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

Roberto Rosati (), Ioannis Paradisanos, Libai Huang, Ziyang Gan, Antony George, Kenji Watanabe, Takashi Taniguchi, Laurent Lombez, Pierre Renucci, Andrey Turchanin, Bernhard Urbaszek and Ermin Malic
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Roberto Rosati: Philipps-Universität Marburg
Ioannis Paradisanos: LPCNO
Libai Huang: Purdue University
Ziyang Gan: Institute of Physical Chemistry
Antony George: Institute of Physical Chemistry
Kenji Watanabe: National Institute for Materials Science
Takashi Taniguchi: National Institute for Materials Science
Laurent Lombez: LPCNO
Pierre Renucci: LPCNO
Andrey Turchanin: Institute of Physical Chemistry
Bernhard Urbaszek: LPCNO
Ermin Malic: Philipps-Universität Marburg

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: Abstract 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.

Date: 2023
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DOI: 10.1038/s41467-023-37889-9

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