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Strong field transient grating spectroscopy has shown to be a very versatiletool in time-resolved molecular spectroscopy. Here we use this technique toinvestigate the high-order harmonic generation from SF6 molecules vibrationallyexcited by impulsive stimulated Raman scattering. Transient gratingspectroscopy enables us to reveal clear modulations of the harmonic emission.This heterodyne detection shows that the harmonic emission generated between 14to 26 eV is mainly sensitive to two among the three active Raman modes in SF6,i.e. the strongest and fully symmetric nu 1-A1g mode (774 cm-1, 43 fs) and theslowest mode nu5-T2g (524 cm-1, 63 fs). A time-frequency analysis of theharmonic emission reveals additional dynamics: the strength and centralfrequency of the nu 1 mode oscillate with a frequency of 52 cm-1 (640 fs). Thiscould be a signature of the vibration of dimers in the generating medium.Harmonic 11 shows a remarkable behavior, oscillating in opposite phase, both onthe fast (774 cm-1) and slow (52 cm-1) timescales, which indicates a strongmodulation of the recombination matrix element as a function of the nucleargeometry. These results demonstrate that the high sensitivity of high-orderharmonic generation to molecularvibrations, associated to the high sensitivityof transient grating spectroscopy, make their combination a unique tool toprobe vibrational dynamics.

Transient grating spectroscopy of SF6 molecular vibrations