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

Chen, Timothy Y.; Liu, Ning; Kliewer, Christopher J.; Dogariu, Arthur; Kolemen, Egemen; Ju, Yiguang

doi:10.1364/ol.453272

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

Journal Article · Thu Mar 03 23:00:00 EST 2022 · Optics Letters

DOI:https://doi.org/10.1364/ol.453272· OSTI ID:1889111

^[1]; Liu, Ning ^[1]; ^[2]; Dogariu, Arthur ^[1]; ^[3]; Ju, Yiguang ^[1]

Princeton University, NJ (United States)
Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Princeton University, NJ (United States); Princeton Plasma Physics Lab. (PPPL), Princeton, NJ (United States)

Here, 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 thermalization in low-temperature plasmas as well as thermal loading of hypersonic vehicles. This approach uses time-domain interferences between ground state and vibrationally excited N₂ 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 N₂ 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 beat frequencies via Fourier transform of the time-domain response and obtained excellent agreement with the model.

View Accepted Manuscript (DOE)

Research Organization:: Princeton Plasma Physics Laboratory (PPPL), Princeton, NJ (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: FE0026825; NA0003525; SC0020233

OSTI ID:: 1889111

Alternate ID(s):: OSTI ID: 1847447
OSTI ID: 1906159

Journal Information:: Optics Letters, Journal Name: Optics Letters Journal Issue: 6 Vol. 47; ISSN 0146-9592

Publisher:: Optical Society of America (OSA)Copyright Statement

Country of Publication:: United States

Language:: English

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