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The structures of a series of donor acceptor thienylmethylene anilines (9, 10), benzylidene aminothiophenes (11, 12), and extended structures containing the azobenzene chromophore (16, 17) have been calculated and their hyperpolarizabilities have been assessed using a sum-over-states approach. The results show that low lying excited states involving the thiophene ring exert a pronounced effect on...