Twist Angle-Dependent Interlayer Exciton Lifetimes in van der Waals Heterostructures

Choi, Junho; Florian, Matthias; Steinhoff, Alexander; Erben, Daniel; Tran, Kha; Kim, Dong Seob; Sun, Liuyang; Quan, Jiamin; Claassen, Robert; Majumder, Somak; Hollingsworth, Jennifer A.; Taniguchi, Takashi; Watanabe, Kenji; Ueno, Keiji; Singh, Akshay; Moody, Galan; Jahnke, Frank; Li, Xiaoqin

doi:10.1103/physrevlett.126.047401

Twist Angle-Dependent Interlayer Exciton Lifetimes in van der Waals Heterostructures

Journal Article · Tue Jan 26 00:00:00 EST 2021 · Physical Review Letters

DOI:https://doi.org/10.1103/physrevlett.126.047401· OSTI ID:1764224

^[1]; Florian, Matthias ^[2]; Steinhoff, Alexander ^[2]; ^[2]; Tran, Kha ^[1]; Kim, Dong Seob ^[1]; Sun, Liuyang ^[1]; Quan, Jiamin ^[1]; ^[1]; ^[3]; ^[3]; Taniguchi, Takashi ^[4]; Watanabe, Kenji ^[5]; ^[6]; ^[7]; Moody, Galan ^[8]; Jahnke, Frank ^[2]; Li, Xiaoqin ^[1]

Univ. of Texas, Austin, TX (United States). Center for Complex Quantum Systems
Univ. of Bremen (Germany). Inst. for Theoretical Physics
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT)
National Inst. for Materials Science, Ibaraki (Japan). International Center for Materials Nanoarchitectonics
National Inst. for Materials Science, Ibaraki (Japan). Research Center for Functional Materials
Saitama Univ. (Japan)
Indian Inst. of Science, Bengaluru (India)
Univ. of California, Santa Barbara, CA (United States)

In van der Waals (vdW) heterostructures formed by stacking two monolayers of transition metal dichalcogenides, multiple exciton resonances with highly tunable properties are formed and subject to both vertical and lateral confinement. We investigate how a unique control knob, the twist angle between the two monolayers, can be used to control the exciton dynamics. We observe that the interlayer exciton lifetimes in MoSe₂/WSe₂ twisted bilayers (TBLs) change by one order of magnitude when the twist angle is varied from 1° to 3.5°. Additionally, using a low-energy continuum model, we theoretically separate two leading mechanisms that influence interlayer exciton radiative lifetimes. The shift to indirect transitions in the momentum space with an increasing twist angle and the energy modulation from the moiré potential both have a significant impact on interlayer exciton lifetimes. We further predict distinct temperature dependence of interlayer exciton lifetimes in TBLs with different twist angles, which is partially validated by experiments. While many recent studies have highlighted how the twist angle in a vdW TBL can be used to engineer the ground states and quantum phases due to many-body interaction, our studies explore its role in controlling the dynamics of optically excited states, thus, expanding the conceptual applications of “twistronics”.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: German Research Foundation (DFG); JSPS KAKENHI; Japan MEXT; National Science Foundation; USDOE Office of Energy Efficiency and Renewable Energy (EERE); Welch Foundation

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1764224

Alternate ID(s):: OSTI ID: 1859894

Report Number(s):: LA-UR--20-28296; LA-UR-20-28297

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 4 Vol. 126; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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