Quantum Kramers turnover: a phase space function approach

Details Quantum Kramers turnover: a phase space function approach Quantum Kramers turnover: a phase space function approach

2004-11-11

arxiv.org/abs/cond-mat/0411294v1

Physics

Condensed Matter

Soft Condensed Matter

22 pages and 5 figures

Scientific paper

The problem of Kramers' turnover is a central issue of dynamical theory of reaction rate. Since its classical solution in the Markovian limit in mid-eighties by Melnikov and Meshkov, the problem has been addressed by a number of groups in the last decade both in classical non-Markovian and quantum mechanical context. Based on a coherent state representation of noise operators and a positive definite Wigner canonical thermal distribution function we have recently developed a c-number quantum Langevin equation [Barik \textit{et al}, J. Chem. Phys. {\bf 119}, 680 (2003); Banerjee \textit{et al}, Phys. Rev. E {\bf 65}, 021109 (2002)]. We implement this scheme within Pollak's well known normal mode description to calculate the quantum transmission coefficient over an arbitrary range of friction, noise correlation and temperature. The theory generalizes the quantum correction to Grote-Hynes factor in the rate expression down to vacuum limit which reduces to well known high temperature quantum correction, \textit{i.e.}, the Wolynes term for quantum transmission and reflection for the barrier in the appropriate limit and also considers the quantum corrections due to nonlinearity of the system potential order by order which contributes to energy loss and dispersion due to coupling between unstable and stable normal modes near the barrier top and is valid for both above and below the activated tunneling regime. Our results have been compared with those obtained earlier for a model potential and found to be good agreement.

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