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Versatile CO2 Transformations into Complex Products: A One-pot Two-step Strategy

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Core-valence double ionization of carbon suboxide.

Emelie Olsson¹, Lucas M Cornetta², Veronica Daver Ideböhn¹

¹Department of Physics, University of Gothenburg, Origovägen 6B, 412 58, Gothenburg, Sweden.

Scientific Reports

|May 6, 2025

Summary

We measured core-valence double ionization spectra of carbon suboxide, finding significant differences from single ionization spectra. Advanced calculations including orbital overlap improved agreement, aiding spectral feature assignments and Auger decay analysis.

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Published on: February 20, 2020

Area of Science:

Atomic and Molecular Physics
Quantum Chemistry
Spectroscopy

Background:

Core-valence double ionization is a complex process involving simultaneous removal of electrons from core and valence shells.
Understanding these processes is crucial for interpreting complex molecular spectra and electronic structure.
Carbon suboxide (C2O2) presents a unique system for studying core-level electron dynamics due to its distinct carbon environments.

Purpose of the Study:

To measure and analyze the core-valence double ionization spectra of carbon suboxide.
To compare experimental spectra with theoretical calculations to understand the ionization dynamics.
To assign spectral features and investigate Auger decay mechanisms following core ionization.

Main Methods:

Experimental measurement of core-valence double ionization spectra using synchrotron radiation above the O 1s and C 1s edges.
Comparison of experimental spectra with theoretical electronic structure calculations using the sudden approximation.
Analysis of Auger decay spectra following core hole formation at different carbon atoms.

Main Results:

Core-valence double ionization spectra of carbon suboxide show significant deviations from single ionization spectra.
Theoretical calculations incorporating core-valence orbital overlap improve agreement with experimental data.
Auger decay following C 1s ionization exhibits selectivity in final multiply charged states, dependent on the initial ionization site.

Conclusions:

A more complex theoretical description, including orbital overlap, is necessary for accurate modeling of core-valence double ionization in carbon suboxide.
Spectral features can be assigned by comparing experimental and calculated spectra.
Auger decay pathways are sensitive to the initial core ionization site, providing insights into molecular electronic structure.