High-harmonic and terahertz wave spectroscopy (HATS) for aligned molecules

We present the experimental and theoretical details of our recent published letter Huang et al (2015 Phys. Rev. Lett. 115 123002) on synchronized high-harmonic and terahertz-wave spectroscopy (HATS) from nonadiabatically aligned nitrogen molecules in dual-color laser fields. By associating alignment-angle dependent terahertz wave generation (TWG) with high harmonic generation (HHG), the angular differential photoionization cross section (PICS) for molecules can be reconstructed. The angles at which the PICS's minima are located show great convergence between the theoretical predictions and the experimentally deduced results when choosing a suitable internuclear distance. We also show the optimal relative phase between the dual-color laser fields for TWG does not change with the alignment angle at a precision of about 50 attoseconds. This all-optical method provides an alternative for investigating molecular structures and dynamics.