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.
Department of Physics, The Ohio State University, Columbus, Ohio 43210, USA.
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Schoun
Department of Physics, The Ohio State University, Columbus, Ohio 43210, USA.
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Camper
LIDYL, CEA, CNRS, Université Paris-Saclay, CEA Saclay, 91191 Gif-Sur-Yvette, France.
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Salières
Department of Chemistry, Texas A&M University, College Station, Texas 77843, USA.
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Lucchese
Department of Physics, The Ohio State University, Columbus, Ohio 43210, USA.
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Agostini
Department of Physics, The Ohio State University, Columbus, Ohio 43210, USA.
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DiMauro