Axis-dependence of molecular high harmonic emission in three dimensions.

High-order harmonic generation in an atomic or molecular gas is a promising source of sub-femtosecond vacuum ultraviolet coherent radiation for transient scattering, absorption, metrology and imaging applications. High harmonic spectra are sensitive to Ångstrom-scale structure and motion of laser-driven molecules, but interference from radiation produced by random molecular orientations obscures this in all but the simplest cases, such as linear molecules. Here we show how to extract full body-frame high harmonic generation information for molecules with more complicated geometries by utilizing the methods of coherent transient rotational spectroscopy. To demonstrate this approach, we obtain the relative strength of harmonic emission along the three principal axes in the asymmetric-top sulphur dioxide. This greatly simplifies the analysis task of high harmonic spectroscopy and extends its usefulness to more complex molecules.