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

• URL: http://arxiv.org/abs/2505.06953v2
• Date: Wed, 16 Jul 2025 23:49:00 GMT
• Title: Surface hopping simulations show valley depolarization driven by exciton-phonon resonance
• Authors: Alex Krotz, Roel Tempelaar,
• Abstract summary: We show that resonances between excitonic transitions and nuclear coordinates contribute to valley depolarization in monolayer MoS$$.<n>Results are consistent with experimental measurements across temperatures.
• Score: 0.0
• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: 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.

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