Time-domain modelling and thermometry of the CH4v1 Q-branch using hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering

Chen, Timothy Y.; Kliewer, Christopher J.; Goldberg, Benjamin M.; Kolemen, Egemen; Ju, Yiguang

doi:10.1016/j.combustflame.2020.11.017

Title: Time-domain modelling and thermometry of the CH₄v₁ Q-branch using hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering

Journal Article · Sat Dec 05 00:00:00 EST 2020 · Combustion and Flame

DOI:https://doi.org/10.1016/j.combustflame.2020.11.017· OSTI ID:1906179

^[1];

^[2]; Goldberg, Benjamin M. ^[3];

^[4]; Ju, Yiguang ^[1]

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

Here, we present time-domain measurements and modelling of the CH₄v₁ vibrational Q-branch, as well as simultaneous temperature acquisition from the CH₄ and N₂ vibrational Q-branches using broadband hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS). Accurate measurements with fs/ps CARS require knowledge of the time-domain response of the probed molecule at different temperatures and pressures. In this work, a fs/ps CARS model was developed for theCH₄v₁ Q-branch and validated using time-resolved probe delay scans at pressures between 70 and 600 Torr and temperatures between 295 and 1000 K. A simplified modified exponential energy gap model was used to determine the linewidths of the Raman transitions within the Q-branch. Total Q-branch linewidths for the entire explored parameter space were also determined from the probe delay scans. This enabled quantitative measurements of CH₄ with fs/ps CARS as well as the temperature through the hot bands of the CH₄v₁ Q-branch. With a broadband fs laser pulse in a two-beam phase matching scheme, the N₂ Q-branch and CH₄v₁ Q-branch were simultaneously measured in a heated cell, and the temperatures from each molecule's spectra was evaluated. Here, the fitted temperatures corresponded well with differences ranging from 4 to 17%. It was also shown that exchanging 90% of CH₄ for N₂ or Ar at 295 K and 500 Torr did not significantly impact the normalized time-domain signal prior to a 100 picosecond probe delay. Spatially resolved one-dimensional (1-D) thermometry using the CH₄ Q-branch was also demonstrated with an imaged spatial resolution of 40 µm. With the developed model, 1-D quantitative measurements of CH₄ concentration and temperature can be measured with time resolution of tens of picoseconds.

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

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF)

Grant/Contract Number:: SC0020233; SC0014664; NA0003525; FE0026825; CBET-1903362; CBET-2029425

OSTI ID:: 1906179

Alternate ID(s):: OSTI ID: 1775650; OSTI ID: 1810632

Journal Information:: Combustion and Flame, Vol. 224; ISSN 0010-2180

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Time-domain modelling and thermometry of the CH4v1 Q-branch using hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering

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Title: Time-domain modelling and thermometry of the CH₄v₁ Q-branch using hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering