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

Zheng Liu, Song-Yuan Ding, Zhao-Bin Chen, Xiang Wang, Jing-Hua Tian, Jason R. Anema, Xiao-Shun Zhou, Wu De-Yin, Bing-Wei Mao, Xin Xu, Bin Ren () and Zhong-Qun Tian
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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
Wu De-Yin: 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

Nature Communications, 2011, vol. 2, issue 1, 1-6

Abstract: 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.

Date: 2011
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DOI: 10.1038/ncomms1310

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