Abstract

The second hyperpolarizabilities of three heterocyclic molecules of C4H4X, where X=O (furan), S (thiophene), or Se (selenophene), were investigated by an optical-heterodyne-detected optical-Kerr-effect experiment and an ab initio Hartree–Fock molecular orbital calculation with largely augmented basis sets. From the observed third-order responses the electronic hyperpolarizabilities were determined after the nuclear nonlinear optical responses were removed by Fourier-transform analysis. Results of both experiment and calculation exhibited 2 times enhancement when the heteroatom of O was replaced by Se. The origin of the enhancement and the contribution of the heteroatom to the hyperpolarizability are discussed. Also, a direct comparison of the experimental values with calculated ones is made.

© 1998 Optical Society of America

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