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

Physical review letters

PubMedID: 28157344

Schoun SB, Camper A, Salières P, Lucchese RR, Agostini P, Dimauro LF. Precise Access to the Molecular-Frame Complex Recombination Dipole through High-Harmonic Spectroscopy. Phys Rev Lett. 2017;118(3):033201.
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.