Information content of high harmonics generated from aligned molecules.

We derive an expression for the harmonic signal from nonadiabatically aligned molecules that accounts for both electronic and rotational motions. We identify a single approximation, which converts the expression into a physically transparent and computationally convenient form. Our analytical result gives explicitly the time dependence of the harmonic spectra, thus explaining the observations of a class of recent experiments. Moreover, it points to new opportunities for generating insights into the structure and dynamics of molecular systems through harmonic generation experiments from aligned molecules. This includes information regarding the rotational and electronic dynamics of isolated systems, as well as regarding the decoherence and relaxation in molecules subject to a dissipative environment.