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Open Access Publications from the University of California

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


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.

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