Second and third harmonic waves excited by focused Gaussian beams

Harmonic generation by tightly-focused Gaussian beams is finding important applications, primarily in nonlinear microscopy. It is often naively assumed that the nonlinear signal is generated predominantly in the focal region. However, the intensity of Gaussian-excited electromagnetic harmonic waves is sensitive to the excitation geometry and to the phase matching condition, and may depend on quite an extended region of the material away from the focal plane. Here we solve analytically the amplitude integral for second harmonic and third harmonic waves and study the generated harmonic intensities vs. focal-plane position within the material. We find that maximum intensity for positive wave-vector mismatch values, for both second harmonic and third harmonic waves, is achieved when the fundamental Gaussian is focused few Rayleigh lengths beyond the front surface. Harmonic-generation theory predicts strong intensity oscillations with thickness if the material is very thin. We reproduced these intensity oscillations in glass slabs pumped at 1550nm. From the oscillations of the 517nm third-harmonic waves with slab thickness we estimate the wave-vector mismatch in a Soda-lime glass as Δk(H)= -0.249μm(-1).