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Fano-ADC(2,2) method for electronic decay rates.

P Kolorenč1, V Averbukh2

  • 1Charles University, Faculty of Mathematics and Physics, Institute of Theoretical Physics, V Holešovičkách 2, 180 00 Prague, Czech Republic.

The Journal of Chemical Physics
|June 8, 2020
PubMed
Summary

The new Fano-ADC(2,2) method accurately predicts electronic decay widths in excited systems. This advancement enables the study of complex decay processes like double Auger decay (DAD), previously inaccessible.

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Area of Science:

  • Quantum Chemistry
  • Theoretical Chemistry
  • Atomic and Molecular Physics

Background:

  • Fano-ADC methods predict electronic decay widths in excited atomic and molecular systems.
  • Current Fano-ADC schemes have limitations in treating initial and final states, restricting accuracy and applicability to first-order decay processes.
  • Unbalanced correlation treatment compromises numerical accuracy in existing Fano-ADC methods.

Purpose of the Study:

  • To introduce an improved Fano-ADC approximation, ADC(2,2), for enhanced accuracy in predicting electronic decay widths.
  • To extend the applicability of Fano-ADC methods to second-order decay processes, including double Auger decay (DAD).
  • To address the limitations of unbalanced correlation treatments in previous Fano-ADC schemes.

Main Methods:

  • Development of the ADC(2,2) approximation for singly ionized states, treating both initial and final states to second order.
  • Construction of the Fano-ADC(2,2) approximation for decay width calculations.
  • Application of the Fano-ADC(2,2) method to a series of decay processes.

Main Results:

  • The Fano-ADC(2,2) approximation demonstrates superior accuracy for predicting electronic decay widths.
  • The new scheme successfully calculates decay widths for processes previously beyond the scope of Fano-ADC.
  • Access to second-order decay processes, such as double Auger decay (DAD), is now enabled.

Conclusions:

  • The Fano-ADC(2,2) method represents a significant advancement in the ab initio prediction of electronic decay widths.
  • This improved method enhances numerical accuracy and expands the range of accessible decay phenomena.
  • Fano-ADC(2,2) is a powerful tool for studying complex electronic decay processes in ionized systems.