4.6 Article

Simultaneous single-shot rotation-vibration non-equilibrium thermometry using pure rotational fs/ps CARS coherence beating

Journal

OPTICS LETTERS
Volume 47, Issue 6, Pages 1351-1354

Publisher

OPTICAL SOC AMER
DOI: 10.1364/OL.453272

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Funding

  1. National Science Foundation [CBET 1903362]
  2. U.S. Department of Energy [DE-FE0026825, DE-NA0003525, DE-SC0020233]
  3. U.S. Department of Energy (DOE) [DE-SC0020233] Funding Source: U.S. Department of Energy (DOE)

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We report the development of a simple and sensitive two-beam hybrid femtosecond/picosecond pure rotational coherent anti-Stokes Raman scattering (fs/ps CARS) method to simultaneously measure the rotational and vibrational temperatures of diatomic molecules. This method utilizes coherence beating effects to infer the temperatures and a model for extraction. The experimental results are in good agreement with the model.
We report the development of a simple and sensitive two-beam hybrid femtosecond/picosecond pure rotational coherent anti-Stokes Raman scattering (fs/ps CARS) method to simultaneously measure the rotational and vibrational temperatures of diatomic molecules. Rotation-vibration non-equilibrium plays a key role in the chemistry and the rmalization in low-temperature plasmas as well as thermal loading of hypersonic vehicles. This approach uses time-domain interferences between ground state and vib rationally excited N-2 molecules to intentionally induce coherence beating that leads to apparent non-Boltzmann distributions in the pure rotational spectra. These distortions enable simultaneous inference of both the rotational and vibrational temperatures. Coherence beating effects were observed in single-shot fs/ps CARS measurements of a 75 Torr N-2 DC glow discharge and were successfully modeled for rotational and vibrational temperature extraction. We show that this method can be more sensitive than a pure rotational fs/ps CARS approach using a spectrally narrow probe pulse. Lastly, we experimentally measured the heat frequencies via Fourier transibrm of the time-domain response and obtained excellent agreement with the model. (C) 2022 Optica Publishing Group

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