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Area of Science:

  • Quantum Chemistry
  • Spectroscopy
  • Computational Physics

Background:

  • Advanced computational methods are crucial for understanding molecular excited states.
  • Previous work established an L² method for valence photoionization cross-sections using Algebraic Diagrammatic Construction (ADC).

Purpose of the Study:

  • To extend the existing L² method for calculating excited-state core photoionization cross-sections.
  • To investigate the sensitivity of X-ray absorption spectra to molecular excited-state properties.

Main Methods:

  • Extension of an L² method based on Stieltjes imaging and Lanczos pseudo-spectrum.
  • Application of the Algebraic Diagrammatic Construction (ADC) method, specifically ADC(2)x.
  • Simulation of X-ray absorption spectra for molecular excited states.

Main Results:

  • Accurate reproduction of ground-state X-ray absorption spectra was achieved at the ADC(2)x level.
  • Calculated excited-state X-ray absorption spectra show sensitivity to geometric distortions (structural dynamics).
  • Spectra also reveal sensitivity to the electronic character (electronic dynamics) of the initial state.

Conclusions:

  • Core excitation spectroscopies are valuable probes for studying excited-state non-adiabatic dynamics.
  • The developed method can be combined with ab initio molecular dynamics for time-resolved spectroscopy simulations.
  • This approach offers a pathway to simulate molecular wavepacket dynamics in excited states.