标题： 表面跳跃模拟显示，激子-声子共振驱动谷极化消失 显示英文标题

标题： Surface hopping simulations show valley depolarization driven by exciton-phonon resonance

摘要： 激子跃迁与核坐标之间的共振已被证明能够驱动分子系统中各种激发态动力学现象。 在这里，我们报告了混合量子-经典模拟，显示类似的共振主要导致单层MoS$_2$中的谷极化退相。 所采用的模拟框架结合了倒易空间表面跳跃与准粒子能带结构、电子-空穴相互作用和载流子-声子相互作用的微观模型，并通过第一性原理计算进行参数化。 这使得能够进行低成本的激发态动力学模拟，这些模拟在载流子-声子相互作用方面是微观的、非马尔可夫的和非微扰的。 该框架还保留了瞬时声子占据情况的显式信息，通过此我们展示了主要光学声子分支与最低激子带之间的共振通过激活Maialle-Silva-Sham机制来主要驱动谷极化退相。 所得的谷极化时间与不同温度下的实验测量结果一致。 显示英文摘要

摘要： Resonances between excitonic transitions and nuclear coordinates have been shown to drive a variety of excited-state dynamical phenomena in molecular systems. Here, we report mixed quantum--classical simulations showing similar resonances to primarily contribute to valley depolarization in monolayer MoS$_2$. The applied simulation framework combines reciprocal-space surface hopping with microscopic models of the quasiparticle band structure, electron--hole interactions, and carrier--phonon interactions, parametrized against ab initio calculations. This enables low-cost excited-state dynamics simulations that are microscopic, non-Markovian, and non-perturbative in the carrier--phonon interaction. The framework furthermore retains explicit information on transient phonon occupancies, through which we show a resonance between the dominant optical phonon branch and the lowest exciton band to largely drive valley depolarization, by activating a Maialle--Silva--Sham mechanism. Resulting valley polarization times are consistent with experimental measurements across temperatures.