Gate-Switchable Molecular Diffusion on a Graphene Field-Effect Transistor

Controlling the surface diffusion of particles on 2D devices creates opportunities for advancing microscopic processes such as nanoassembly, thin-film growth, and catalysis. Here, we demonstrate the ability to control the diffusion of F<sub>4</sub>TCNQ molecules at the surface of clean graphene field-effect transistors (FETs) via electrostatic gating. Tuning the back-gate voltage (<i>V</i><sub>G</sub>) of a graphene FET switches molecular adsorbates between negative and neutral charge states, leading to dramatic changes in their diffusion properties. Scanning tunneling microscopy measurements reveal that the diffusivity of neutral molecules decreases rapidly with a decreasing <i>V</i><sub>G</sub> and involves rotational diffusion processes. The molecular diffusivity of negatively charged molecules, on the other hand, remains nearly constant over a wide range of applied <i>V</i><sub>G</sub> values and is dominated by purely translational processes. First-principles density functional theory calculations confirm that the energy landscapes experienced by neutral vs charged molecules lead to diffusion behavior consistent with experiment. Gate-tunability of the diffusion barrier for F<sub>4</sub>TCNQ molecules on graphene enables graphene FETs to act as diffusion switches.

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Publication Details

Journal
ACS Nano
Published
2024-08-19
DOI
https://doi.org/10.1021/acsnano.4c05808
Citations
3
Primary Topic
Graphene research and applications
Type
article
Field-Weighted Citation Impact
0.35

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article

Gate-Switchable Molecular Diffusion on a Graphene Field-Effect Transistor

Yiming Yang, Xiaomin Xu, Zhichao Cheng, Sergey Trishin et al.
3 citations
ACS Nano
Graphene research and applications
0.35
article

Gate-Switchable Molecular Diffusion on a Graphene Field-Effect Transistor

Yiming Yang, Xiaomin Xu, Zhichao Cheng, Sergey Trishin, Franklin Liou, Johannes Lischner, Zachary A. H. Goodwin, Sergio Pezzini, Andrew S. Aikawa, Michael F. Crommie, Shizhe Zhou, Takashi Taniguchi, Kenji Watanabe, V. Bellani, Feng Wang, Hsin‐Zon Tsai, Luc Nguyen, Brian R. P. Angeles, Paul W. Roberts
article en
3 citations

Abstract

Controlling the surface diffusion of particles on 2D devices creates opportunities for advancing microscopic processes such as nanoassembly, thin-film growth, and catalysis. Here, we demonstrate the ability to control the diffusion of F<sub>4</sub>TCNQ molecules at the surface of clean graphene field-effect transistors (FETs) via electrostatic gating. Tuning the back-gate voltage (<i>V</i><sub>G</sub>) of a graphene FET switches molecular adsorbates between negative and neutral charge states, leading to dramatic changes in their diffusion properties. Scanning tunneling microscopy measurements reveal that the diffusivity of neutral molecules decreases rapidly with a decreasing <i>V</i><sub>G</sub> and involves rotational diffusion processes. The molecular diffusivity of negatively charged molecules, on the other hand, remains nearly constant over a wide range of applied <i>V</i><sub>G</sub> values and is dominated by purely translational processes. First-principles density functional theory calculations confirm that the energy landscapes experienced by neutral vs charged molecules lead to diffusion behavior consistent with experiment. Gate-tunability of the diffusion barrier for F<sub>4</sub>TCNQ molecules on graphene enables graphene FETs to act as diffusion switches.

ACS NanoVol. 18(35)
Harvard University (US), Lawrence Berkeley National Laboratory (US), Scuola Normale Superiore (IT), National Institute for Materials Science (JP), University of Pavia (IT), ShanghaiTech University (CN), Istituto Nanoscienze (IT), Tsinghua–Berkeley Shenzhen Institute (CN), Kavli Energy NanoScience Institute (US), Imperial College London (GB), University of California, Berkeley (US), Tsinghua University (CN)
University of California Berkeley, Ministry of Education, Culture, Sports, Science and Technology, Thomas Young Centre, Engineering and Physical Sciences Research Council, Japan Society for the Promotion of Science
Affordable and clean energy
Openalex Percentile: Top 45%
Graphene research and applications
0.35
DOISourceOpenAlex
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