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Time-domain measurements of S-branch N2–N2 Raman linewidths using picosecond pure rotational coherent anti-Stokes Raman spectroscopy

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Abstract

Time-resolved dual-broadband picosecond pure rotational CARS has been applied to measure self-broadened S-branch N2–N2 Raman linewidths in the temperature range 294–1466 K. The coherence decays were detected directly in the time domain by following the J-dependent CARS signal decay as a function of probe delay. The rotational Raman N2–N2 linewidths were derived from these time-dependent decays and evaluated for thermometric accuracy. Comparisons were made to the energy-corrected sudden (ECS) and modified exponential gap (MEG) dynamical scaling laws, and the results were used to quantify the sensitivity of nanosecond rotational CARS thermometry to the linewidth model employed. The uncertainty based on the linewidth model used in pure N2 was found to be 2 %. The merits and limitations of this rapid method for the determination of accurate Raman linewidths are discussed.

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Acknowledgements

Funding provided by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-AC04-94AL85000. PEB, AB, and EN acknowledge the financial support of the Swedish Energy Agency and the Centre of Combustion Science and Technology (CECOST).

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Authors and Affiliations

  1. Combustion Research Facility, Sandia National Laboratory, PO Box 969 MS 9055, Livermore, CA, 94551, USA

    C. J. Kliewer, B. D. Patterson & T. B. Settersten

  2. Division of Combustion Physics, Lund University, P.O. Box 118, 221 00, Lund, Sweden

    A. Bohlin, E. Nordström & P.-E. Bengtsson

Authors
  1. C. J. Kliewer
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  2. A. Bohlin
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  3. E. Nordström
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  4. B. D. Patterson
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  5. P.-E. Bengtsson
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  6. T. B. Settersten
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Correspondence to C. J. Kliewer.

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Kliewer, C.J., Bohlin, A., Nordström, E. et al. Time-domain measurements of S-branch N2–N2 Raman linewidths using picosecond pure rotational coherent anti-Stokes Raman spectroscopy. Appl. Phys. B 108, 419–426 (2012). https://doi.org/10.1007/s00340-012-5037-2

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  • DOI: https://doi.org/10.1007/s00340-012-5037-2

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