Transition metal dichalcogenides (TMDs) are regarded as a possible material platform for quantum information science and related device applications. In TMD monolayers, the dephasing time and inhomogeneity are crucial parameters for any quantum information application. In TMD heterostructures, coupling strength and interlayer exciton lifetimes are also parameters of interest. However, many demonstrations in TMDs can only be realized at specific spots on the sample, presenting a challenge to the scalability of these applications. Here, using multi-dimensional coherent imaging spectroscopy, we shed light on the underlying physics—including dephasing, inhomogeneity, and strain—for a MoSe2 monolayer and identify both promising and unfavorable areas for quantum information applications. We, furthermore, apply the same technique to a MoSe2/WSe2 heterostructure. Despite the notable presence of strain and dielectric environment changes, coherent and incoherent coupling and interlayer exciton lifetimes are mostly robust across the sample. This uniformity is despite a significantly inhomogeneous interlayer exciton photoluminescence distribution that suggests a bad sample for device applications. This robustness strengthens the case for TMDs as a next-generation material platform in quantum information science and beyond.
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7 June 2022
Research Article|
June 01 2022
Imaging dynamic exciton interactions and coupling in transition metal dichalcogenides
Special Collection:
Low-Dimensional Materials for Quantum Information Science
,
JCP Editors' Choice 2022
Torben L. Purz
;
Torben L. Purz
1
Department of Physics, University of Michigan
, Ann Arbor, Michigan 48109-1040, USA
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Eric W. Martin
;
Eric W. Martin
2
MONSTR Sense Technologies LLC
, Ann Abor, Michigan 48104, USA
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William G. Holtzmann;
William G. Holtzmann
3
Department of Physics, University of Washington
, Seattle, Washington 98195-1560, USA
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Pasqual Rivera
;
Pasqual Rivera
3
Department of Physics, University of Washington
, Seattle, Washington 98195-1560, USA
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Adam Alfrey;
Adam Alfrey
1
Department of Physics, University of Michigan
, Ann Arbor, Michigan 48109-1040, USA
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Kelsey M. Bates
;
Kelsey M. Bates
1
Department of Physics, University of Michigan
, Ann Arbor, Michigan 48109-1040, USA
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Hui Deng
;
Hui Deng
1
Department of Physics, University of Michigan
, Ann Arbor, Michigan 48109-1040, USA
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Xiaodong Xu;
Xiaodong Xu
3
Department of Physics, University of Washington
, Seattle, Washington 98195-1560, USA
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Steven T. Cundiff
Steven T. Cundiff
a)
1
Department of Physics, University of Michigan
, Ann Arbor, Michigan 48109-1040, USA
a)Author to whom correspondence should be addressed: cundiff@umich.edu
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a)Author to whom correspondence should be addressed: cundiff@umich.edu
J. Chem. Phys. 156, 214704 (2022)
Article history
Received:
February 07 2022
Accepted:
April 21 2022
Citation
Torben L. Purz, Eric W. Martin, William G. Holtzmann, Pasqual Rivera, Adam Alfrey, Kelsey M. Bates, Hui Deng, Xiaodong Xu, Steven T. Cundiff; Imaging dynamic exciton interactions and coupling in transition metal dichalcogenides. J. Chem. Phys. 7 June 2022; 156 (21): 214704. https://doi.org/10.1063/5.0087544
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