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Probing the interplay between geometric and electronic-structure features via high-harmonic spectroscopy.

T T Gorman1, T D Scarborough1, P M Abanador2

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We measured recombination dipole matrix elements in CO2, N2O, and OCS molecules. OCS showed unique interference patterns, suggesting a combination of geometric and electronic structure effects.

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Area of Science:

  • Quantum Chemistry
  • Molecular Spectroscopy
  • Attosecond Science

Background:

  • The recombination dipole matrix element (RDME) governs electron recombination dynamics.
  • Understanding molecular structure influences electron behavior during recombination.
  • High-harmonic spectroscopy is a powerful tool for probing ultrafast molecular processes.

Purpose of the Study:

  • To measure molecular-frame RDMEs in CO2, N2O, and OCS.
  • To investigate the role of molecular geometry and electronic structure in RDME.
  • To identify interference phenomena affecting RDME in these molecules.

Main Methods:

  • High-harmonic spectroscopy was employed for molecular-frame measurements.
  • Measurements were conducted on aligned and unaligned molecular samples.
  • Ab initio calculations using time-dependent density functional theory were performed for comparison.

Main Results:

  • RDMEs in CO2, N2O, and OCS show two-center interference minima dependent on molecular alignment.
  • OCS exhibits anomalous phase shifts in its two-center minimum, differing from CO2 and N2O.
  • A Cooper-like electronic structure minimum, in addition to the geometric minimum, is proposed for OCS.

Conclusions:

  • The RDME in OCS is influenced by both geometric and electronic structure interferences.
  • An empirical model was developed to describe these combined interference effects.
  • Destructive interference in unaligned samples can reduce yields at high photon energies.