Contribution of two-photon states to the third-order optical nonlinearity in squaraine compounds

James H. Andrews; Kenneth D. Singer; Carl W. Dirk; Diana L. Hull; Kathy C. Chuang

doi:10.1117/12.328177

16 October 1998 Contribution of two-photon states to the third-order optical nonlinearity in squaraine compounds

James H. Andrews, Kenneth D. Singer, Carl W. Dirk, Diana L. Hull, Kathy C. Chuang

Proceedings Volume 3473, Third-Order Nonlinear Optical Materials; (1998) https://doi.org/10.1117/12.328177
Event: SPIE's International Symposium on Optical Science, Engineering, and Instrumentation, 1998, San Diego, CA, United States

Abstract

We investigate the contribution of two-photon states to the third-order optical nonlinearity in four squaraine compounds. Our experimental results using third-harmonic spectral dispersion are compared to experimental results obtained by other researchers using quadratic electro-optic spectral dispersion and femtosecond excited state absorption measurements. Different relative contributions from high lying two-photon states are seen using different experimental techniques. We also relate these results to finite-field and sum-over states quantum chemical methods which indicate that there are multiple high-lying states that contribute to the third-order nonlinearity. For one of these dyes, we find that contributions from a mixture of isomers needs to be considered. For this latter dye, we compare our calculated transition moments and third harmonic dispersion curve using quantum mechanical methods with our results from third harmonic spectral dispersion and find substantial agreement between the experimental and theoretical results.

Citation Download Citation

James H. Andrews, Kenneth D. Singer, Carl W. Dirk, Diana L. Hull, and Kathy C. Chuang "Contribution of two-photon states to the third-order optical nonlinearity in squaraine compounds", Proc. SPIE 3473, Third-Order Nonlinear Optical Materials, (16 October 1998); https://doi.org/10.1117/12.328177

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