表面跳跃
含时密度泛函理论
密度泛函理论
振动耦合
分子动力学
非绝热的
化学
弹道
光异构化
统计物理学
电子结构
分子物理学
计算化学
物理
量子力学
拓扑(电路)
分子
绝热过程
异构化
数学
组合数学
生物化学
催化作用
作者
Noriyuki Minezawa,Takahito Nakajima
摘要
This paper presents the nonadiabatic molecular dynamics simulation combined with the spin-flip time-dependent density functional theory (SF-TDDFT). In contrast to the conventional single-reference electronic structure methods, which have difficulty in describing the S0/S1 conical intersections, the SF-TDDFT can yield the correct topology of crossing points. Thus, one expects that the method can take naturally into account the S1 → S0 nonadiabatic transitions. We adopt Tully’s fewest switch surface hopping algorithm by introducing the analytic SF-TDDFT nonadiabatic coupling vector. We apply the proposed method to the photoisomerization reactions of E-azomethane, methanimine, and ethene molecules and reproduce the results of previous studies based on the multireference methods. The proposed approach overcomes the ad hoc treatment of S1 → S0 transition at the single-reference calculation level and affords both the dynamics on the S1 state and the recovery of the S0 state with modest computational costs.
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