We study high-order harmonic generation in excited media using a four-wave-mixing-like configuration. We analyze the spatial profile of high harmonics emitted by a grating of rotationally excited molecules as a function of the pump-probe delay. We demonstrate a dramatic improvement in the contrast of the diffracted signal relative to the total high harmonic signal. This allows us to observe subtle effects in the rotational wave packet excitation such as the pump-intensity dependence of the wave packet dynamics. High harmonic transient grating spectroscopy can be extended to all forms of molecular excitation and to weak resonant excitation.

• Received 11 May 2007

DOI:https://doi.org/10.1103/PhysRevLett.100.143903