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Towards time resolved tip-enhanced Raman spectroscopy: TERS with chopped laser pulses.

Ana M Gómez-Marín1,2, Katrin F Domke1

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Summary

This study introduces mechanically chopped laser excitation for ambient tip-enhanced Raman (TER) spectroscopy, achieving millisecond time resolution. This method maintains spectral quality comparable to continuous wave excitation without system modifications.

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Area of Science:

  • Spectroscopy
  • Surface Science
  • Nanotechnology

Background:

  • Tip-enhanced Raman spectroscopy (TER) offers high spatial resolution for analyzing surfaces.
  • Current limitations in TER include a trade-off between temporal and spectral resolution, especially with pulsed lasers.
  • Achieving millisecond-scale temporal resolution in ambient TER is challenging.

Purpose of the Study:

  • To investigate the use of a mechanically chopped laser beam as an excitation source for ambient TER.
  • To enhance the time resolution of TER spectroscopy towards the millisecond timescale.
  • To assess the impact of chopped excitation on TER signal stability, sensitivity, and spectral quality.

Main Methods:

  • Utilized a mechanically chopped laser beam as the excitation source for ambient TER.
  • Analyzed a submonolayer of thiophenol adsorbed on an Au(111) surface.
  • Compared TER spectra obtained with chopped excitation versus continuous wave (cw) excitation.

Main Results:

  • TER spectra acquired with chopped excitation showed comparable stability, sensitivity, spectral resolution, and signal-to-noise ratio to cw excitation.
  • The chopped laser approach successfully overcame the spectral-temporal resolution trade-off associated with pulsed lasers.
  • Increased tolerance to higher pulsed laser power before sample degradation was observed.

Conclusions:

  • Mechanically chopped laser excitation is a viable method for ambient TER spectroscopy.
  • This technique enables millisecond temporal resolution while maintaining high spectral resolution and signal quality.
  • The methodology allows for ambient TER measurements with improved temporal resolution without altering the standard detection system.