Abstract

The importance of electron correlation effects on the nonresonant third-order nonlinear optical susceptibility γ_ijkl(−ω_4;ω₂ω₃) of conjugated organic molecules was discovered earlier theoretical .studies based on many-electron configuration interaction theory.¹ Experimental measurements of γ_ijkl(−ω_4;ω₁,ω₂,ω₃), however, have been made at only a few isolated wavelengths. Quantitative comparison between experimental and theoretical values for the dispersion of γ_ijkl(−ω_4;ω₁,ω₂,ω₃) can rigorously test the accuracy of many-electron, multiple-excited configuration interaction calculations.

© 1993 Optical Society of America