Mechanisms for enhancement of two-photon absorption in donor–acceptor conjugated chromophores

Abstract Two-photon absorption (TPA) is a nonlinear optical process that is gaining increasing attention since it can be exploited in a number of optical applications. Here, on the basis of correlated quantum-chemical calculations, we investigate the structure–TPA property relationships for donor–acceptor π-conjugated compounds. These relationships provide strategies to design dyes with large TPA cross-sections for fundamental photon wavelengths in the desired 0.6–1.0 μm range of wavelengths.

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