Nonlinear optics experiments measuring phase shifts induced in a weak probe pulse by a strong pump pulse must account for coherent effects that only occur when the pump and probe pulses are temporally overlapped. It is well known that a weak probe beam experiences a greater phase shift from a strong pump beam than the pump beam induces on itself. The physical mechanism behind the enhanced phase shift is diffraction of pump light into the probe direction by a nonlinear refractive index grating produced by interference between the two beams. For an instantaneous third-order response, the effect of the grating is to simply double the probe phase shift, but when delayed nonlinearities are considered, the effect is more complex. A comprehensive treatment is given for both degenerate and nondegenerate pump-probe experiments in noble and diatomic gases. Results of numerical calculations are compared to a recent transient birefringence measurement [Loriot et al., Opt. Express 17, 13429 (2009)] and a recent spectral interferometry experiment [Wahlstrand et al., Phys. Rev. A 85, 043820 (2012)]. We also present results from two new experiments using spectrally-resolved transient birefringence with 800 nm pulses in Ar and air and degenerate chirped pulse spectral interferometry in Ar. Both experiments support the interpretation of the negative birefringence at high intensity as arising from a plasma grating. arXiv:1302.3208v2 [physics.optics]

We report experimental confirmation of the ionization-grating-induced transient birefringence predicted by Wahlstrand and Milchberg [Opt. Lett. 36, 3822 (2011)] and discuss its impact on the higher-order Kerr effect interpretation by Loriot et al. of pump-probe transient birefringence measurements made at 800 nm [Opt. Express 17, 13429 (2009)]. Measurement of the transient birefringence in air at 400 nm shows a negative contribution to the index of refraction at zero delay for frequencies within the pump bandwidth, the degenerate case, and no negative contribution for frequencies exceeding the pump bandwidth, the nondegenerate case. Our findings suggest that a reevaluation of the higher-order Kerr effect hypothesis of Loriot et al. is necessary.

Vibrational Raman spectroscopy is performed in the gas phase using a femtosecond laser pulse undergoing filamentation as an impulsive excitation source. The molecular coherence induced by the filamentary pulse is subsequently probed using a narrowband, sub-picosecond laser pulse to produce Raman spectra of gas phase species in a few tens of milliseconds (~10 laser shots). Pulse shortening with concomitant spectral broadening during filamentation results in a pulse that is both sufficiently short and of sufficient spectral power density to impulsively excite the highest energy ground state vibrations (up to 4158 cm(-1) corresponding to H(2)). Gas phase detection of chloroform, methylene chloride, cyclohexane, toluene, pentane, triethylamine, ammonia, nitromethane, and gasoline is performed.