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Measurement of Ultrafast Vibrational Coherences in Polyatomic Radical Cations with Strong-Field Adiabatic Ionization
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Application of the complex Kohn variational method to attosecond spectroscopy.

N Douguet1, B I Schneider2, L Argenti1

  • 1Department of Physics, University of Central Florida, Orlando, Florida 32186, USA.

Physical Review. A
|December 14, 2020
PubMed
Summary

We extended the complex Kohn variational method to study light-driven electronic transitions in atoms and molecules. This enables analysis of multiphoton ionization processes, advancing attosecond science for complex systems.

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Area of Science:

  • Atomic and Molecular Physics
  • Quantum Chemistry
  • Attosecond Science

Background:

  • Light-driven electronic transitions are crucial for understanding atomic and molecular dynamics.
  • Studying multiphoton processes requires advanced computational methods.
  • Existing methods have limitations in handling arbitrary light polarization and complex systems.

Purpose of the Study:

  • To extend the complex Kohn variational method for computing light-driven electronic transitions.
  • To enable the study of multiphoton processes in the perturbative regime for arbitrary light polarization.
  • To apply the method to analyze pump-probe two-photon ionization of helium.

Main Methods:

  • Extension of the complex Kohn variational method.
  • Computation of light-driven electronic transitions between continuum wave functions.
  • Application to pump-probe two-photon ionization of helium using extreme ultraviolet and infrared pulses.
  • Comparison with atomic B-spline close-coupling STOCK code simulations.

Main Results:

  • Successfully computed photoelectron spectra for two-photon ionization of helium.
  • Demonstrated good agreement between the extended complex Kohn variational method and the STOCK code.
  • Validated the finite-pulse perturbative approach for analyzing resonant multiphoton ionization.

Conclusions:

  • The extended complex Kohn variational method is a viable tool for studying light-driven electronic transitions.
  • This approach facilitates the *ab initio* study of weak-field attosecond processes.
  • It paves the way for investigating complex polyelectronic molecules in strong laser fields.