Application of the anisotropic bond model to second-harmonic generation from amorphous media

Abstract

As a step toward analyzing second-harmonic generation (SHG) from crystalline Si nanospheres in glass, we develop an anisotropic bond model (ABM) that expresses SHG in terms of physically meaningful parameters and provides a detailed understanding of the basic physics of SHG on the atomic scale. Nonlinear-optical (NLO) responses are calculated classically via the four fundamental steps of optics: evaluate the local field at a given bond site, solve the force equation for the acceleration of the charge, calculate the resulting radiation, then superpose the radiation from all charges. The ABM goes beyond previous bond models by including the complete set of underlying contributions: retardation (RD), spatial-dispersion (SD), and magnetic (MG) effects, in addition to the anharmonic restoring force acting on the bond charge. We apply the ABM to obtain analytic expressions for SHG from amorphous materials under Gaussian-beam excitation. These materials represent an interesting test case not only because they are ubiquitous but also because the anharmonic-force contribution that dominates the SHG response of crystalline materials and ordered interfaces vanishes by symmetry. Using the paraxial-ray approximation, we reduce the results to the isotropic case in two limits, that where the linear restoring force dominates (glasses), and that where it is absent (metals). Both forward- and backscattering geometries are discussed. Estimated signal strengths and conversion efficiencies for fused silica appear to be in general agreement with data, where available. Predictions are made that allow additional critical tests of these results.