Theory of out-of-equilibrium electron and phonon dynamics in metals after ultrafast laser excitation

TL;DR

This paper develops a microscopic model to accurately describe ultrafast electron and phonon dynamics in metals after laser excitation, revealing deviations from traditional models and highlighting the role of phonon-dependent electron-phonon coupling.

Contribution

It introduces a parameter-free out-of-equilibrium model that captures ultrafast dynamics beyond the two-temperature approximation in various metals.

Findings

Strong deviations from the two-temperature model on picosecond timescales.

Phonon-mode dependent electron-phonon coupling significantly influences relaxation.

Electronic system mediates indirect phonon-phonon coupling during lattice equilibration.

Abstract

The out-of-equilibrium dynamics of electrons and phonons upon laser excitation are often described by the two-temperature model, which assumes that both subsystems are separately in thermal equilibrium. However, recent experiments show that this description is not sufficient to describe the out-of-equilibrium dynamics on ultrashort timescales. Here, we extend and apply a parameter-free microscopic out-of-equilibrium model to describe the ultrafast laser-induced system dynamics of archetypical metallic systems such as gold, aluminum, iron, nickel, and cobalt. We report strong deviations from the two-temperature model on the picosecond timescale for all the materials studied, even for those where the assumption of separate thermal equilibriums seemed less restrictive, like in gold. Furthermore, we demonstrate the importance of the phonon-mode dependent electron-phonon coupling for the relaxation process and reveal the significance of this channel in the lattice equilibration through an indirect coupling between phonons via the electronic system.