TITLE

Vibronic analysis of overlapping resonances and the third-harmonic-generation spectrum of β-carotene

AUTHOR(S)
Soos, Z. G.; Mukhopadhyay, D.
PUB. DATE
October 1994
SOURCE
Journal of Chemical Physics;10/1/1994, Vol. 101 Issue 7, p5515
SOURCE TYPE
Academic Journal
DOC. TYPE
Article
ABSTRACT
Vibronic contributions to third-harmonic-generation (THG) are obtained in the Condon approximation for displaced harmonic oscillators in the region of overlapping three- and two-photon resonances, where enhanced THG intensity and explicit dependence on the relative signs of the displacements are found. The THG intensity and phase of β-carotene are then modeled in terms of four electronic states, including overlapping 2 1Ag and 1 1Bu resonances whose displacements are taken from two-photon and linear spectra, respectively, and a high-energy Ag state based on a Pariser–Parr–Pople (PPP) sum rule for transition dipoles. Relations between THG and other spectra show the limitations of three-state models and provide useful constraints on the excited-state structure of related conjugated systems such as polyenes and β-carotene.
ACCESSION #
7648811

 

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