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arXiv:1705.10866 · Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Relaxation of nonequilibrium populations after a pump: the breaking of Mathiessen's rule

James K. Freericks, Omadillo Abdurazakov, Alexander F. Kemper

Published May 8, 2017• 1 citation
arXivHTMLPDF

Abstract

From the early days of many-body physics, it was realized that the self-energy governs the relaxation or lifetime of the retarded Green’s function. So it seems reasonable to directly extend those results into the nonequilibrium domain. But experiments and calculations of the response of quantum materials to a pump show that the relationship between the relaxation and the self-energy only holds in special cases. Experimentally, the decay time for a population to relax back to equilibrium and the linewidth measured in a linear-response angle-resolved photoemission spectroscopy differ by large amounts. Theoretically, aside from the weak-coupling regime where the relationship holds, one also finds deviations and additionally one sees violations of Mathiessen’s rule. In this work, we examine whether looking at an effective transport relaxation time helps to analyze the decay times of excited populations as they relax back to equilibrium. We conclude that it may do a little better, but it has a fitting parameter for the overall scale which must be determined.

DOI
10.1117/12.2261872

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From the early days of many-body physics, it was realized that the self-energy governs the relaxation or lifetime of the retarded Green’s function. So it seems reasonable to directly extend those results into the nonequilibrium domain. But experiments and calculations of the response of quantum materials to a pump show that the relationship between the relaxation and the self-energy only holds in special cases. Experimentally, the decay time for a population to relax back to equilibrium and the linewidth measured in a linear-response angle-resolved photoemission spectroscopy differ by large amounts. Theoretically, aside from the weak-coupling regime where the relationship holds, one also finds deviations and additionally one sees violations of Mathiessen’s rule. In this work, we examine whether looking at an effective transport relaxation time helps to analyze the decay times of excited populations as they relax back to equilibrium. We conclude that it may do a little better, but it has a fitting parameter for the overall scale which must be determined.
We examine the exact equation of motion for the relaxation of populations of strongly correlated electrons after a nonequilibrium excitation by a pulsed field, and prove that the populations do not change when the Green's functions have no average time dependence. We show how the average time dependence enters into the equation of motion to lowest order and describe what governs the relaxation process of the electron populations in the long‐time limit. While this result may appear, on the surface, to be required by any steady‐state solution, the proof is nontrivial, and provides new critical insight into how nonequilibrium populations relax, which goes beyond the assumption that they thermalize via a simple relaxation rate determined by the imaginary part of the self‐energy, or that they can be described by a quasi‐equilibrium condition with a Fermi‐Dirac distribution and a time‐dependent temperature. We also discuss the implications of this result to approximate theories, which may not satisfy the exact relation in the equation of motion.
We compare the decay rates of excited populations directly calculated within a Keldysh formalism to the equation of motion of the population itself for a Hubbard-Holstein model in two dimensions. While it is true that these two approaches must give the same answer, it is common to make a number of simplifying assumptions, within the differential equation for the populations, that allows one to interpret the decay in terms of hot electrons interacting with a phonon bath. Here, we show how care must be taken to ensure an accurate treatment of the equation of motion for the populations due to the fact that there are identities that require cancellations of terms that naively look like they contribute to the decay rates. In particular, the average time dependence of the Green’s functions and self-energies plays a pivotal role in determining these decay rates.
We derive frequency moment sum rules for the retarded electronic Green's function and self-energy of the Holstein model for both equilibrium and nonequilibrium cases. We also derive sum rules for the phonon propagator in equilibrium and nonequilibrium. These sum rules allow one to benchmark nonequilibrium calculations and help with interpreting the behavior of electrons driven out of equilibrium by an applied electric field. We exactly evaluate the sum rules when the system is in the atomic limit. We also discuss the application of these sum rules to pump/probe experiments like time-resolved angle-resolved photoemission spectroscopy.
We derive frequency moment sum rules for the retarded electronic Green's function and self-energy of the Holstein model for both equilibrium and nonequilibrium cases. We also derive sum rules for the phonon propagator in equilibrium and nonequilibrium. These sum rules allow one to benchmark nonequilibrium calculations and help with interpreting the behavior of electrons driven out of equilibrium by an applied electric field. We exactly evaluate the sum rules when the system is in the atomic limit. We also discuss the application of these sum rules to pump/probe experiments like time-resolved angle-resolved photoemission spectroscopy.
We examine electron-electron mediated relaxation following ultrafast electric field pump excitation of the fermionic degrees of freedom in the Falicov-Kimball model for correlated electrons. The results reveal a dichotomy in the temporal evolution of the system as one tunes through the Mott metal-to-insulator transition: in the metallic regime relaxation can be characterized by evolution toward a steady state well described by Fermi-Dirac statistics with an increased effective temperature; however, in the insulating regime this quasithermal paradigm breaks down with relaxation toward a nonthermal state with a complicated electronic distribution as a function of momentum. We characterize the behavior by studying changes in the energy, photoemission response, and electronic distribution as functions of time. This relaxation may be observable qualitatively on short enough time scales that the electrons behave like an isolated system not in contact with additional degrees of freedom which would act as a thermal bath, especially when using strong driving fields and studying materials whose physics may manifest the effects of correlations.
Within the nonequilibrium Green's function framework, we systematically analyze the momentum relaxation dynamics of strongly coupled impurities in three-dimensional nondegenerate quantum gases. Using the Hartree-Fock approximation, we establish that the impurity velocity exhibits exponential decay asymptotically. When the impurity velocity is much lower than the thermal velocity of the gas atoms, the relaxation time $\ensuremath{\tau}$ is governed entirely by the self-energy evaluated at zero momentum and zero frequency, $\mathrm{\ensuremath{\Sigma}}(\mathbf{p}=0;\ensuremath{\omega}=0)$. Furthermore, via virial expansion theory, $\ensuremath{\tau}$ admits a systematic expansion in powers of the fugacity $z\ensuremath{\equiv}{e}^{\ensuremath{\beta}\ensuremath{\mu}}$. The leading-order term precisely recovers the Boltzmann semiclassical result, while higher-order corrections capture quantum many-body effects beyond the semiclassical approximation.