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

In this paper, we report on spectral intensity and group delay measurements of the highest-occupied molecular-orbital (HOMO) recombination dipole moment of $${\mathrm{N}}_{2}$$ in the molecular-frame using high harmonic spectroscopy. We take advantage of the long-wavelength $$1.3\text{ }\text{ }{\mu}\mathrm{m}$$ driving laser to isolate the HOMO in the near threshold region, 19–67 eV. Finally, 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.
 [1] ;  [1] ;  [2] ;  [3] ;  [1] ;  [1]
  1. The Ohio State Univ., Columbus, OH (United States). Dept. of Physics
  2. Alternative Energies and Atomic Energy Commission (CEA), Saclay (France). Interactions, Dynamics and Lasers Lab. (LIDYL)
  3. Texas A & M Univ., College Station, TX (United States). Dept. of Chemistry
Publication Date:
Grant/Contract Number:
FG02-04ER15614; FG02-06ER15833; 5460
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 118; Journal Issue: 3; Journal ID: ISSN 0031-9007
American Physical Society (APS)
Research Org:
The Ohio State Univ., Columbus, OH (United States); Alternative Energies and Atomic Energy Commission (CEA), Saclay (France)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Center for Scientific Research (CNRS) International Project of Scientific Cooperation (PICS) (France)
Country of Publication:
United States
74 ATOMIC AND MOLECULAR PHYSICS; electronic structure of atoms & molecules; high-order harmonic generation
OSTI Identifier:
Alternate Identifier(s):
OSTI ID: 1341314