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Time-resolved electronic sum-frequency generation spectroscopy with fluorescence suppression using optical Kerr

Caleb J C Jordan1, Jan R R Verlet1

  • 1Department of Chemistry, Durham University, Durham DH1 3LE, United Kingdom.

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|October 31, 2021
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Summary
This summary is machine-generated.

This study introduces optical Kerr gating to improve time-resolved electronic sum-frequency generation (SFG) spectroscopy. This method effectively suppresses fluorescence, enabling clearer observation of molecular dynamics at interfaces.

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Area of Science:

  • Chemical Physics
  • Spectroscopy
  • Surface Science

Background:

  • Studying excited state dynamics at interfaces is crucial for understanding chemical processes.
  • Time-resolved electronic sum-frequency generation (SFG) is a powerful technique for this purpose.
  • Fluorescence often interferes with SFG signals, limiting measurement accuracy.

Purpose of the Study:

  • To overcome the limitation of fluorescence interference in SFG measurements.
  • To develop a method for enhancing signal discrimination in time-resolved SFG.
  • To demonstrate the applicability of the new technique to interfacial molecular dynamics.

Main Methods:

  • Utilized optical Kerr gating to selectively filter the SFG signal.
  • Applied time-resolved electronic sum-frequency generation (SFG) spectroscopy.
  • Investigated molecular dynamics at the water/air interface.

Main Results:

  • Successfully discriminated SFG signals from overwhelming fluorescence.
  • Demonstrated the technique's effectiveness on malachite green excited state dynamics.
  • Showcased its utility in studying phenolate anion photo-oxidation at interfaces.

Conclusions:

  • Optical Kerr gating is a viable method to suppress fluorescence in SFG measurements.
  • This technique significantly enhances the study of excited state dynamics at interfaces.
  • The approach holds broad applicability for various interfacial phenomena.