Iterative linearized approach to nonadiabatic dynamics.
This paper presents a new approach to propagating the density matrix based on a time stepping procedure arising from a Trotter factorization and combining the forward and backward incremental propagators. The sums over intermediate states of the discrete quantum subsystem are implemented by a Monte Carlo surface hopping-like procedure, while the integrals over the continuous variables are performed using a linearization in the difference between the forward and backward paths of these variables leading to classical-like equations of motion with forces determined by the quantum subsystem states. The approach is tested on several models and numerical convergence is explored.
Dunkel
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Department of Physics, Harvard University, 17 Oxford Street, Cambridge, Massachusetts 02138, USA.
Bonella
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Coker
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