Time-resolved pure-rotational coherent anti-Stokes Raman spectroscopy using picosecond-duration laser pulses is investigated for gas thermometry. The use of picosecond laser pulses significantly reduces background caused by scattering of the probe beam, and delayed probing of the Raman coherence enables elimination of interference from nonresonant four-wave mixing processes. Temperatures inferred from rotational spectra are sensitive to the probe delay because of the rotational-level dependence of collisional dephasing of Raman coherences. The sensitivity decreases, however, with increasing temperature, and accurate temperature measurements in a flame are demonstrated using a standard frequency-domain analysis of the spectra.
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