Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 142, Issue 9, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.4913686
Keywords
-
Funding
- Terman fellowship
- Alfred P. Sloan Research fellowship
- Hellman Faculty Scholar Fund fellowship
- Stanford University
- Stanford Center for Molecular Analysis and Design
- National Science Foundation Graduate Research Fellowship Program [DGE-114747]
Ask authors/readers for more resources
In this article, we show how Ehrenfest mean field theory can be made both a more accurate and efficient method to treat nonadiabatic quantum dynamics by combining it with the generalized quantum master equation framework. The resulting mean field generalized quantum master equation (MF-GQME) approach is a non-perturbative and non-Markovian theory to treat open quantum systems without any restrictions on the form of the Hamiltonian that it can be applied to. By studying relaxation dynamics in a wide range of dynamical regimes, typical of charge and energy transfer, we show that MF-GQME provides a much higher accuracy than a direct application of mean field theory. In addition, these increases in accuracy are accompanied by computational speed-ups of between one and two orders of magnitude that become larger as the system becomes more nonadiabatic. This combination of quantum-classical theory and master equation techniques thus makes it possible to obtain the accuracy of much more computationally expensive approaches at a cost lower than even mean field dynamics, providing the ability to treat the quantum dynamics of atomistic condensed phase systems for long times. (c) 2015 AIP Publishing LLC.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available