Experimental and theoretical study of second and third harmonic generation in amorphous silicon

We report contrasted experimental and theoretical results on second and third harmonic generation from an amorphous silicon nanolayer. We perform this study by analysing the harmonic optical signals generated when fs and ps pulses tuned at 800nm and 1064nm, respectively, interact with the material. We measure second and third harmonic efficiencies as functions of angle of incidence and compare with numerical simulations based on a microscopic hydrodynamic model that accounts for different possible contributions to the nonlinear polarization. We measure and estimate the efficiencies of the nonlinear signals using no assumptions about effective surface or volume nonlinearities, enabling proper explanations about the microscopic origins of SH and TH signals arising from the amorphous silicon nanolayer.