An elementary description of nonlinear optical properties of octupolar molecules: Four-state model for guanidinium-type molecules

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A theoretical description of the molecular polarizability (α) and first and second hyperpolarizabilities (β and γ) of a guanidinium-type octupolar molecule is presented. By using a valence bond and three charge-transfer states with nonzero transfer integrals, the electronic states are obtained as linear combinations of these basis states. It is found that a doubly degenerate excited state is only optically coupled to the ground state. Based on the analytic expressions for α, β, and γ obtained, it is shown that the resultant tensor elements of β satisfy the symmetry requirements of point group D3h. Unlike the linear push-pull polyenes, the magnitudes of α, β, and γ of the guanidinium-type octupolar molecules increase as the charge-transfer character of the electronic ground state increases. Also, their dependences on the distance (d) between the donor and acceptor are briefly discussed.

Original languageEnglish
Pages (from-to)7114-7120
Number of pages7
JournalJournal of Chemical Physics
Issue number17
Publication statusPublished - 1998 May 1


ASJC Scopus subject areas

  • Atomic and Molecular Physics, and Optics

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