Anomalous Interlayer Exciton Diffusion in WS2/WSe2 Moiré Heterostructure

Rossi, Antonio; Zipfel, Jonas; Maity, Indrajit; Lorenzon, Monica; Dandu, Medha; Barré, Elyse; Francaviglia, Luca; Regan, Emma C.; Zhang, Zuocheng; Nie, Jacob H.; Barnard, Edward S.; Watanabe, Kenji; Taniguchi, Takashi; Rotenberg, Eli; Wang, Feng; Lischner, Johannes; Raja, Archana; Weber-Bargioni, Alexander

doi:10.1021/acsnano.4c00015

Anomalous Interlayer Exciton Diffusion in WS₂/WSe₂ Moiré Heterostructure

Journal Article · Mon Jul 01 00:00:00 EDT 2024 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.4c00015· OSTI ID:2446598

^[1]; Zipfel, Jonas ^[2]; ^[3]; Lorenzon, Monica ^[2]; ^[2]; ^[2]; Francaviglia, Luca ^[2]; Regan, Emma C. ^[4]; Zhang, Zuocheng ^[4]; Nie, Jacob H. ^[5]; Barnard, Edward S. ^[2]; ^[6]; ^[6]; ^[7]; Wang, Feng ^[4]; ^[3]; ^[2]; Weber-Bargioni, Alexander ^[2]

Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry; Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Instituto Italiano di Tecnologia, Pisa (Italy)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry
Imperial College, London (United Kingdom)
Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Univ. of California, Santa Barbara, CA (United States)
National Institute for Materials Science (NIMS), Tsukuba (Japan)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)

Stacking van der Waals crystals allows for the on-demand creation of a periodic potential landscape to tailor the transport of quasiparticle excitations. We investigate the diffusion of photoexcited electron-hole pairs, or excitons, at the interface of WS₂/WSe₂ van der Waals heterostructure over a wide range of temperatures. We observe the appearance of distinct interlayer excitons for parallel and antiparallel stacking and track their diffusion through spatially and temporally resolved photoluminescence spectroscopy from 30 to 250 K. While the measured exciton diffusivity decreases with temperature, it surprisingly plateaus below 90 K. Our observations cannot be explained by classical models like hopping in the moiré potential. A combination of ab initio theory and molecular dynamics simulations suggests that low-energy phonons arising from the mismatched lattices of moiré heterostructures, also known as phasons, play a key role in describing and understanding this anomalous behavior of exciton diffusion. Our observations indicate that the moiré potential landscape is dynamic down to very low temperatures and that the phason modes can enable efficient transport of energy in the form of excitons.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; SC0022289

OSTI ID:: 2446598

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 28 Vol. 18; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Anomalous Interlayer Exciton Diffusion in WS2/WSe2 Moiré Heterostructure

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Anomalous Interlayer Exciton Diffusion in WS₂/WSe₂ Moiré Heterostructure