Coherent anti-Stokes Raman scattering (CARS) is used to measure the amplitude, the dephasing lifetime, and parameters of optical nonlinearities of optical phonons in a synthetic diamond film. A compact CARS apparatus demonstrated in this work relies on the use of an unamplified 70 fs 340 mW Cr:forsterite laser output and photonic-crystal fibers optimized for the generation of wavelength-tunable Stokes field and the spectral compression of the probe pulse.

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We show that sequences of femtosecond laser pulses can control the rotational Raman response of a gas mixture, giving rise to a tunable manifold of echo recurrences in the retarded nonlinear-optical response of the gas. Tailored phase masks for high-intensity ultrashort laser pulses are experimentally demonstrated using molecular rotations in the gas phase driven by optimally time-ordered pulse sequences.