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Proceedings Paper

Symmetry-breaking effects on photoinduced processes in solution
Author(s): Anne B. Myers; Alan E. Johnson; Hirofumi Sato; Fumio Hirata
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Paper Abstract

Raman and resonance Raman spectroscopies are employed to explore the degree of solvent-induced symmetry breaking int he ground and excited electronic states of the nominally symmetric linear molecules CS2 and I3-. A signature of broken symmetry is intensity in the antisymmetric stretching fundamental. CS2 breaks symmetry only slightly in all solvents examined, and the effects on the nuclear dynamics of the S3 excited state appear to be minimal. In I3-, asymmetry is pronounced in alcoholic solvents but undetectable in acetonitrile. MCSCF/RISM calculations support the experimental result and indicate that solvent stabilization of separated charges renders a wide range of asymmetric ground-state structures energetically accessible. Recent femtosecond time-domain studies of the photodissociated process indicate a significant influence of asymmetry of the reactant on the dynamics of product formation.

Paper Details

Date Published: 24 April 1998
PDF: 8 pages
Proc. SPIE 3273, Laser Techniques for Condensed-Phase and Biological Systems, (24 April 1998); doi: 10.1117/12.306109
Show Author Affiliations
Anne B. Myers, Univ. of Rochester (United States)
Alan E. Johnson, Univ. of Rochester (United States)
Hirofumi Sato, Institute for Molecular Science (Japan)
Fumio Hirata, Institute for Molecular Science (Japan)

Published in SPIE Proceedings Vol. 3273:
Laser Techniques for Condensed-Phase and Biological Systems
Norbert F. Scherer; Janice M. Hicks, Editor(s)

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