Metastable electronic states and nonlinear response for high-intensity optical pulses

Abstract

In this paper we propose and demonstrate that the ultrafast nonlinear optical response of atoms may be accurately calculated in terms of metastable states obtained as solutions of the stationary Schrodinger equation including the quasi-static applied electric field. We first develop the approach in the context of an exactly soluble one-dimensional atomic model with delta-function potential, as this allows comparison between the exact ultrafast nonlinear optical response and our approximate approach, both in adiabatic approximation and beyond. These ideas are then applied to a three-dimensional hydrogen-like atom and yield similar excellent agreement between the metastable state approach and simulations of the Schrodinger equation for off-resonant excitation. Finally, our approach yields a model for the ultrafast nonlinear optical response with no free parameters. It can potentially replace the light–matter interaction treatment currently used in optical filamentation, and we present a numerical example of application to femtosecond pulse propagation.