AI 中文总结
本文提出开放非平衡分子系统的混合量子-经典表述，基于PP-NEGF方法推导密度矩阵运动方程，并指出FSSH近似在绝热面接近时不成立。
AI 中文摘要
我们考虑开放非平衡分子系统的混合量子-经典表述。我们采用赝粒子非平衡格林函数（PP-NEGF）方法作为完全量子描述，并作为引入开放系统经典核动力学的起点。我们利用这一表述推导出描述量子-经典演化的密度矩阵运动方程。我们将我们的结果与先前的表述进行比较，并强调与分子系统的非平衡和开放特性相关的重要差异。我们还分析了将完全量子-经典动力学简化到最少切换面跳跃（FSSH）方法所需的近似，并表明当绝热面彼此接近时这些近似是不合理的。
英文摘要
We consider a mixed quantum-classical formulation for open nonequilibrium molecular systems. We employ the pseudoparticle nonequilibrium Green's function (PP-NEGF) method as a fully quantum description and a starting point for introducing classical nuclear dynamics for an open system. We use this formulation to derive a density-matrix equation of motion describing the quantum-classical evolution. We compare our results with previous formulations and highlight important differences related to the nonequilibrium and open character of the molecular system. We also analyze the approximations needed to reduce full quantum-classical dynamics to the fewest-switches surface hopping (FSSH) method and show that these approximations are unreasonable when adiabatic surfaces come close to each other.
Comments11 pages
