Femtosecond Pure-Rotational Coherent Anti-Stokes Raman Scattering Gas-Phase Diagnostics

We discuss recent experiments for the characterization of our femtosecond purerotational CARS facility for observation of Raman transients in N2 and atmospheric air. The construction of a simplified femtosecond four-wave mixing system with only a single laser source is presented. Pure-rotational Raman transients reveal well-ordered time-domain recurrence peaks associated with the near-uniform spacing of rotational Raman peaks in the spectral domain. Long-time, 100-ps duration observations of the transient Raman polarization are presented, and the observed transients are compared to simulated results. Fourier transformation of the transients reveals two distinct sets of beat frequencies. Simulation results for temperatures from 300-700 K are used to illustrate the temperature sensitivity of the time-domain transients and their Fourier-transform counterparts. And strategies for diagnostics are briefly discussed. These results are being utilized to develop gas-phase measurement strategies for temperature and species concentration.