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Ultrahigh Photoluminescence Quenching (>90%) and Negative Photoresponse in Vertically Stacked Graphene/WSe2 van der Waals Heterojunctions
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    Ultrahigh Photoluminescence Quenching (>90%) and Negative Photoresponse in Vertically Stacked Graphene/WSe2 van der Waals Heterojunctions
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    • Yao Feng
      Yao Feng
      School of Physics, Beijing Institute of Technology, Beijing 100081, P. R. China
      More by Yao Feng
    • Ze Cao
      Ze Cao
      School of Physics, Beijing Institute of Technology, Beijing 100081, P. R. China
      More by Ze Cao
    • Longkun Yang
      Longkun Yang
      Beijing Key Laboratory for Nano-Photonics and Nano-Structure (NPNS), Department of Physics, Capital Normal University, Beijing 100048, P. R. China
      More by Longkun Yang
      Orcidhttp://orcid.org/0000-0002-4378-3717
    • Mingyu Shi
      Mingyu Shi
      School of Physics, Beijing Institute of Technology, Beijing 100081, P. R. China
      More by Mingyu Shi
    • Yujing Fan
      Yujing Fan
      School of Physics, Beijing Institute of Technology, Beijing 100081, P. R. China
      More by Yujing Fan
    • Zhuoshuai Huang
      Zhuoshuai Huang
      School of Physics, Beijing Institute of Technology, Beijing 100081, P. R. China
      More by Zhuoshuai Huang
    • Mohamed Abid
      Mohamed Abid
      EduAI Dynamics, Akhmet Baitursynuly 63, Astana 010000, Kazakhstan
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    • Fengjiang An
      Fengjiang An
      State Key Laboratory of Explosion Science and Safety, Beijing Institute of Technology, Beijing 100081, P. R. China
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    • Huei-Ru Fuh*
      Huei-Ru Fuh
      Department of Chemical Engineering & Materials Science, Yuan Ze University, Taoyuan City 320, Taiwan, ROC
      *Email: hrfuh@saturn.yzu.edu.tw
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    • Yuh-Renn Wu*
      Yuh-Renn Wu
      Graduate Institute of Photonics and Optoelectronics and Department of Electrical Engineering, National Taiwan University, Taipei 10617, Taiwan, ROC
      *Email: yrwu@ntu.edu.tw
      More by Yuh-Renn Wu
    • Ching-Ray Chang*
      Ching-Ray Chang
      Quantum Information Center, Chung Yuan Christian University, Taoyuan 32023, Taiwan, ROC
      Department of Physics, National Taiwan University, Taipei 106, Taiwan, ROC
      *Email: crchang@phys.ntu.edu.tw
      More by Ching-Ray Chang
      Orcidhttp://orcid.org/0000-0003-1974-9583
    • Han-Chun Wu*
      Han-Chun Wu
      School of Physics, Beijing Institute of Technology, Beijing 100081, P. R. China
      *Email: wuhc@bit.edu.cn
      More by Han-Chun Wu
      Orcidhttp://orcid.org/0000-0003-0293-9022
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    ACS Applied Electronic Materials

    Cite this: ACS Appl. Electron. Mater. 2026, 8, 12, 5124–5133
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    https://doi.org/10.1021/acsaelm.6c00961
    Published June 10, 2026
    © 2026 American Chemical Society
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    Abstract

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    The interface effect plays a crucial role in determining the performance of van der Waals heterojunctions. Here, we fabricated graphene/WSe2 heterojunctions and investigated how graphene proximity dramatically alters their optical, electrical, and photoelectrical properties. It was found that graphene proximity induces ultrahigh photoluminescence quenching exceeding 90%, accompanied by substantial effective hole depletion in the WSe2 layer due to strong interfacial charge transfer. Photo illumination can further enhance charge transfer and charge accumulation at the interface. Electrical characterization shows that gate voltage effectively modulates interfacial charge transfer and thus the tunneling behavior. Notably, a transition from positive to negative photoresponse emerges when the effective tunneling barrier width is reduced below ∼1 nm, highlighting a tunneling-controlled photoresponse mechanism governed by the competition between interfacial charge transfer and bias-induced electric fields. These results provide comprehensive insights into interlayer charge transfer, exciton dynamics, and tunable photoelectrical properties in graphene/WSe2 heterostructures, paving the way for next-generation optoelectronic devices based on 2D vdW materials.

    © 2026 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsaelm.6c00961.

    • Topographical AFM images and corresponding height profiles of individual graphene and WSe2 layers; Raman spectra of WSe2 and overlapping graphene/WSe2 areas under 532 nm laser excitation; Ids–Vg transfer curves of isolated graphene measured in the dark; schematic of the interlayer charge transfer between graphene and WSe2; optical images of the device before and after graphene transfer onto WSe2; Ids–Vds curves of the device before and after graphene transfer onto WSe2; Ids–Vg transfer curves of the device before and after graphene transfer onto WSe2; Ids–Vg transfer curves of sample 2 measured with a bias voltage of 3 V; Ids–Vds curves of graphene/WSe2 heterojunction measured under a variety of gate voltages; calculated barrier height as a function of gate voltages; and calculated photoresponsivity (R) as a function of incident power density at Vds = 2 V for a variety of gate voltages (DOCX)

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    ACS Applied Electronic Materials

    Cite this: ACS Appl. Electron. Mater. 2026, 8, 12, 5124–5133
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsaelm.6c00961
    Published June 10, 2026
    © 2026 American Chemical Society
    Request reuse permissions

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