期刊
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
卷 -, 期 -, 页码 -出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jctc.3c00276
关键词
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We have developed a rare-event sampling scheme to quantify the rate of thermally activated nonadiabatic transitions in the condensed phase. Through surface hopping scheme, our simulations provide insight into the participation ratio of a solvent and the effect of ion separation distance on electron transfer.
We implement a rare-event sampling scheme for quantifying the rate of thermally activated nonadiabatic transitions in the condensed phase. Our Quantum mechanics/molecular mechanics (QM/MM) methodology uses the recently developed Interface for NonAdiabatic QM/MM in Solvent (INAQS) package to interface an elementary electronic structure package and a popular open-source molecular dynamics software (GROMACS) to simulate an electron transfer event between two stationary ions in a solution of acetonitrile solvent molecules. Nonadiabatic effects are implemented through a surface hopping scheme, and our simulations allow further quantitative insight into the participation ratio of a solvent and the effect of ion separation distance as far as facilitating electron transfer. We also demonstrate that the standard gas-phase approaches for treating frustrated hops and velocity reversal must be refined when working in the condensed phase with many degrees of freedom. The code and methodology developed here can be easily expanded upon and modified to incorporate other systems and should provide a great deal of new insight into a wide variety of condensed phase nonadiabatic phenomena.
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