Exciton lifetime and optical linewidth profile via exciton-phonon interactions: Theory and first-principles calculations for monolayer MoS${}_2$

Abstract

Exciton dynamics dictate the evolution of photoexcited carriers in photovoltaic and optoelectronic devices. However, interpreting their experimental signatures is a challenging theoretical problem due to the presence of both electron-phonon and many-electron interactions. We develop and apply here a first-principles approach to exciton dynamics resulting from exciton-phonon coupling in monolayer MoS2 and reveal the highly selective nature of exciton-phonon coupling due to the internal spin structure of excitons, which leads to a surprisingly long lifetime of the lowest energy bright A exciton. Moreover, we show that optical absorption processes rigorously require a second-order perturbation theory approach, with photon and phonon treated on an equal footing, as proposed by Toyozawa and Hopfield. Such a treatment, thus far neglected in first-principles studies, gives rise to off-diagonal exciton-phonon coupling matrix elements, which are critical for the description of dephasing mechanisms, and yields exciton linewidths in excellent agreement with experiment.

arXiv comment11 pages, 4 figures

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• Mixed quantum-classical modeling of exciton-phonon scattering in solids: Application to optical linewidths of monolayer MoS2
• Origin of interlayer exciton-phonon coupling in 2D heterostructures
• Wannier-Function-Based Approach to Coupled Exciton-Phonon-Photon Dynamics in Two-Dimensional Semiconductors
• Designable exciton mixing through layer alignment in WS${}_2$-graphene heterostructures
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• Symmetries in zero and finite center-of-mass momenta excitons