Dispersion of the nonlinear optical susceptibilities of organic liquids and solutions

Abstract

The dispersion of the third order optical nonlinear polarizabilities of benzene, chlorobenzene, and nitrobenzene is measured in the vicinity of Raman active vibrations. Observation of interference between resonant and nonresonant contributions determines the magnitude and phase of the electronic hyperpolarizability. Shifts in the frequency and linewidth of the interference minima occur when additional components such as CCl₄, CS₂, or 2,5‐diphenyloxazole are added to the solution. Analysis of the resulting line shape yields the hyperpolarizability of the solute species.