Quantum-classical Liouville dynamics of nonadiabatic proton transfer.
Quantum-classical Liouville dynamics of nonadiabatic proton transfer.
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非绝热质子转移的量子经典刘维尔动力学。
DOI：
10.1063/1.1940051
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发表时间：
2005
期刊：
影响因子：
--
通讯作者：
R. Kapral
中科院分区：
文献类型：
--
作者：
G. Hanna;R. Kapral
用混合量子-经典Liouville动力学方法研究了极性溶剂中线性氢键复合物的质子转移反应。在这个系统中，质子被量子力学地处理，其余的自由度被经典地处理。采用绝热和非绝热分子动力学研究了反应的速率和机理。我们使用的非绝热动力学算法，它允许系统的发展上单绝热表面和相干耦合对绝热表面。无功通量相关函数表达式被用来计算速率系数和相干耦合表面上的动态的作用阐明。
A proton transfer reaction in a linear hydrogen-bonded complex dissolved in a polar solvent is studied using mixed quantum-classical Liouville dynamics. In this system, the proton is treated quantum mechanically and the remainder of the degrees of freedom is treated classically. The rates and mechanisms of the reaction are investigated using both adiabatic and nonadiabatic molecular dynamics. We use a nonadiabatic dynamics algorithm which allows the system to evolve on single adiabatic surfaces and on coherently coupled pairs of adiabatic surfaces. Reactive-flux correlation function expressions are used to compute the rate coefficients and the role of the dynamics on the coherently coupled surfaces is elucidated.