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Modulating and probing the dynamic intermolecular interactions in plasmonic molecule-pair junctions.

Tao Ma1, Jing Guo, Shuai Chang

  • 1The State Key Laboratory of Refractories and Metallurgy, School of Chemistry and Chemical Engineering, School of Materials and Metallurgy, Wuhan University of Science and Technology, Wuhan, 430081, China. schang23@wust.edu.cn feng.liang@whu.edu.cn.

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Monitoring dynamic intermolecular interactions at the single-molecule level is challenging. This study uses a plasmonic nanocavity to observe hydrogen bond formation and modulation in carboxyl interfaces with millisecond resolution.

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Area of Science:

  • Physical Chemistry
  • Nanotechnology
  • Spectroscopy

Background:

  • Reversible intermolecular interactions are crucial in natural processes.
  • Monitoring these interactions at the single-molecule level in aqueous solutions remains difficult.
  • Carboxyl/carboxyl interfaces are fundamental in many biological and chemical systems.

Purpose of the Study:

  • To develop and demonstrate a method for monitoring dynamic intermolecular interactions at the single-molecule level.
  • To investigate the formation and modulation of hydrogen bonds at carboxyl interfaces.
  • To probe the influence of nanogap distance on intermolecular interactions.

Main Methods:

  • Utilizing a plasmonic nanocavity formed by a gold nanoparticle (GNP) and a gold nanoelectrode (GNE).
  • Employing time-resolved surface-enhanced Raman spectroscopy (TR-SERS) with tens of milliseconds time resolution.
  • Analyzing spectral fingerprints of carboxyl groups to identify non-specific interactions and hydrogen bonds.

Main Results:

  • Successfully monitored the dynamic changes of intermolecular interactions, including hydrogen bond formation, during single GNP collision events.
  • Identified distinct spectral signatures for non-specific interactions and hydrogen bonds at the carboxyl interface.
  • Demonstrated mechanical modulation of intermolecular interaction strength by tuning the applied bias on the GNE, altering nanogap distance.

Conclusions:

  • The study presents a novel approach to modulate and probe intermolecular interactions within nanogaps.
  • Intermolecular hydrogen bonds exhibit stochastic formation and are sensitive to nanogap distance modulation.
  • This technique offers a powerful tool for studying dynamic molecular interactions at the nanoscale.