Bulletin of the Korean Chemical Society

Korean Chemical Society (대한화학회)
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Vibronically Induced Two-Photon Transitions in Benzene

  • Published : 1989.06.20
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Abstract

The strengths of two-photon transitions from the ground state to excited vibronic states in benzene are calculated by using the CNDO/2-U wave functions. The role of vibronic coupling in two-photon absorption process is discussed. The $A_{1{\bar{g}}}-A_{2g}^+$ two-photon transitions, which are forbidden by the identity-forbidden selection rule in single frequency two-photon absorption, are too weak to be experimentally observed even when two photons of different energies are used. It is because the transitions are forbidden also by the pseudo-parity selection rule which are applicable for alternant hydrocarbons such as benzene. It is also shown that the vibronic coupling is not very effective in altering the pseudo-parity property of the electronic state. The strength of the vibronically induced two-photon absorption is strongly affected by the presence of an electronic state from which two-photon absorption can borrow the intensity. It is pointed out that the pseudo-parity selection rule may be violated in such cases.

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