Frequency-agile hyper-Rayleigh scattering studies of electro-optic chromophores

Kimberly A. Firestone; David B. Lao; Daniel M. Casmier; Olivier Clot; Larry Raymond Dalton; Philip J. Reid

doi:10.1117/12.617624

18 August 2005 Frequency-agile hyper-Rayleigh scattering studies of electro-optic chromophores

Kimberly A. Firestone, David B. Lao, Daniel M. Casmier, Olivier Clot, Larry Raymond Dalton, Philip J. Reid

Proceedings Volume 5935, Linear and Nonlinear Optics of Organic Materials V; 59350P (2005) https://doi.org/10.1117/12.617624
Event: Optics and Photonics 2005, 2005, San Diego, California, United States

Abstract

Hyper-Rayleigh scattering (HRS) is used to measure the first-hyperpolarizability (β) of electro-optic (EO) chromophores. One of the inherent concerns in any HRS measurement is the extent to which resonant enhancement contributes to the observed intensity thereby leading to inaccuracies when evaluating chromophore potential for application in electro-optical devices. One way to address this concern is to employ increasingly longer excitation wavelengths far from resonance. However, in charge-transfer-based non-linear optical chromophores, enhanced β generally correlates with a red-shift of the charge transfer absorption band so that even at the longest excitation wavelengths generally employed in HRS studies, resonant enhancement remains an issue. We have adopted an alternative approach in which the wavelength dispersion of the HRS intensity is determined by performing measurements at a variety of excitation wavelengths. This approach allows one to ascertain the role of resonance enhancement thereby allowing for more accurate correlation of improved β with molecular architecture. We report the results of our HRS studies for nine chromophores employing excitation wavelengths ranging from 780 to 1907 nm. Our HRS results demonstrate good agreement with the predictions of density functional theory. This synthesis of experimental and theoretical techniques has resulted in more effective designs for the next generations of electro-optical chromophores.

Citation Download Citation

Kimberly A. Firestone, David B. Lao, Daniel M. Casmier, Olivier Clot, Larry Raymond Dalton, and Philip J. Reid "Frequency-agile hyper-Rayleigh scattering studies of electro-optic chromophores", Proc. SPIE 5935, Linear and Nonlinear Optics of Organic Materials V, 59350P (18 August 2005); https://doi.org/10.1117/12.617624

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