Femtosecond coherent anti-Stokes Raman scattering measurement of gas temperatures from frequency-spread dephasing of the Raman coherence

Gas-phase temperatures and concentrations are measured from the magnitude and decay of the initial Raman coherence in femtosecond coherent anti-Stokes Raman scattering (CARS). A time-delayed probe beam is scattered from the Raman polarization induced by pump and Stokes beams to generate CARS signal; the dephasing rate of this initial coherence is determined by the temperature-sensitive frequency spread of the Raman transitions. Temperature is measured from the CARS signal decrease with increasing probe delay. Concentration is found from the ratio of the CARS and nonresonant background signals. Collision rates do not affect the determination of these quantities.