Oxygen-Induced In Situ Manipulation of the Interlayer Coupling and Exciton Recombination in Bi2Se3/MoS2 2D Heterostructures

Hennighausen, Zachariah; Lane, Christopher; Benabbas, Abdelkrim; Mendez, Kevin; Eggenberger, Monika; Champion, Paul M.; Robinson, Jeremy T.; Bansil, Arun; Kar, Swastik

doi:10.1021/acsami.9b02929

Title: Oxygen-Induced In Situ Manipulation of the Interlayer Coupling and Exciton Recombination in Bi₂Se₃/MoS₂ 2D Heterostructures

Journal Article · Mon Apr 08 00:00:00 EDT 2019 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.9b02929· OSTI ID:1527368

^[1];

^[1]; Benabbas, Abdelkrim ^[2]; Mendez, Kevin ^[1]; Eggenberger, Monika ^[1]; Champion, Paul M. ^[2];

^[3]; Bansil, Arun ^[2]; Kar, Swastik ^[1]

Northeastern Univ., Boston, MA (United States). Dept. of Physics
Northeastern Univ., Boston, MA (United States). Physics Dept. and Center for Interdisciplinary Research on Complex Systems
Naval Research Lab. (NRL), Washington, DC (United States)

Two-dimensional (2D) heterostructures are more than a sum of the parent 2D materials, but are also a product of the interlayer coupling, which can induce new properties. In this paper, we present a method to tune the interlayer coupling in Bi₂Se₃/MoS₂ 2D heterostructures by regulating the oxygen presence in the atmosphere, while applying laser or thermal energy. Our data suggest that the interlayer coupling is tuned through the diffusive intercalation and deintercalation of oxygen molecules. When one layer of Bi₂Se₃ is grown on monolayer MoS₂, an influential interlayer coupling is formed, which quenches the signature photoluminescence (PL) peaks. However, thermally treating in the presence of oxygen disrupts the interlayer coupling, facilitating the emergence of the MoS₂ PL peak. Our density functional theory calculations predict that intercalated oxygen increases the interlayer separation ∼17%, disrupting the interlayer coupling and inducing the layers to behave more electronically independent. The interlayer coupling can then be restored by thermally treating in N₂ or Ar, where the peaks will requench. Hence, this is an interesting oxygen-induced switching between “non-radiative” and “radiative” exciton recombination. This switching can also be accomplished locally, controllably, and reversibly using a low-power focused laser, while changing the environment from pure N₂ to air. This allows for the interlayer coupling to be precisely manipulated with submicron spatial resolution, facilitating site-programmable 2D light-emitting pixels whose emission intensity could be precisely varied by a factor exceeding 200×. Our results show that these atomically thin 2D heterostructures may be excellent candidates for oxygen sensing.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Complex Materials from First Principles (CCM); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-07ER46352; AC02-05CH11231; SC0012575

OSTI ID:: 1527368

Journal Information:: ACS Applied Materials and Interfaces, Vol. 11, Issue 17; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 18 works

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Title: Oxygen-Induced In Situ Manipulation of the Interlayer Coupling and Exciton Recombination in Bi2Se3/MoS2 2D Heterostructures

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Title: Oxygen-Induced In Situ Manipulation of the Interlayer Coupling and Exciton Recombination in Bi₂Se₃/MoS₂ 2D Heterostructures