A Molecular Dynamics Study of Laser-Excited Gold

TL;DR

This study uses advanced molecular dynamics simulations to accurately model laser-induced melting in gold, aligning with experimental electron diffraction data by incorporating hot electron energy loss mechanisms.

Contribution

It introduces a novel approach that accounts for hot electron energy transport, resolving previous discrepancies between simulations and experiments in laser-excited gold.

Findings

Simulations match experimental electron diffraction data.

Energy loss via hot electrons is crucial for accurate modeling.

Threshold energies for melting are consistent with experimental observations.

Abstract

The structural evolution of laser-excited systems of gold has previously been measured through ultrafast MeV electron diffraction. However, there has been a long-standing inability of atomistic simulations to provide a consistent picture of the melt process, concluding in large discrepancies between the predicted threshold energy density for complete melt, as well as the transition between heterogeneous and homogeneous melting. We make use of two-temperature classical molecular dynamics simulations utilizing three highly successful interatomic potentials and reproduce electron diffraction data presented by Mo et al. We recreate the experimental electron diffraction data employing both a constant and temperature-dependent electron-ion equilibration rate. In all cases we are able to match time-resolved electron diffraction data, and find consistency between atomistic simulations and experiments, only by allowing laser energy to be transported away from the interaction region. This additional energy-loss pathway, which scales strongly with laser fluence, we attribute to hot electrons leaving the target on a timescale commensurate with melting.