论文标题
用电子退化对自旋依赖性的非绝热动力学进行建模：一种相位空间跳跃方法
Modeling Spin-Dependent Nonadiabatic Dynamics with Electronic Degeneracy: A Phase-Space Surface-Hopping Method
论文作者
论文摘要
核浆果曲率效应从电子自旋退化和canlead到非平凡的自旋依赖性（非绝热）核动力学出现。但是，在当前所有混合量子古典方法（例如最少的开关表面跳跃）中，完全忽略了这种效果。在这项工作中，我们提出了一种相位空间的表面跳跃（PSSH）方法，以模拟单线 - 三个跨系统交叉动力学。我们表明，使用简单的伪脱糖ANSATZ，PSSH算法可以捕获相关的浆果曲率效应，并使预测与精确的量子动力学一致，用于简单的Singlet-Triplet模型Hamiltonian。因此，这种方法代表了与与系统交叉和旋转晶格弛豫动力学相关的光化学和旋转过程的重要步骤。
Nuclear Berry curvature effects emerge from electronic spin degeneracy and canlead to non-trivial spin-dependent (nonadiabatic) nuclear dynamics. However, such effects are completely neglected in all current mixed quantum-classical methods such as fewest switches surface-hopping. In this work, we present a phase-space surface-hopping (PSSH) approach to simulate singlet-triplet intersystem crossing dynamics. We show that with a simple pseudo-diabatic ansatz, a PSSH algorithm can capture the relevant Berry curvature effects and make predictions in agreement with exact quantum dynamics for a simple singlet-triplet model Hamiltonian. Thus, this approach represents an important step towards simulating photochemical and spin processes concomitantly, as relevant to intersystem crossing and spin-lattice relaxation dynamics.
