Monitoring molecular dynamics using coherent electrons from high harmonic generation

We report a previously undescribed spectroscopic probe that makes use of electrons rescattered during the process of high-order harmonic generation. We excite coherent vibrations in SF(6) using impulsive stimulated Raman scattering with a short laser pulse. A second, more intense laser pulse generates high-order harmonics of the fundamental laser, at wavelengths of approximately 20-50 nm. The high-order harmonic yield is observed to oscillate,...