Time-domain modelling and thermometry of the CH4v1 Q-branch using hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering
Abstract
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 exchangingmore »
- Authors:
-
- 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)
- Publication Date:
- Research Org.:
- Princeton Univ., NJ (United States); Princeton Plasma Physics Laboratory (PPPL), Princeton, NJ (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF)
- OSTI Identifier:
- 1906179
- Alternate Identifier(s):
- OSTI ID: 1775650; OSTI ID: 1810632
- Grant/Contract Number:
- SC0020233; SC0014664; NA0003525; FE0026825; CBET-1903362; CBET-2029425
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Combustion and Flame
- Additional Journal Information:
- Journal Volume: 224; Journal ID: ISSN 0010-2180
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 70 PLASMA PHYSICS AND FUSION TECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; laser diagnostics; coherent anti-Stokes raman scattering; thermometry; femtosecond/picosecond CARS; methane; ultrafast spectroscopy
Citation Formats
Chen, Timothy Y., Kliewer, Christopher J., Goldberg, Benjamin M., Kolemen, Egemen, and Ju, Yiguang. Time-domain modelling and thermometry of the CH4v1 Q-branch using hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering. United States: N. p., 2020.
Web. doi:10.1016/j.combustflame.2020.11.017.
Chen, Timothy Y., Kliewer, Christopher J., Goldberg, Benjamin M., Kolemen, Egemen, & Ju, Yiguang. Time-domain modelling and thermometry of the CH4v1 Q-branch using hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering. United States. https://doi.org/10.1016/j.combustflame.2020.11.017
Chen, Timothy Y., Kliewer, Christopher J., Goldberg, Benjamin M., Kolemen, Egemen, and Ju, Yiguang. Sat .
"Time-domain modelling and thermometry of the CH4v1 Q-branch using hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering". United States. https://doi.org/10.1016/j.combustflame.2020.11.017. https://www.osti.gov/servlets/purl/1906179.
@article{osti_1906179,
title = {Time-domain modelling and thermometry of the CH4v1 Q-branch using hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering},
author = {Chen, Timothy Y. and Kliewer, Christopher J. and Goldberg, Benjamin M. and Kolemen, Egemen and Ju, Yiguang},
abstractNote = {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.},
doi = {10.1016/j.combustflame.2020.11.017},
journal = {Combustion and Flame},
number = ,
volume = 224,
place = {United States},
year = {Sat Dec 05 00:00:00 EST 2020},
month = {Sat Dec 05 00:00:00 EST 2020}
}
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