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Revealing the molecular structure of single-molecule junctions in different conductance states by fishing-mode tip-enhanced Raman spectroscopy

Author

Listed:
  • Zheng Liu

    (State Key Laboratory of Physical Chemistry of Solid Surfaces and Key Laboratory of Analytical Sciences, College of Chemistry and Chemical Engineering, Xiamen University)

  • Song-Yuan Ding

    (State Key Laboratory of Physical Chemistry of Solid Surfaces and Key Laboratory of Analytical Sciences, College of Chemistry and Chemical Engineering, Xiamen University)

  • Zhao-Bin Chen

    (State Key Laboratory of Physical Chemistry of Solid Surfaces and Key Laboratory of Analytical Sciences, College of Chemistry and Chemical Engineering, Xiamen University)

  • Xiang Wang

    (State Key Laboratory of Physical Chemistry of Solid Surfaces and Key Laboratory of Analytical Sciences, College of Chemistry and Chemical Engineering, Xiamen University)

  • Jing-Hua Tian

    (State Key Laboratory of Physical Chemistry of Solid Surfaces and Key Laboratory of Analytical Sciences, College of Chemistry and Chemical Engineering, Xiamen University)

  • Jason R. Anema

    (State Key Laboratory of Physical Chemistry of Solid Surfaces and Key Laboratory of Analytical Sciences, College of Chemistry and Chemical Engineering, Xiamen University)

  • Xiao-Shun Zhou

    (State Key Laboratory of Physical Chemistry of Solid Surfaces and Key Laboratory of Analytical Sciences, College of Chemistry and Chemical Engineering, Xiamen University)

  • De-Yin Wu

    (State Key Laboratory of Physical Chemistry of Solid Surfaces and Key Laboratory of Analytical Sciences, College of Chemistry and Chemical Engineering, Xiamen University)

  • Bing-Wei Mao

    (State Key Laboratory of Physical Chemistry of Solid Surfaces and Key Laboratory of Analytical Sciences, College of Chemistry and Chemical Engineering, Xiamen University)

  • Xin Xu

    (State Key Laboratory of Physical Chemistry of Solid Surfaces and Key Laboratory of Analytical Sciences, College of Chemistry and Chemical Engineering, Xiamen University)

  • Bin Ren

    (State Key Laboratory of Physical Chemistry of Solid Surfaces and Key Laboratory of Analytical Sciences, College of Chemistry and Chemical Engineering, Xiamen University)

  • Zhong-Qun Tian

    (State Key Laboratory of Physical Chemistry of Solid Surfaces and Key Laboratory of Analytical Sciences, College of Chemistry and Chemical Engineering, Xiamen University)

Abstract

The conductance of single-molecule junctions may be governed by the structure of the molecule in the gap or by the way it bonds with the leads, and the information contained in a Raman spectrum is ideal for examining both. Here we demonstrate that molecule-to-surface bonding may be characterized during electron transport by 'fishing-mode' tip-enhanced Raman spectroscopy (FM-TERS). This technique allows mutually verifiable single-molecule conductance and Raman signals with single-molecule contributions to be acquired simultaneously at room temperature. Density functional theory calculations reveal that the most significant spectral change seen for a gold-4,4′-bipyridine-gold junction results from the deformation of the pyridine ring in contact with the drain electrode at high voltage, and these calculations suggest that a stronger bonding interaction between the molecule and the drain may account for the nonlinear dependence of conductance on bias voltage. FM-TERS will lead to a better understanding of electron-transport processes in molecular junctions.

Suggested Citation

  • Zheng Liu & Song-Yuan Ding & Zhao-Bin Chen & Xiang Wang & Jing-Hua Tian & Jason R. Anema & Xiao-Shun Zhou & De-Yin Wu & Bing-Wei Mao & Xin Xu & Bin Ren & Zhong-Qun Tian, 2011. "Revealing the molecular structure of single-molecule junctions in different conductance states by fishing-mode tip-enhanced Raman spectroscopy," Nature Communications, Nature, vol. 2(1), pages 1-6, September.
    • Handle: RePEc:nat:natcom:v:2:y:2011:i:1:d:10.1038_ncomms1310
    DOI: 10.1038/ncomms1310
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    Cited by:

    1. Ling Tong & Zhou Yu & Yi-Jing Gao & Xiao-Chong Li & Ju-Fang Zheng & Yong Shao & Ya-Hao Wang & Xiao-Shun Zhou, 2023. "Local cation-tuned reversible single-molecule switch in electric double layer," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Youngwook Park & Ikutaro Hamada & Adnan Hammud & Takashi Kumagai & Martin Wolf & Akitoshi Shiotari, 2024. "Atomic-precision control of plasmon-induced single-molecule switching in a metal–semiconductor nanojunction," Nature Communications, Nature, vol. 15(1), pages 1-9, December.

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