Abstract

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 ${\gamma }_{\mathit{xxxx}}(-{\omega }_2;{\omega }_1,-{\omega }_1, {\omega }_2)$ in this spectral region is markedly different, with ${\mathfrak{R}}_{\{\gamma \mathrm{ISQ}\}}>0$ and ${\mathfrak{R}}_{\{\gamma \mathrm{SiPc}\}}<0.$ 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)].

© 2001 Optical Society of America

Measuring the electronic third-order susceptibility of the silicon phthalocyanine-monomethacrylate molecule with quadratic electroabsorption spectroscopy

Robert J. Kruhlak and Mark G. Kuzyk
J. Opt. Soc. Am. B 22(3) 643-654 (2005)

Mechanisms of the nonlinear optical properties of squaraine dyes in poly(methyl methacrylate) polymer

K. S. Mathis, M. G. Kuzyk, C. W. Dirk, A. Tan, S. Martinez, and G. Gampos
J. Opt. Soc. Am. B 15(2) 871-883 (1998)

Rapid-scan pump–probe spectroscopy with high time and wave-number resolution: optical-Kerr-effect measurements of neat liquids

M. J. Feldstein, P. Vöhringer, and N. F. Scherer
J. Opt. Soc. Am. B 12(8) 1500-1510 (1995)

Frequency dependence of the optical Kerr effect and third-order electronic nonlinear-optical processes of organic liquids

M. G. Kuzyk, R. A. Norwood, J. W. Wu, and A. F. Garito
J. Opt. Soc. Am. B 6(2) 154-164 (1989)

Heavy-atom effect on second hyperpolarizabilities of thiophene homologues investigated by a femtosecond optical-Kerr-effect experiment and ab initio molecular orbital calculation

Kenji Kamada, Minoru Ueda, Toru Sakaguchi, Koji Ohta, and Toshio Fukumi
J. Opt. Soc. Am. B 15(2) 838-845 (1998)