Resonant and static cubic hyperpolarizabilities of push-pull dipolar and quadrupolar chromophores: toward enhanced two-photon absorption

Marguerite Barzoukas; Mireille H. Blanchard-Desce

doi:10.1117/12.449818

7 December 2001 Resonant and static cubic hyperpolarizabilities of push-pull dipolar and quadrupolar chromophores: toward enhanced two-photon absorption

Marguerite Barzoukas, Mireille H. Blanchard-Desce

Author Affiliations +

Proceedings Volume 4461, Linear and Nonlinear Optics of Organic Materials; (2001) https://doi.org/10.1117/12.449818
Event: International Symposium on Optical Science and Technology, 2001, San Diego, CA, United States

Abstract

Recent reports of push-pull dipolar and quadrupolar chromophores with enhanced two-photon absorption have generated considerable interest in these two molecular systems. Two photon absorption is related to the imaginary part of the two-photon resonant cubic hyperpolarizability Im[(gamma) ((omega) )]. In this work, we have described both push-pull dipolar and quadrupolar chromophores using multi valence-bond states models based on measurable parameters of the valence-bond forms. We have derived analytical expressions of their non-resonant static cubic hyperpolarizability (gamma) (0) and of Im[(gamma) ((omega) )]. Comparison between the transparency / Im[(gamma) ((omega) )] trade-off and Im[(gamma) ((omega) )] / (gamma) (0) correlation helps understand the advantages and drawbacks of each of these two push-pull systems. Furthermore by understanding how the valence-bond parameters are related to the molecular structure and its environment, it is possible to predict how Im[(gamma) ((omega) )] will be affected by changing either the conjugation size, the donor-acceptor pair or the solvent polarity for both of these push-pull systems. The results of this study suggest common guidelines for the molecular engineering of both the push-pull dipolar and quadrupolar chromophores.

Citation Download Citation

Marguerite Barzoukas and Mireille H. Blanchard-Desce "Resonant and static cubic hyperpolarizabilities of push-pull dipolar and quadrupolar chromophores: toward enhanced two-photon absorption", Proc. SPIE 4461, Linear and Nonlinear Optics of Organic Materials, (7 December 2001); https://doi.org/10.1117/12.449818

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