Hubbard model. By employing time-dependent calculations based on the exact diagonalization and infinite time-evolving block decimation methods, we find the strong enhancement of the HHG intensity around the exciton energy. The subcycle analysis in the sub-Mott-gap regime shows that the intensity region of the time-resolved spectrum around the exciton energy splits into two levels and oscillates following the driving electric field. This …
We study the nonequilibrium steady state of a Mott insulator coupled to a thermostat and driven by a constant electric field, starting from weak fields, until the dielectric breakdown, and beyond. We find that the conventional Zener picture does not describe the steady-state physics. In particular, the current at weak field is found to be controlled by the dissipation. Moreover, in connection with the electric-field-driven dimensional crossover, we find that the dielectric breakdown occurs when the field strength is on the order of the Mott gap of the corresponding lower-dimensional system. We…
Nonequilibrium states induced by an applied bias voltage (V) and the corresponding current-voltage characteristics of one-dimensional models describing band and Mott insulators are investigated theoretically by using nonequilibrium Green's functions. We attach the models to metallic electrodes whose effects are incorporated into the self-energy. Modulation of the electron density and the scalar potential coming from the additional long-range interaction are calculated self-consistently within the Hartree approximation. For both models of band and Mott insulators with length L_C, the bias volta…
The elucidation of nonequilibrium states in strongly correlated systems holds the key to emergence of novel quantum phases. The nonequilibrium-induced insulator-to-metal transition is particularly interesting since it reflects the fundamental nature of competition between itinerancy and localization of the charge degrees of freedom. We investigate pulse-excited insulator-to-metal transition of the half-filled one-dimensional extended Hubbard model. Calculating the time-dependent optical conductivity with the time-dependent density-matrix renormalization group, we find that strong mono- and hal…
We compute the time-resolved photoemission spectrum after photo-doping in a two-dimensional Mott-Hubbard insulator. We find that the relaxation rate of high-energy photo-doped electrons in the paramagnetic phase scales with the strength of the nearest-neighbor spin correlations, which implies a pronounced increase of the relaxation times with temperature and excitation density. Finite doping, in contrast, opens additional scattering channels and leads to a faster relaxation. To obtain our results we have implemented a nonequilibrium version of the dynamical cluster approximation (DCA), which, …
The formalism for exactly calculating the retarded and advanced Green's functions of strongly correlated lattice models in a uniform electric field is derived within dynamical mean-field theory. To illustrate the method, we solve for the nonequilibrium density of states of the Hubbard model in both the metallic and Mott insulating phases at half-filling (with an arbitrary strength electric field) by employing the numerical renormalization group as the impurity solver. This general approach can be applied to any strongly correlated lattice model in the limit of large dimensions.
We investigate how fast and how effective photocarrier excitation can modify the exchange interaction $J_\mathrm{ex}$ in the prototype Mott-Hubbard insulator. We demonstrate an ultrafast quenching of $J_\mathrm{ex}$ both by evaluating exchange integrals from a time-dependent response formalism and by explicitly simulating laser-induced spin precession in an antiferromagnet that is canted by an external magnetic field. In both cases, the electron dynamics is obtained from nonequilibrium dynamical mean-field theory. We find that the modified $J_\mathrm{ex}$ emerges already within a few electron …
Time-dependent nonequilibrium properties of a strongly correlated electron system driven by large electric fields is obtained by means of solving the time-dependent Schrödinger equation for the many-body wave function numerically in one dimension. While the insulator-to-metal transition depends on the electric field and the interaction, the metallization is found to be described in terms of a universal Landau-Zener quantum tunneling among the many-body levels. These processes induces current oscillation for small systems, while give rise to finite resistivity through dissipation for larger sys…
We study the finite-momentum spin dynamics in the one-dimensional XXZ spin chain within the Ising-type regime at high temperatures using density autocorrelations within linear response theory and real-time propagation of nonequilibrium densities. While for the nonintegrable model results are well consistent with normal diffusion, the finite-size integrable model unveils the coexistence of anomalous and normal diffusion in different regimes of time. In particular, numerical results show a Gaussian relaxation at smallest nonzero momenta which we relate to nonzero stiffness in a grand canonical e…
Nonlinear transport in the one dimensional Hubbard model at half-filling under a finite bias voltage is investigated by the adaptive time-dependent density matrix renormalization group method. For repulsive on-site interaction, dielectric breakdown of the Mott insulating ground state to a current-carrying nonequilibrium steady state is clearly observed when the voltage exceeds the charge gap. It is found that by increasing the voltage further the current-voltage characteristics are scaled only by the charge gap and the scaling curve exhibits almost linear dependence on the voltage whose slope …
We use nonequilibrium dynamical mean-field theory in combination with a recently implemented strong-coupling impurity solver to investigate the relaxation of a Mott insulator after a laser excitation with frequency comparable to the Hubbard gap. The time evolution of the double occupancy exhibits a crossover from a strongly damped transient at short times towards an exponential thermalization at long times. In the limit of strong interactions, the thermalization time is consistent with the exponentially small decay rate for artificially created doublons, which was measured in ultracold atomic …
Femtosecond time-resolved core-level photoemission spectroscopy with a free-electron laser is used to measure the atomic-site specific charge-order dynamics in the charge-density-wave/Mott insulator 1T-TaS2. After strong photoexcitation, a prompt loss of charge order and subsequent fast equilibration dynamics of the electron-lattice system are observed. On the time scale of electron-phonon thermalization, about 1 ps, the system is driven across a phase transition from a long-range charge ordered state to a quasi-equilibrium state with domain-like short-range charge and lattice order. The exper…
Ultrafast pump-probe spectroscopy with high temporal and spectral resolutions provides new insight into ultrafast nonequilibrium phenomena. We propose that transient interference between pump and probe pulses is realized in pump-probe spectroscopy of band and Mott insulators, which can be observed only after recent developments of ultrafast spectroscopic techniques. A continuum structure in the excitation spectrum of band insulators is found to act as a medium for storing the spectral information of the pump pulse, and the spectrum detected by the probe pulse is interfered with by the medium, …
Nonlinear phononics holds the promise for controlling properties of quantum materials on the ultrashort timescale. Using nonequilibrium dynamical mean-field theory, we solve a model for the description of organic solids, where correlated electrons couple nonlinearly to a quantum phonon mode. Unlike previous works, we exactly diagonalize the local phonon mode within the noncrossing approximation to include the full phononic fluctuations. By exciting the local phonon in a broad range of frequencies near resonance with an ultrashort pulse, we show it is possible to induce a Mott insulator-to-meta…
We develop a real space theory of the voltage bias driven transition from a Mott insulator to a correlated metal. Within our Keldysh mean field approach the problem reduces to a self-consistency scheme for the charge and spin profiles in this open system. We solve this problem for a two dimensional antiferromagnetic Mott insulator at zero temperature. The charge and spin magnitude is uniform over the system at zero bias, but a bias $V$ leads to spatial modulation over a lengthscale $ξ(V)$ near the edges. $ξ(V)$ grows rapidly and becomes comparable to system size as $V$ increases towards a thre…
Sub-cycle doublon-holon dynamics in one-dimensional Mott insulators revealed by two-color high-harmonic spectroscopy
Purdue University（普渡大学）；Los Alamos National Laboratory（洛斯阿拉莫斯国家实验室）；Colorado State University（科罗拉多州立大学）；Brookhaven National Laboratory（布鲁克海文国家实验室）；Joint Attosecond Science Laboratory (JASLab), National Research Council of Canada and University of Ottawa（联合阿秒科学实验室（JASLab），加拿大国家研究委员会和渥太华大学）
Using a nonequilibrium implementation of the extended dynamical mean field theory (EDMFT) we simulate the relaxation after photo excitation in a strongly correlated electron system with antiferromagnetic spin interactions. We consider the $t$-$J$ model and focus on the interplay between the charge- and spin-dynamics in different excitation and doping regimes. The appearance of string states after a weak photo excitation manifests itself in a nontrivial scaling of the relaxation time with the exchange coupling and leads to a correlated oscillatory evolution of the kinetic energy and spin-spin c…
We study the photoinduced ultrafast dynamics in relativistic Mott insulators, i.e., Mott insulators with strong spin-orbit coupling. For this purpose, we consider a minimal one-band Hubbard model on lattices with square and triangular symmetries, as relevant for layered transition metal compounds such as Sr$_2$IrO$_4$. Depending on the lattice and the spin-orbit coupling, the systems have canted antiferromagnetic or $120^\circ$ order. They are excited by simulating a short laser pulse, and the dynamics is solved using nonequilibrium dynamical mean-field theory. The pulse generates hot carriers…
We present time-resolved magneto-optical spectroscopy on the magnetic Mott-Hubbard-insulating Kitaev spin liquid candidate $α$-RuCl$_3$ to investigate the nonequilibrium dynamics of its antiferromagnetically ordered zigzag groundstate after photoexcitation. A systematic study of the transient magnetic linear dichroism under different experimental conditions (temperature, external magnetic field, photoexcitation density) gives direct access to the dynamical interplay of charge excitations with the zigzag ordered state on ultrashort time scales. We observe a rather slow initial demagnetization (…
A model for nonequilibrium dynamical mean-field theory is constructed for the infinite dimensional Hubbard lattice. We impose nonequilibrium by expressing the physical orbital as a superposition of a left-($L$) moving and right-($R$) moving electronic state with the respective chemical potential $μ_L$ and $μ_R$. Using the second-order iterative perturbation theory we calculate the quasi-particle properties as a function of the chemical potential bias between the $L$ and $R$ movers, i.e. $Φ= μ_L - μ_R$. The evolution of the nonequilibrium quasi-particle spectrum is mapped out as a function of t…
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 …
We propose a novel approach to nonequilibrium real-time dynamics of quantum impurities models coupled to biased non-interacting leads, such as those relevant to quantum transport in nanoscale molecular devices. The method is based on a Diagrammatic Monte Carlo sampling of the real-time perturbation theory along the Keldysh contour. We benchmark the method on a non-interacting resonant level model and, as a first non-trivial application, we study zero temperature non-equilibrium transport through a vibrating molecule.
