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A Multimodal Wide-Field Fourier-Transform Raman Microscope
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Validating free spectral range tracking as a robust method for mitigating artifacts in VSC kinetics.

Kaihao Gu1, Xinmin Zhao1, Runling Peng1

  • 1Terahertz Technology Innovation Research Institute, Terahertz Spectrum and Imaging Technology Cooperative Innovation Center, Shanghai Key Lab of Modern Optical System, School of Optical-Electrical and Computer Engineering, University of Shanghai for Science and Technology Shanghai 200093 China fzhang@usst.edu.cn.

RSC Advances
|May 21, 2026
PubMed
Summary
This summary is machine-generated.

Vibrational strong coupling (VSC) can alter chemical reactions. This study shows that monitoring cavity changes via free spectral range variations (ΔFSR) provides more accurate kinetic data than single-mode frequency shifts (Δf) for VSC-controlled chemistry.

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Area of Science:

  • Chemistry
  • Physical Chemistry
  • Chemical Kinetics

Background:

  • Vibrational strong coupling (VSC) is a phenomenon where light and molecular vibrations interact intensely within an optical cavity.
  • VSC has shown potential in modifying ground-state chemical reactivity.
  • Accurate kinetic analysis of VSC-controlled reactions relies on appropriate spectroscopic observables.

Purpose of the Study:

  • To systematically compare two common spectroscopic methods for monitoring VSC-modulated reactions: single-mode frequency shifts (Δf) and free spectral range variations (ΔFSR).
  • To evaluate the quantitative reliability of these methods for extracting rate constants in cavity-controlled chemistry.
  • To identify the most robust observable for kinetic studies under VSC conditions.

Main Methods:

  • A benchmark reaction, the deprotection of 1-phenyl-2-trimethylsilylacetylene (PTA), was studied under VSC conditions within a Fabry-Pérot cavity.
  • Reaction kinetics were monitored in real-time using both Δf and ΔFSR cavity readout strategies.
  • Rate constants were extracted using a normalized first-order kinetic formalism.

Main Results:

  • Single-mode frequency shifts (Δf) were found to be sensitive to thermal drift and global cavity perturbations, causing deviations in extracted rate constants (even with ΔT = 1 K).
  • ΔFSR-based analysis revealed a reaction rate suppression factor of approximately 5.1 under VSC conditions compared to the non-cavity case.
  • Δf-based analysis reported a lower suppression factor of only ~4.25, highlighting its susceptibility to non-reactive influences.

Conclusions:

  • Differential cavity observables, specifically ΔFSR, offer improved quantitative reliability for kinetic analysis in VSC-controlled chemical reactions.
  • Single-mode observables (Δf) are prone to systematic errors from environmental factors, impacting kinetic interpretations.
  • Rigorous methodological validation is crucial for advancing the field of cavity-controlled chemistry and accurately quantifying VSC effects.