Interface engineering of charge-transfer excitons in 2D lateral heterostructures

The existence of bound charge transfer (CT) excitons at the interface of monolayer lateral heterojunctions has been debated in literature, but contrary to the case of interlayer excitons in vertical heterostructure their observation still has to be confirmed. Here, we present a microscopic study inv...

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Main Authors: Rosati, Roberto, Paradisanos, Ioannis, Huang, Libai, Gan, Ziyang, George, Antony, Watanabe, Kenji, Taniguchi, Takashi, Lombez, Laurent, Renucci, Pierre, Turchanin, Andrey, Urbaszek, Bernhard, Malic, Ermin
Format: Article
Language:English
Published: Philipps-Universität Marburg 2023
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Summary:The existence of bound charge transfer (CT) excitons at the interface of monolayer lateral heterojunctions has been debated in literature, but contrary to the case of interlayer excitons in vertical heterostructure their observation still has to be confirmed. Here, we present a microscopic study investigating signatures of bound CT excitons in photoluminescence spectra at the interface of hBN-encapsulated lateral MoSe2-WSe2 heterostructures. Based on a fully microscopic and material-specific theory, we reveal the many-particle processes behind the formation of CT excitons and how they can be tuned via interface- and dielectric engineering. For junction widths smaller than the Coulomb-induced Bohr radius we predict the appearance of a low-energy CT exciton. The theoretical prediction is compared with experimental low-temperature photoluminescence measurements showing emission in the bound CT excitons energy range. We show that for hBN-encapsulated heterostructures, CT excitons exhibit small binding energies of just a few tens meV and at the same time large dipole moments, making them promising materials for optoelectronic applications (benefiting from an efficient exciton dissociation and fast dipole-driven exciton propagation). Our joint theory-experiment study presents a significant step towards a microscopic understanding of optical properties of technologically promising 2D lateral heterostructures.
Item Description:Gefördert durch den Open-Access-Publikationsfonds der UB Marburg.
DOI:10.1038/s41467-023-37889-9