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

Abstract

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.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [4]; ORCiD logo [2]; ORCiD logo [3]
  1. 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
  2. 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
  3. Department of Physics and JILA University of Colorado Boulder CO 80309 USA
  4. Department of Physics and Astronomy Texas A&,M University College Station, TX 77843 USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
2283099
Grant/Contract Number:  
DESC0008807
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
Small
Additional Journal Information:
Journal Name: Small; Journal ID: ISSN 1613-6810
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Luo, Wenjin, Song, Renkang, Whetten, Benjamin G., Huang, Di, Cheng, Xinbin, Belyanin, Alexey, Jiang, Tao, and Raschke, Markus B. Nonlinear Nano‐Imaging of Interlayer Coupling in 2D Graphene‐Semiconductor Heterostructures. Germany: N. p., 2024. Web. doi:10.1002/smll.202307345.
Luo, Wenjin, Song, Renkang, Whetten, Benjamin G., Huang, Di, Cheng, Xinbin, Belyanin, Alexey, Jiang, Tao, & Raschke, Markus B. Nonlinear Nano‐Imaging of Interlayer Coupling in 2D Graphene‐Semiconductor Heterostructures. Germany. https://doi.org/10.1002/smll.202307345
Luo, Wenjin, Song, Renkang, Whetten, Benjamin G., Huang, Di, Cheng, Xinbin, Belyanin, Alexey, Jiang, Tao, and Raschke, Markus B. Fri . "Nonlinear Nano‐Imaging of Interlayer Coupling in 2D Graphene‐Semiconductor Heterostructures". Germany. https://doi.org/10.1002/smll.202307345.
@article{osti_2283099,
title = {Nonlinear Nano‐Imaging of Interlayer Coupling in 2D Graphene‐Semiconductor Heterostructures},
author = {Luo, Wenjin and Song, Renkang and Whetten, Benjamin G. and Huang, Di and Cheng, Xinbin and Belyanin, Alexey and Jiang, Tao and Raschke, Markus B.},
abstractNote = {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.},
doi = {10.1002/smll.202307345},
journal = {Small},
number = ,
volume = ,
place = {Germany},
year = {Fri Jan 26 00:00:00 EST 2024},
month = {Fri Jan 26 00:00:00 EST 2024}
}

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