Strategies for single-laser-shot femtosecond pure-rotational CARS thermometry

We discuss recent experiments and modeling for the chirped-probe-pulse generation of single-laser-shot femtosecond pure-rotational CARS/CSRS spectra from room-temperature gases. A pure-rotational Raman coherence is impulsively generated using near-transform-limited femtosecond pump/Stokes excitation, and the coherence is probed by stretching a nominally 100-fs near-transform-limited probe beam to approximately 1.7 ps via the refractive-index dispersion in a 30-cm long flint-glass rod. The linearly chirped probe spectrum and phase beat against the time-dependent Raman polarization to generate complex spectra. Chirped-probe-pulse rotational CARS/CSRS offers an interesting alternative to hybrid fs/ps rotational CARS, in which a band-limited pulse of limited energy is used, because all of the available probe pulse energy can be retained in a chirped-probe-pulse experiment. Our early chirped-probe spectra are presented and the details of our initial model calculations are provided. The temperature sensitivity of the chirped-probe results is illustrated using calculated spectra.