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Theoretical investigation of two-photon absorption and third-harmonic generation in a long thiophene oligomer: α-heptathiophene

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Abstract

Taking into account the full chemical and molecular structure, we calculate the two-photon absorption spectrum (TPA) and the frequency-dependent third-harmonic generation (THG) of a long thiophene oligomer method based (T7, the α-heptathiophene) by means of a multireference-determinant–configuration-interaction on the intermediate-neglect-of-differential-overlap Hamiltonian. The TPA spectrum is dominated by a very intense peak associated with an mA excited state (m = 6). Three excited states (1B, mA, and mA) contribute primarily to the static third-order nonlinear optical response; however, a more complex model including both the 2A state and higher-lying B states is needed for description of all the features observed in the frequency-dependent THG spectrum. Extrapolation of the results from the oligomer to the polymer is a nontrivial task because of the presence of double resonances that are characteristic of finite chains.

© 1994 Optical Society of America

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