We report the results of pump–probe optical Kerr effect (OKE) experiments performed on neat solutions of carbon tetrachloride, nitrobenzene, methyl methacrylate monomer, binary solutions of the squaraine dye indole squarylium, and the phthalocyanine dye silicon phthalocyanine-monomethacrylate, respectively, in carbon tetrachloride, and solid solutions of indole squarylium and phthalocyanine-monomethacrylate in poly(methyl methacrylate). Dispersion measurements of the dye solutions were performed in the visible one-photon resonant region of the dyes defined by their linear-absorption spectra. The dyes’ third-order molecular susceptibility response in this spectral region is markedly different, with and Analysis of the dyes’ OKE response requires the inclusion of high-lying two-photon states and suggests that a purely electronic mechanism dominates their OKE response. The results are used to calculate the dyes’ off-resonant third-order molecular susceptibilities, which are well within the limits predicted by the Thomas–Reiche–Kuhn sum rule [M. G. Kuzyk, Opt. Lett. 25, 1183–1185 (2000)].
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