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Updated: Jun 8, 2026

Stimulated Stokes and Antistokes Raman Scattering in Microspherical Whispering Gallery Mode Resonators
Published on: April 4, 2016
Measurement method of nonresonant third-order susceptibility by using off-resonant coherent anti-Stokes Raman
This study measured nonresonant third-order susceptibilities (χ(nr)) in N(2) and Ar gases using a novel off-resonant coherent anti-Stokes Raman spectroscopy method. The technique offers advantages like simplified measurements and no need for precise Raman linewidth data.
Area of Science:
- Nonlinear Optics
- Spectroscopy
- Quantum Chemistry
Background:
- Nonresonant third-order susceptibilities (χ(nr)) are crucial for understanding nonlinear optical phenomena.
- Accurate measurement of χ(nr) in gases like N(2) and Ar is essential for various applications.
Purpose of the Study:
- To demonstrate a new method for measuring nonresonant third-order susceptibilities (χ(nr)) in gases.
- To validate the method by comparing experimental results with previous studies.
- To assess the impact of Raman linewidth uncertainties on the determined χ(nr) values.
Main Methods:
- Utilized off-resonant coherent anti-Stokes Raman spectroscopy (CARS) focusing on the N(2) Q branch.
- Theoretically calculated off-resonant spectra using a modified exponential gap model for Raman linewidth.
- Compared experimental and theoretical spectra to determine χ(nr).
Main Results:
- Measured χ(nr) for N(2) and Ar gases as 8.4 ± 0.2 and 9.7 ± 0.8 (× 10⁻¹⁸ cm³/erg/amagat), respectively.
- Obtained values are in good agreement with existing literature data.
- Investigated the effect of Raman linewidth variations, finding minimal impact (0.05% change in χ(nr) for a 50% change in linewidth).
Conclusions:
- The developed off-resonant CARS method is a viable technique for measuring gas susceptibilities.
- The method is robust against uncertainties in Raman linewidth data.
- Advantages include no requirement for high spectral resolution, accurate linewidth data, or optical delay between pump beams.
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