Abstract
To provide an insight into the third-order nonlinear optical (NLO) behaviour of a series of tetrathiafulvalene (TTF)-based molecules, the third-order NLO properties and two-photon absorption characterizations have been theoretically investigated by means of the time-dependent Hartree–Fock method. According to ab-initio calculation results, the examined molecules exhibit second hyperpolarizabilities \((\gamma )\) with non-zero values, implying microscopic third-order optical nonlinearity. Our computed results are also in good agreement with the previous experimental observations on the title compounds.
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