Time-domain measurements of S-branch N-2-N-2 Raman linewidths using picosecond pure rotational coherent anti-Stokes Raman spectroscopy

• Time-resolved dual-broadband picosecond pure rotational CARS has been applied to measure self-broadened S-branch N-2-N-2 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 N-2-N-2 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 N-2 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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NATURVETENSKAP  -- Fysik -- Atom- och molekylfysik och optik (hsv//swe)

NATURAL SCIENCES  -- Physical Sciences -- Atom and Molecular Physics and Optics (hsv//eng)

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