Abstract
The theory of two-photon absorption has been implemented within the CNDO/S-CI formalism to calculate two-photon absorptivity of doublet states. The method was utilized to investigate the origins of below threshold optical absorption in ion cyclotron resonance photodissociation spectra of benzene, t-butylbenzene, styrene, and 1-methylnaphthalene. The computations suggest that these below threshold processes may be due to simultaneous two-photon absorption rather than sequential absorption as postulated by Freiser and Beauchamp. Some photodissociation pathways are found to be both mono- and biphotonic in nature. Some wavelength dependent processes found in t-butylbenzene may well be biphotonic and could be competitive with monophotonic absorption below 3.08 eV.
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