Electronic nonequilibrium effect in ultrafast-laser-irradiated solids

Abstract: This paper describes the effects of electronic nonequilibrium in a simulation of ultrafast laser irradiation of materials. The simulation scheme based on tight-binding molecular dynamics, in which the electronic populations are traced with a combined Monte Carlo and Boltzmann equation, enables the modeling of nonequilibrium, nonthermal, and nonadiabatic (electron-phonon coupling) effects simultaneously. The electron-electron thermalization is described within the relaxation-time approximation, which automatically restores various known limits such as instantaneous thermalization (the thermalization time ${\tau}{e-e} \rightarrow 0$) and Born-Oppenheimer approximation (${\tau}{e-e} \rightarrow \infty$). The results of the simulation suggest that the non-equilibrium state of the electronic system slows down electron-phonon coupling with respect to the electronic equilibrium case in all studied materials: metals, semiconductors, and insulators. In semiconductors and insulators, it also alters the damage threshold of ultrafast nonthermal phase transitions induced by modification of the interatomic potential due to electronic excitation. It is demonstrated that the models that exclude electron-electron thermalization (using the assumption of ${\tau}_{e-e} \rightarrow \infty$, such as BO or Ehrenfest approximations) may produce qualitatively different results, and a reliable model should include all three effects: electronic nonequilibrium, nonadiabatic electron-ion coupling, and nonthermal evolution of interatomic potential.