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Influence of Solvation Environment on Excited State Avoided Crossings and Photodissociation Dynamics
Journal article   Peer reviewed

Influence of Solvation Environment on Excited State Avoided Crossings and Photodissociation Dynamics

N Yu, C. J Margulis and D. F Coker
The journal of physical chemistry. B, Vol.105(28), pp.6728-6737
07/19/2001
DOI: 10.1021/jp0108925

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Abstract

Photodissociation dynamics of I2 in rare gas liquids and solid matrixes have been the focus of much experimental and theoretical research. Experimental studies of both A and B state photoexcitation leading to dissociation have been thoroughly investigated by Apkarian and Schwentner, showing very dissimilar behavior between solid and liquid phases. B state excitation of I2 in liquid rare gases results in fast dissociation in a few hundred femtoseconds, while the B state lifetime in the solid is measured to be on the order of a few picoseconds. The current paper addresses various important issues related to the implementation of the nonadiabatic dynamics methods in the situation where quasi-nonavoided crossings take place and play a crucial role in determining the dynamics. Reliable treatment of quasi-nonavoided crossings in nonadiabatic MD calculations enables the accurate computation of pump−probe signals that reproduce experimental results. Analysis of trajectory data provides a detailed understanding of the interactions between local solvation environment symmetries and electronic coupling symmetries that are fundamentally important in governing nonadiabatic relaxation in condensed phases. The paper also explores the fundamental issue of the existence of approximate “selection rules” for nonadiabatic electronic relaxation arising from symmetries of electronic state coupling and the local symmetries present in ordered or even disordered condensed phase environments.

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