标题： 快速处理多站点电荷转移过程的方法 I：约束态平均 CASSCF(1,M) 和 CASSCF(2M-1,M) 模拟 显示英文标题

标题： Fast Methods For Multisite Charge Transfer Processes I: Constrained, State Averaged CASSCF(1,M) and CASSCF(2M-1,M) Simulations

摘要： 我们设计了一种动态加权状态平均约束CASSCF方法，以处理\ul{e}电子或\ul{h}空穴在$n$分子碎片之间的移动（其中$n$可以大于2）。 在所谓的eDSCn/hDSCn方法中，我们考虑彼此为单激发的构型，并应用一组广义约束，以定制该方法用于研究电荷转移问题。 受约束的优化问题通过DIIS-SQP算法高效求解，从而保持计算效率。 我们对该方法进行了有限Su-Schrieffer-Heeger（SSH）链进行演示，成功再现了二面耦合随距离的预期指数衰减。 当与梯度结合时，当前扩展立即实现了复杂多态电荷转移过程的有效非绝热动力学模拟。 显示英文摘要

摘要： We design a dynamically-weighted state-averaged constrained CASSCF to treat \ul{e}lectrons or \ul{h}oles moving between $n$ molecular fragments (where $n$ can be larger than 2). Within such a so-called eDSCn/hDSCn approach, we consider configurations that are mutually single excitations of each other, and we apply a generalized set of constraints to tailor the method for studying charge transfer problems. The constrained optimization problem is efficiently solved using a DIIS-SQP algorithm, thus maintaining computational efficiency. We demonstrate the method for a finite Su-Schrieffer-Heeger (SSH) chain, successfully reproducing the expected exponential decay of diabatic couplings with distance. When combined with a gradient, the current extension immediately enables efficient nonadiabatic dynamics simulations of complex multi-state charge transfer processes.