Phonon-Assisted Intervalley Scattering Determines Ultrafast Exciton Dynamics in MoSe2 Bilayers

Helmrich, Sophia; Sampson, Kevin; Huang, Di; Selig, Malte; Hao, Kai; Tran, Kha; Achstein, Alexander; Young, Carter; Knorr, Andreas; Malic, Ermin; Woggon, Ulrike; Owschimikow, Nina; Li, Xiaoqin

doi:10.1103/physrevlett.127.157403

Phonon-Assisted Intervalley Scattering Determines Ultrafast Exciton Dynamics in MoSe 2 Bilayers

Journal Article · Fri Oct 08 00:00:00 EDT 2021 · Physical Review Letters

DOI:https://doi.org/10.1103/physrevlett.127.157403· OSTI ID:1980216

Helmrich, Sophia ^[1]; Sampson, Kevin ^[2]; ^[3]; ^[4]; Hao, Kai ^[3]; Tran, Kha ^[3]; Achstein, Alexander ^[4]; ^[3]; Knorr, Andreas ^[4]; Malic, Ermin ^[5]; ^[4]; Owschimikow, Nina ^[4]; ^[2]

Technical Univ. of Berlin (Germany); OSTI
Univ. of Texas, Austin, TX (United States); Univ. of Texas, Austin, TX (United States). Texas Materials Inst. (TMI)
Univ. of Texas, Austin, TX (United States)
Technical Univ. of Berlin (Germany)
Philipps Univ. Marburg (Germany)

While valleys (energy extrema) are present in all band structures of solids, their preeminent role in determining exciton resonances and dynamics in atomically thin transition metal dichalcogenides (TMDC) is unique. Using two-dimensional coherent electronic spectroscopy, we find that exciton decoherence occurs on a much faster timescale in MoSe₂ bilayers than that in the monolayers. We further identify two population relaxation channels in the bilayer, a coherent and an incoherent one. Our microscopic model reveals that phonon-emission processes facilitate scattering events from the K valley to other lower-energy Γ and Λ valleys in the bilayer. Our combined experimental and theoretical studies unequivocally establish different microscopic mechanisms that determine exciton quantum dynamics in TMDC monolayers and bilayers. Understanding exciton quantum dynamics provides critical guidance to the manipulation of spin-valley degrees of freedom in TMDC bilayers.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Texas, Austin, TX (United States)

Sponsoring Organization:: German Research Foundation (DFG); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES); Welch Foundation

Grant/Contract Number:: SC0019398

OSTI ID:: 1980216

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 15 Vol. 127; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Phonon-Assisted Intervalley Scattering Determines Ultrafast Exciton Dynamics in MoSe 2 Bilayers

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