Modeling nonadiabatic dynamics with degenerate electronic states, intersystem crossing, and spin separation: A key goal for chemical physics
Modeling nonadiabatic dynamics with degenerate electronic states, intersystem crossing, and spin separation: A key goal for chemical physics
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DOI：
10.1063/5.0039371
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发表时间：
2021-03-21
影响因子：
4.4
通讯作者：
Subotnik, Joseph E.
中科院分区：
文献类型：
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作者：
Bian, Xuezhi;Wu, Yanze;Subotnik, Joseph E.
我们研究了在存在简并电子态的非绝热动力学中出现的许多悬而未决的问题，例如，对于单重态到三重态的系统间交叉，其中最小哈密顿量必须包含四个态（其中两个总是简并的）。在这种情况下，标准的曲面跳跃方法是不够的，因为该算法不包括Berry力。然而，我们假设这样的贝里力对于产生手性诱导自旋分离可能是至关重要的，这是一个新兴的研究领域。因此，这一观点强调了这样一个事实，即如果人们能够为简并态的情况产生一种鲁棒而精确的半经典方法，人们将在将化学物理学与自旋电子学融合的道路上迈出一大步。
We examine the many open questions that arise for nonadiabatic dynamics in the presence of degenerate electronic states, e.g., for singlet-to-triplet intersystem crossing where a minimal Hamiltonian must include four states (two of which are always degenerate). In such circumstances, the standard surface hopping approach is not sufficient as the algorithm does not include Berry force. Yet, we hypothesize that such a Berry force may be crucial as far as creating chiral induced spin separation, which is now a burgeoning field of study. Thus, this Perspective highlights the fact that if one can generate a robust and accurate semiclassical approach for the case of degenerate states, one will take a big step forward toward merging chemical physics with spintronics.