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Area of Science:

  • Surface Science
  • Chemical Physics
  • Nanophotonics

Background:

  • Understanding single-molecule chemical dynamics is crucial for catalysis.
  • Ensemble measurements obscure individual molecular pathways.

Purpose of the Study:

  • To develop a method for tracking single-molecule chemical dynamics.
  • To investigate deprotonation and binding dynamics of surface ligands.
  • To explore optical manipulation of reaction pathways.

Main Methods:

  • Cascaded nano-optics approach with laser-induced atomic protrusions in plasmonic nanojunctions.
  • High-speed field-enhanced vibrational spectroscopy.
  • Theoretical calculations.

Main Results:

  • Direct tracking of chemical trajectories of single surface-bound molecules.
  • Observation of single-molecule deprotonation and binding dynamics under ambient conditions.
  • Monitoring chemical switching of a single carboxylic group between three states.
  • Identification of reversible proton transfer dynamics and molecule-metal coordination switching.

Conclusions:

  • The developed nano-optics approach enables direct observation of single-molecule interfacial mechanisms.
  • This method allows optical manipulation of reaction pathways.
  • Findings provide insights into catalysis and interfacial chemistry at the single-molecule level.