Convenient Expression of the Rate Constant for Nonadiabatic Transition


YOSHISHIGE OKUNO, SHINRO MASHIKO

National Institute of Information and Communications Technology, 588-2 Iwaoka Iwaoka-cho, Nishi-ku, Kobe 651-2401, Japan

Received 1 December 2003; accepted 21 July 2004
Published online 10 November 2004 in Wiley InterScience (www.interscience.wiley.com).
DOl 10.1002/qua.20351


ABSTRACT: We derived a convenient expression of the rate constant for nonadiabatic transitions, with the intention of making it possible and practical to calculate the rate constant. For this derivation, we first assume that the seam, at which the adiabatic potential energy surfaces of reactant and product electronic states exhibit an avoided crossing, corresponds to the dividing surface of the nonadiabatic transition. Second, we use the probability that a nonadiabatic transition occurs in the seam. Third, the partition function in the seam is described by the local profile of the adiabatic potential energy surfaces of both the reactant and product electronic states. The rate constant expression thus derived not only gives significant insight into understanding nonadiabatic transitions, but also makes it possible to obtain a rough estimate of the rate constant. ©2004 Wiley Periodicals,Inc.Int J Quantum Chem 102: 8-18, 2005

Key words: nonadiabatic transition; rate constant; transition state theory; excitation energy transfer; parphyrin wire