Abstract

A wide range of third-order nonlinear optical processes are mediated by the molecular second hyperpoiarizability(γ −ω_σ;ω₁,ω₂,ω₃). The relations between these nonlinear processes are complicated because γ is a function of three frequency arguments and the electronic and vibrational¹ contributions to γ quite different frequency dependences. However, by considering the electronic and vibrational contributions to γ separately, the complete frequency dependence of γ becomes simpler to understand.

© 1987 Optical Society of America