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Reduced Absorption Due to Defect-Localized Interlayer Excitons in Transition-Metal Dichalcogenide-Graphene Heterostructures.
Nano Letters 2023 June 23
Associating atomic vacancies to excited-state transport phenomena in two-dimensional semiconductors demands a detailed understanding of the exciton transitions involved. We study the effect of such defects on the electronic and optical properties of WS2 -graphene and MoS2 -graphene van der Waals heterobilayers, employing many-body perturbation theory. We find that chalcogen defects and the graphene interface radically alter the optical properties of the transition-metal dichalcogenide in the heterobilayer, due to a combination of dielectric screening and the many-body nature of defect-induced intralayer and interlayer optical transitions. By analyzing the intrinsic radiative rates of the subgap excitonic features, we show that while defects introduce low-lying optical transitions, resulting in excitons with non-negligible oscillator strength, they decrease the optical response of the pristine-like transition-metal dichalcogenide intralayer excitons. Our findings relate excitonic features with interface design for defect engineering in photovoltaic and transport applications.
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