Exciton fine structure in twisted transition metal dichalcogenide heterostructures

Abstract Moiré superlattices of transition metal dichalcogenide (TMD) heterostructures give rise to rich excitonic phenomena associated with the interlayer twist angle. Theoretical calculations of excitons in such systems are typically based on model moiré potentials that mitigate the computational...

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Main Authors: Sudipta Kundu, Tomer Amit, H. R. Krishnamurthy, Manish Jain, Sivan Refaely-Abramson
Format: Article
Language:English
Published: Nature Portfolio 2023-10-01
Series:npj Computational Materials
Online Access:https://doi.org/10.1038/s41524-023-01145-x
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author Sudipta Kundu
Tomer Amit
H. R. Krishnamurthy
Manish Jain
Sivan Refaely-Abramson
author_facet Sudipta Kundu
Tomer Amit
H. R. Krishnamurthy
Manish Jain
Sivan Refaely-Abramson
author_sort Sudipta Kundu
collection DOAJ
description Abstract Moiré superlattices of transition metal dichalcogenide (TMD) heterostructures give rise to rich excitonic phenomena associated with the interlayer twist angle. Theoretical calculations of excitons in such systems are typically based on model moiré potentials that mitigate the computational cost. However, predictive understanding of the electron-hole coupling dominating the excitations is crucial to realize the twist-induced modifications of the optical selection rules. In this work, we use many-body perturbation theory to evaluate the relation between twist angle and exciton properties in TMD heterostructures. We present an approach for unfolding excitonic states from the moiré Brillouin zone onto the separate-layer ones. Applying this method to a large-angle twisted MoS2/MoSe2 bilayer, we find that the optical spectrum is dominated by mixed electron–hole transitions with different momenta in the separate monolayers, leading to unexpected hybridization between interlayer and intralayer excitons. Our findings offer a design pathway for exciton layer-localization in TMD heterostructures.
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publishDate 2023-10-01
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spelling doaj-art-f09a8f4ed58249d3bddc697c9e903dc62024-12-08T12:37:40ZengNature Portfolionpj Computational Materials2057-39602023-10-01911710.1038/s41524-023-01145-xExciton fine structure in twisted transition metal dichalcogenide heterostructuresSudipta Kundu0Tomer Amit1H. R. Krishnamurthy2Manish Jain3Sivan Refaely-Abramson4Centre for Condensed Matter Theory, Department of Physics, Indian Institute of ScienceDepartment of Molecular Chemistry and Materials Science, Weizmann Institute of ScienceCentre for Condensed Matter Theory, Department of Physics, Indian Institute of ScienceCentre for Condensed Matter Theory, Department of Physics, Indian Institute of ScienceDepartment of Molecular Chemistry and Materials Science, Weizmann Institute of ScienceAbstract Moiré superlattices of transition metal dichalcogenide (TMD) heterostructures give rise to rich excitonic phenomena associated with the interlayer twist angle. Theoretical calculations of excitons in such systems are typically based on model moiré potentials that mitigate the computational cost. However, predictive understanding of the electron-hole coupling dominating the excitations is crucial to realize the twist-induced modifications of the optical selection rules. In this work, we use many-body perturbation theory to evaluate the relation between twist angle and exciton properties in TMD heterostructures. We present an approach for unfolding excitonic states from the moiré Brillouin zone onto the separate-layer ones. Applying this method to a large-angle twisted MoS2/MoSe2 bilayer, we find that the optical spectrum is dominated by mixed electron–hole transitions with different momenta in the separate monolayers, leading to unexpected hybridization between interlayer and intralayer excitons. Our findings offer a design pathway for exciton layer-localization in TMD heterostructures.https://doi.org/10.1038/s41524-023-01145-x
spellingShingle Sudipta Kundu
Tomer Amit
H. R. Krishnamurthy
Manish Jain
Sivan Refaely-Abramson
Exciton fine structure in twisted transition metal dichalcogenide heterostructures
npj Computational Materials
title Exciton fine structure in twisted transition metal dichalcogenide heterostructures
title_full Exciton fine structure in twisted transition metal dichalcogenide heterostructures
title_fullStr Exciton fine structure in twisted transition metal dichalcogenide heterostructures
title_full_unstemmed Exciton fine structure in twisted transition metal dichalcogenide heterostructures
title_short Exciton fine structure in twisted transition metal dichalcogenide heterostructures
title_sort exciton fine structure in twisted transition metal dichalcogenide heterostructures
url https://doi.org/10.1038/s41524-023-01145-x
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AT hrkrishnamurthy excitonfinestructureintwistedtransitionmetaldichalcogenideheterostructures
AT manishjain excitonfinestructureintwistedtransitionmetaldichalcogenideheterostructures
AT sivanrefaelyabramson excitonfinestructureintwistedtransitionmetaldichalcogenideheterostructures