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arXiv:0903.2332 · Physical Review Letters

Nonequilibrium Steady State of Photoexcited Correlated Electrons in the Presence of Dissipation

Naoto Tsuji, Takashi Oka, Hideo Aoki

Published Jul 24, 2009• 128 citations
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Abstract

We present a framework to determine nonequilibrium steady states in strongly correlated electron systems in the presence of dissipation. This is demonstrated for a correlated electron (Falicov-Kimball) model attached to a heat bath and irradiated by an intense pump light, for which an exact solution is obtained with the Floquet method combined with the nonequilibrium dynamical mean-field theory. On top of a Drude-like peak indicative of photometallization as observed in recent pump-probe experiments, new nonequilibrium phenomena are predicted to emerge, where the optical conductivity exhibits dip and kink structures around the frequency of the pump light, a midgap absorption arising from photoinduced Floquet subbands, and a negative attenuation (gain) due to a population inversion.

DOI
10.1103/physrevlett.103.047403

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We present a framework to determine nonequilibrium steady states in strongly correlated electron systems in the presence of dissipation. This is demonstrated for a correlated electron (Falicov-Kimball) model attached to a heat bath and irradiated by an intense pump light, for which an exact solution is obtained with the Floquet method combined with the nonequilibrium dynamical mean-field theory. On top of a Drude-like peak indicative of photometallization as observed in recent pump-probe experiments, new nonequilibrium phenomena are predicted to emerge, where the optical conductivity exhibits dip and kink structures around the frequency of the pump light, a midgap absorption arising from photoinduced Floquet subbands, and a negative attenuation (gain) due to a population inversion.
To reveal the nature of the photoinduced insulator-metal transition, we show that an exact analysis of the Falicov-Kimball model subject to external ac electric fields becomes possible with Floquet's method combined with the nonequilibrium dynamical mean-field theory. The nonequilibrium steady state that appears during irradiation of a pump light is shown to be determined if the dissipation in a certain heat-bath model is introduced. This has enabled us to predict that novel features characteristic of the photoexcited steady states, i.e., negative weight (gain) in the low-energy region and dip structures around the photon energy of the pump light, should be observed in the optical conductivity. Special emphasis is put on the role of dissipation, for which we elaborate the dependence of the steady state on the strength of dissipation and the temperature of the heat bath.
In order to investigate photoinduced insulator-metal transitions observed in correlated electron systems, we propose a new theoretical method, where we combine a Floquet-matrix method for AC-driven systems with the dynamical mean-field theory. The method can treat nonequilibrium steady states exactly beyond the linear-response regime. We have applied the method to the Falicov-Kimball model coupled to AC electric fields, and numerically obtained the spectral function, the nonequilibrium distribution function and the current-voltage characteristic. The results show that intense AC fields indeed drive Mott-like insulating states into photoinduced metallic states in a nonlinear way.
We propose to combine the Floquet formalism for systems in ac fields with the dynamical mean-field theory to study correlated electron systems periodically driven out of equilibrium by external fields such as intense laser light. This approach has a virtue that we can nonperturbatively include both the correlation effects and nonlinear effects due to the driving field, which is imperative in analyzing recent experiments for photoinduced phase transitions. In solving the problem, we exploit a general theorem that the Hamiltonian in a Floquet matrix form can be exactly diagonalized for single-band noninteracting systems. As a demonstration, we have applied the method to the Falicov-Kimball model in intense ac fields to calculate the spectral function. The result shows that photoinduced midgap states emerge from strong ac fields, triggering an insulator-metal transition.
We investigate a photoinduced insulator-metal transition in the Falicov-Kimball model with the dynamical mean-field theory (DMFT) extended to nonequilibrium systems in periodic modulations in time. When the photon energy of the pump light is Ω≈ ( U : the interaction strength), a Drude-like peak is found to grow in the optical conductivity spectrum, which is an evidence that the system is driven into a metallic state. During the transition, the band gap does not collapse, whereas the distribution function exhibits a non-monotonic behaviour away from the Fermi distribution. This indicates that the transition cannot be accounted for by heating effects, but creation of photo-carriers is responsible.
We develop the theory for nonresonant Raman scattering of strongly correlated electrons in time-resolved pump- probe experiments. The electrons are initially pumped with an intense pulse of light and then a probe pulse measures the Raman response function after an adjustable time delay. We describe how the width of the probe pulse and the strength of the electron correlations affect the Raman cross section. The theory is developed for the case of B1g symmetry, where incident and scattered light are polarized perpendicular to each other. We illustrate the exact solution with the Falicov-Kimball model, which is solved via nonequilibrium dynamical mean-field theory.
The real-time dynamics of interacting electrons out of equilibrium contains detailed microscopic information about electronically correlated materials, which can be read out with time-resolved optical spectroscopy. The reflectivity that is typically measured in pump-probe experiments is related to the nonequilibrium optical conductivity. We show how to express this quantity in terms of real-time Green's functions using dynamical mean-field theory. As an application we study the electrical response of the Falicov-Kimball model during the ultrafast buildup of the gapped phase at large interaction.