Real-time GW -BSE investigations on spin-valley exciton dynamics in monolayer transition metal dichalcogenide

Jiang, Xiang; Zheng, Qijing; Lan, Zhenggang; Saidi, Wissam A.; Ren, Xinguo; Zhao, Jin

doi:10.1126/sciadv.abf3759

Title: Real-time GW -BSE investigations on spin-valley exciton dynamics in monolayer transition metal dichalcogenide

Journal Article · Fri Mar 05 00:00:00 EST 2021 · Science Advances

DOI:https://doi.org/10.1126/sciadv.abf3759· OSTI ID:1816450

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Univ. of Science and Technology of China, Hefei (China). Dept. of Physics. CAS Key Lab. of Strongly-Coupled Quantum Matter Physics. ICQD/Hefei National Lab. for Physical Sciences at Microscale
South China Normal Univ., Guangzhou (China). MOE Key Lab. of Theoretical Chemistry of Environment. Guangdong Provincial Key Lab. of Chemical Pollution and Environmental Safety. SCNU Environmental Research Inst.; South China Normal Univ., Guangzhou (China). School of Environment
Univ. of Pittsburgh, PA (United States). Dept. of Mechanical Engineering and Materials Science
Chinese Academy of Sciences, Beijing (China). Inst. of Physics
Univ. of Science and Technology of China, Hefei (China). Dept. of Physics. CAS Key Lab. of Strongly-Coupled Quantum Matter Physics. ICQD/Hefei National Lab. for Physical Sciences at Microscale; Univ. of Pittsburgh, PA (United States). Dept. of Physics and Astronomy; Univ. of Science and Technology of China, Hefei (China). Synergetic Innovation Center of Quantum Information and Quantum Physics

We develop an ab initio nonadiabatic molecular dynamics (NAMD) method based on GW plus real-time Bethe-Salpeter equation (GW + rtBSE-NAMD) for the spin-resolved exciton dynamics. From investigations on MoS₂, we provide a comprehensive picture of spin-valley exciton dynamics where the electron-phonon (e-ph) scattering, spin-orbit interaction (SOI), and electron-hole (e-h) interactions come into play collectively. In particular, we provide a direct evidence that e-h exchange interaction plays a dominant role in the fast valley depolarization within a few picoseconds, which is in excellent agreement with experiments. Moreover, there are bright-to-dark exciton transitions induced by e-ph scattering and SOI. Our study proves that e-h many-body effects are essential to understand the spin-valley exciton dynamics in transition metal dichalcogenides and the newly developed GW + rtBSE-NAMD method provides a powerful tool for exciton dynamics in extended systems with time, space, momentum, energy, and spin resolution.

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Research Organization:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1816450

Journal Information:: Science Advances, Vol. 7, Issue 10; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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