Nonlinear Nano‐Imaging of Interlayer Coupling in 2D Graphene‐Semiconductor Heterostructures

Luo, Wenjin; Song, Renkang; Whetten, Benjamin G.; Huang, Di; Cheng, Xinbin; Belyanin, Alexey; Jiang, Tao; Raschke, Markus B.

doi:10.1002/smll.202307345

Title: Nonlinear Nano‐Imaging of Interlayer Coupling in 2D Graphene‐Semiconductor Heterostructures

Journal Article · Fri Jan 26 00:00:00 EST 2024 · Small

DOI:https://doi.org/10.1002/smll.202307345· OSTI ID:2283099

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MOE Key Laboratory of Advanced Micro‐Structured Materials Shanghai Frontiers Science Center of Digital Optics Institute of Precision Optical Engineering and School of Physics Science and Engineering Tongji University Shanghai 200092 China, Department of Physics and JILA University of Colorado Boulder CO 80309 USA
MOE Key Laboratory of Advanced Micro‐Structured Materials Shanghai Frontiers Science Center of Digital Optics Institute of Precision Optical Engineering and School of Physics Science and Engineering Tongji University Shanghai 200092 China
Department of Physics and JILA University of Colorado Boulder CO 80309 USA
Department of Physics and Astronomy Texas A&,M University College Station, TX 77843 USA

Abstract The emergent electronic, spin, and other quantum properties of 2D heterostructures of graphene and transition metal dichalcogenides are controlled by the underlying interlayer coupling and associated charge and energy transfer dynamics. However, these processes are sensitive to interlayer distance and crystallographic orientation, which are in turn affected by defects, grain boundaries, or other nanoscale heterogeneities. This obfuscates the distinction between interlayer charge and energy transfer. Here, nanoscale imaging in coherent four‐wave mixing (FWM) and incoherent two‐photon photoluminescence (2PPL) is combined with a tip distance‐dependent coupled rate equation model to resolve the underlying intra‐ and inter‐layer dynamics while avoiding the influence of structural heterogeneities in mono‐ to multi‐layer graphene/WSe ₂ heterostructures. With selective insertion of hBN spacer layers, it is shown that energy, as opposed to charge transfer, dominates the interlayer‐coupled optical response. From the distinct nano‐FWM and ‐2PPL tip‐sample distance‐dependent modification of interlayer and intralayer relaxation by tip‐induced enhancement and quenching, an interlayer energy transfer time of ps consistent with recent reports is derived. As a local probe technique, this approach highlights the ability to determine intrinsic sample properties even in the presence of large sample heterogeneity.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: DESC0008807

OSTI ID:: 2283099

Journal Information:: Small, Journal Name: Small; ISSN 1613-6810

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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