Bian Xuezhi, Wu Yanze, Teh Hung-Hsuan, Zhou Zeyu, Chen Hsing-Ta, Subotnik Joseph E
Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, USA.
J Chem Phys. 2021 Mar 21;154(11):110901. doi: 10.1063/5.0039371.
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.
我们研究了在简并电子态存在的情况下非绝热动力学中出现的诸多开放性问题，例如对于单重态到三重态的系间窜越，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，标准的表面跳跃方法并不充分，因为该算法不包括贝里力。然而，我们推测，就产生手性诱导自旋分离而言，这样的贝里力可能至关重要，而手性诱导自旋分离如今是一个新兴的研究领域。因此，这篇综述强调了这样一个事实，即如果能够为简并态的情况生成一种稳健且准确的半经典方法，那么在将化学物理与自旋电子学融合方面将向前迈出一大步。
