Thermalization after photoexcitation from the perspective of optical spectroscopy

TL;DR

This paper investigates how a photoexcited charge carrier in the Holstein model thermalizes, showing that both static and dynamic correlations reach thermal equilibrium, supporting quasithermal descriptions in ultrafast spectroscopy.

Contribution

It demonstrates that static and dynamic fermionic correlations thermalize simultaneously in a nonequilibrium Holstein model after photoexcitation.

Findings

Static fermionic correlations match Gibbs ensemble values.

Dynamic current-current correlations also thermalize.

Both types of correlations reach the same temperature.

Abstract

We analyze the thermalization of a photoexcited charge carrier coupled to a single branch of quantum phonons within the Holstein model. To this end, we calculate the far-from-equilibrium time evolution of a pure many-body state and compare it with predictions of the thermal Gibbs ensemble. We show that at strong enough carrier excitation, the nonequilibrium system evolves towards a thermal steady state. Our analysis is based on two classes of observables. First, the occupations of fermionic momenta, which are the eigenvalues of the one-particle density matrix, match in the steady state the values in the corresponding Gibbs ensemble. This indicates thermalization of static fermionic correlations on the entire lattice. Second, the dynamic current-current correlations, including the time-resolved optical conductivity, also take the form of their thermal counterparts. Remarkably, both static and dynamic fermionic correlations thermalize with identical temperatures. Our results suggest that the subsequent relaxation processes, observed in time-resolved ultrafast spectroscopy, may be efficiently described by applying quasithermal approaches, e.g., multi-temperature models.