Theory for the Dependence of Optical Second Harmonic Generation Intensity on Non-equilibrium Electron Temperatures at Metal Surfaces

Abstract

We present a theory for the electron-temperature dependence $T_{el}$ of optical second harmonic generation (SHG). Such an analysis is required to study the dynamics of metallic systems with many hot electrons not at equilibrium with the lattice. Using a tight-binding theory for the nonlinear susceptibility \cwtel and the Fresnel coefficients we present results for the SHG intensity \iwtel for a Cu monolayer. In the case of linear optical response we find that the intensity will decrease monotonously for increasing $T_{el}$. In agreement with experiment we find a frequency range where \iwtel may be enhanced or reduced depending on electron temperature. Note, \cwtel rather than the Fresnel coefficients determines essentially the temperature dependence. Our theory yields also that SHG probes effects due to hot electrons more sensitively than linear optics. We also discuss the $T_{el}$-dependence of SHG for Au and Ag.