Relaxation of photo-excited hot carriers beyond multi-temperature models: General theory description verified by experiments on Pb/Si(111)

TL;DR

This paper introduces an extended rate-equation model that accounts for non-thermal electronic carriers and first-principles electron-phonon interactions, providing a more accurate description of hot carrier relaxation in metals, verified by experiments on Pb/Si(111).

Contribution

The work presents a novel, comprehensive model that explicitly includes non-thermal carriers and detailed electron-phonon coupling data, improving understanding of ultrafast carrier dynamics beyond traditional multi-temperature models.

Findings

Enhanced agreement with experimental data at short times (<0.3ps).

Demonstrated electron-mediated energy transfer between phonon groups.

Showed delayed equilibration of phonon subsystems due to different coupling strengths.

Abstract

The equilibration of electronic carriers in metals after excitation by an ultra-short laser pulse provides an important class of non-equilibrium phenomena in metals and allows measuring the effective electron-phonon coupling parameter. Since the observed decay of the electronic distribution is governed by the interplay of both electron-electron and electron-phonon scattering, the interpretation of experimental data must rely on models that ideally should be easy to handle, yet accurate. In this work, an extended rate-equation model is proposed that explicitly includes non-thermal electronic carriers while at the same time incorporating data from first-principles calculations of the electron-phonon coupling via Eliashberg-Migdal theory. The model is verified against experimental data for thin Pb films grown on Si(111). Improved agreement between theory and experiment at short times (<0.3ps) due to non-thermal electron contributions is found. Moreover, the rate equations allow for widely different coupling strength to different phonon subsystems. Consequently, an indirect, electron-mediated energy transfer between strongly and weakly coupled groups of phonons can be observed in the simulations that leads to a retarded equilibration of the subsystems only after several picoseconds.