A broadened classical master equation approach for nonadiabatic dynamics at metal surfaces: Beyond the weak molecule-metal coupling limit
A broadened classical master equation approach for nonadiabatic dynamics at metal surfaces: Beyond the weak molecule-metal coupling limit
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DOI：
10.1063/1.4939734
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发表时间：
2016-01-14
影响因子：
4.4
通讯作者：
Subotnik, Joseph E.
中科院分区：
文献类型：
--
作者：
Dou, Wenjie;Subotnik, Joseph E.
提出了一个扩展的经典主方程（BCME），用于模拟金属表面附近分子在宽参数范围内的非绝热动力学行为。与仅在弱分子-金属耦合下有效的标准经典主方程相比，该BCME对弱分子-金属耦合和强分子-金属耦合都有效。(The BCME可以映射到正确捕获能级展宽的福克-普朗克方程。最后，我们的BCME可以用一个简单的表面跳跃算法来解决，平衡和动态可观测量的数值测试看起来非常有前途。(C)2016 AIP Publishing LLC.
A broadened classical master equation (BCME) is proposed for modeling nonadiabatic dynamics for molecules near metal surfaces over a wide range of parameter values and with arbitrary initial conditions. Compared with a standard classical master equation-which is valid in the limit of weak molecule-metal couplings-this BCME should be valid for both weak and strong molecule-metal couplings. (The BCME can be mapped to a Fokker-Planck equation that captures level broadening correctly.) Finally, our BCME can be solved with a simple surface hopping algorithm; numerical tests of equilibrium and dynamical observables look very promising. (C) 2016 AIP Publishing LLC.