Symmetry-breaking effects on photoinduced processes in solution

Anne B. Myers; Alan E. Johnson; Hirofumi Sato; Fumio Hirata

doi:10.1117/12.306109

24 April 1998 Symmetry-breaking effects on photoinduced processes in solution

Anne B. Myers, Alan E. Johnson, Hirofumi Sato, Fumio Hirata

Proceedings Volume 3273, Laser Techniques for Condensed-Phase and Biological Systems; (1998) https://doi.org/10.1117/12.306109
Event: Optoelectronics and High-Power Lasers and Applications, 1998, San Jose, CA, United States

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.

Citation Download Citation

Anne B. Myers, Alan E. Johnson, Hirofumi Sato, and Fumio Hirata "Symmetry-breaking effects on photoinduced processes in solution", Proc. SPIE 3273, Laser Techniques for Condensed-Phase and Biological Systems, (24 April 1998); https://doi.org/10.1117/12.306109

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