RhoDyn: A ρ-TD-RASCI Framework to Study Ultrafast Electron Dynamics in Molecules.
RhoDyn: A ρ-TD-RASCI Framework to Study Ultrafast Electron Dynamics in Molecules.
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DOI：
10.1021/acs.jctc.1c01097
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发表时间：
2021-11
影响因子：
5.5
通讯作者：
V. Kochetov;S. I. Bokarev
中科院分区：
文献类型：
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作者：
V. Kochetov;S. I. Bokarev
本文介绍了程序模块 RhoDyn，作为 OpenMOLCAS 项目的一部分，旨在研究基于密度矩阵的时间相关受限活动空间配置交互框架 (ρ-TD-RASCI) 内的超快电子动力学。该形式允许处理自旋轨道耦合效应，以振动热浴的形式解释核振动，并且自然地包含（自动）电离效应。除了描述背后的理论和程序工作流程外，本文还包含其在钛配合物的线性 L2,3 吸收光谱、氢分子中的高次谐波产生、苯和碘乙炔中的超快电荷迁移以及铁配合物核心激发态中的自旋翻转动力学的模拟中的应用示例。
This article presents the program module RhoDyn as part of the OpenMOLCAS project intended to study ultrafast electron dynamics within the density-matrix-based time-dependent restricted active space configuration interaction framework (ρ-TD-RASCI). The formalism allows for the treatment of spin-orbit coupling effects, accounts for nuclear vibrations in the form of a vibrational heat bath, and naturally incorporates (auto)ionization effects. Apart from describing the theory behind and the program workflow, the paper also contains examples of its application to the simulations of the linear L2,3 absorption spectra of a titanium complex, high harmonic generation in the hydrogen molecule, ultrafast charge migration in benzene and iodoacetylene, and spin-flip dynamics in the core excited states of iron complexes.