分子与金属表面相互作用的非绝热动力学：将运动分层方程和朗之万动力学方法扩展至位置依赖的金属-分子耦合
Nonadiabatic Dynamics of Molecules Interacting with Metal Surfaces: Extending the Hierarchical Equations of Motion and Langevin Dynamics Approach to Position-Dependent Metal-Molecule Couplings
AI总结：
本文将运动分层方程框架内的电子摩擦理论扩展至位置依赖的金属-分子耦合模型，为朗之万动力学引入了新的力贡献，适用于平衡与非平衡态及强相互作用分子模型。
摘要：
电子摩擦和朗之万动力学是一种流行的混合量子-经典方法，用于模拟分子与金属表面相互作用的非绝热动力学，因为它的计算效率比完全量子方法更高。然而，先前计算电子摩擦和其他力的方法仅限于非相互作用分子模型或位置无关的金属-分子耦合。在这项工作中，我们将运动分层方程形式体系内的电子摩擦理论扩展到具有位置依赖的金属-分子耦合的模型。我们表明，位置依赖的金属-分子耦合的加入为电子摩擦和其他力增加了新的贡献，这与许多物理过程高度相关。我们在朗之万方程中对电子力的表达式在平衡态和非平衡态下以及对于包含强相互作用的分子模型均有效。我们通过将其应用于不同的感兴趣模型来演示该方法。
英文摘要：
Electronic friction and Langevin dynamics is a popular mixed quantum-classical method for simulating the nonadiabatic dynamics of molecules interacting with metal surfaces, as it can be computationally more efficient than fully quantum approaches. Previous approaches to calculating the electronic friction and other forces, however, have been limited to either noninteracting molecular models or position-independent metal-molecule couplings. In this work, we extend the theory of electronic friction within the hierarchical equations of motion formalism to models with a position-dependent metal-molecule coupling. We show that the addition of a position-dependent metal-molecule coupling adds new contributions to the electronic friction and other forces, which are highly relevant for many physical processes. Our expressions for the electronic forces within the Langevin equation are valid both in and out of equilibrium and for molecular models containing strong interactions. We demonstrate the approach by applying it to different models of interest.
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