Exciton Lifetime and Optical Line Width Profile via Exciton–Phonon Interactions: Theory and First-Principles Calculations for Monolayer MoS2

Chan, Yang-hao; Haber, Jonah B.; Naik, Mit H.; Neaton, Jeffrey B.; Qiu, Diana Y.; da Jornada, Felipe H.; Louie, Steven G.

doi:10.1021/acs.nanolett.3c00732

Title: Exciton Lifetime and Optical Line Width Profile via Exciton–Phonon Interactions: Theory and First-Principles Calculations for Monolayer MoS₂

Journal Article · Tue Apr 18 00:00:00 EDT 2023 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.3c00732· OSTI ID:1991077

^[1]; Haber, Jonah B. ^[2];

^[2]; Neaton, Jeffrey B. ^[2];

^[3];

^[4];

^[2]

National Center of Theoretical Physics, Taipei (Taiwan); Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Yale Univ., New Haven, CT (United States)
Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Exciton dynamics dictates 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. Here, 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 self-energy, which is critical for the description of dephasing mechanisms and yields exciton line widths in excellent agreement with experiment.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC02-76SF00515; AC02-05CH11231

OSTI ID:: 1991077

Journal Information:: Nano Letters, Vol. 23, Issue 9; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Exciton Lifetime and Optical Line Width Profile via Exciton–Phonon Interactions: Theory and First-Principles Calculations for Monolayer MoS2

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References (47)

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Title: Exciton Lifetime and Optical Line Width Profile via Exciton–Phonon Interactions: Theory and First-Principles Calculations for Monolayer MoS₂