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Observing dynamic molecular changes at single-molecule level in a cucurbituril based plasmonic molecular junction.

Qiushuang Ai1, Jianghao Zhou2, Jing Guo3

  • 1The State Key Laboratory of Refractories and Metallurgy, Wuhan University of Science and Technology, Wuhan, Hubei, 430081, China. schang23@wust.edu.cn feng_liang@whu.edu.cn and School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan, Hubei, 430081, China and Department of Physics, Florida International University, Miami, Florida, 33199, USA. jinhe@fiu.edu.

Nanoscale
|August 14, 2020
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Summary

Surface-enhanced Raman spectroscopy (SERS) reveals dynamic changes in cucurbit[7]uril (CB[7]) molecular junctions. This technique probes gold-carbonyl interactions and guest molecule rotation within CB[7] cavities for enhanced stability.

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Area of Science:

  • Plasmonics
  • Nanotechnology
  • Spectroscopy

Background:

  • Surface-enhanced Raman spectroscopy (SERS) enables single-molecule sensitivity for molecular interaction studies.
  • Cucurbit[7]uril (CB[7]) based plasmonic molecular junctions offer a platform for investigating dynamic molecular processes.
  • Gold nanoparticles (GNPs) and gold nanoelectrodes (GNEs) are key components in forming these molecular junctions.

Purpose of the Study:

  • To investigate dynamic changes in CB[7]-based plasmonic molecular junctions using SERS.
  • To understand the role of noncovalent interactions and charge transfer in stabilizing these junctions.
  • To reveal the rotational motion of guest molecules within the CB[7] cavity.

Main Methods:

  • Utilizing SERS to analyze molecular junctions formed by GNP adsorption on CB[7]-modified GNEs.
  • Examining bias-dependent spectral changes of the C=O peak to probe gold-carbonyl interactions.
  • Analyzing spectral shifts of the cyclopentadienyl ring to monitor guest molecule orientation and motion.

Main Results:

  • Chemically enhanced Raman peaks were observed due to charge transfer and noncovalent interactions.
  • Positive bias on the GNE strengthened the gold-carbonyl interaction, stabilizing CB[7] junctions.
  • Inclusion of amino-ferrocene stabilized junctions via gold adatom-cyclopentadienyl ring interactions.
  • The rotational motion of amino-ferrocene within the CB[7] cavity was successfully revealed.

Conclusions:

  • SERS is effective in probing dynamic changes and interactions within CB[7] molecular junctions.
  • Noncovalent interactions, including gold-carbonyl and gold adatom-guest molecule interactions, are crucial for junction stability.
  • The orientation and motion of guest molecules can be precisely monitored through SERS analysis.