Phase sensitivity of high harmonic transient grating spectroscopy

We study the spatial profile of high order harmonics generated by a transient grating of rotational excitation. We show that the phase modulation of the harmonic emission as a function of molecular alignment is encoded in the diffraction pattern. In molecular nitrogen, the phase difference between aligned and isotropic molecules decreases from 1.6 rad for harmonic 19 to less than 0.3 rad for harmonic 27. In CO2 we observe a strong phase jump for the highest harmonics. The position of this phase jump in the harmonic spectrum depends on the laser intensity, reflecting the contribution from multiple molecular orbitals to the harmonic emission. (Some figures in this article are in colour only in the electronic version)