2025/05/11 by Alex Krotz, Krotz, Alex, Roel Tempelaar +1 · 1 citation
Materials Science · Physics and Astronomy · #2D Materials and Applications #Chemical Physics (physics.chem-ph) #Chemical and Physical Properties of Materials #FOS: Physical sciences #Materials Science (cond-mat.mtrl-sci) #Mesoscale and Nanoscale Physics (cond-mat.mes-hall) #Quantum Physics (quant-ph) #Spectroscopy and Quantum Chemical Studies
paper · pdf · doi:10.48550/arxiv.2505.06953
openalex publication_date 2025/05/11 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
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 MoS2. 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.