Precise Access to the Molecular-Frame Complex Recombination Dipole through High-Harmonic Spectroscopy

Abstract

We report on spectral intensity and group delay measurements of the highest-occupied molecular-orbital (HOMO) recombination dipole moment of N_{2} in the molecular-frame using high harmonic spectroscopy. We take advantage of the long-wavelength 1.3 μm driving laser to isolate the HOMO in the near threshold region, 19-67 eV. The precision of our group delay measurements reveals previously unseen angle-resolved spectral features associated with autoionizing resonances, and allows quantitative comparison with cutting-edge correlated 8-channel photoionization dipole moment calculations.