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High-Resolution Photoelectron Spectroscopy of Cryogenically Cooled VO3H2.

Korina Vlahos1, Martin DeWitt1, Daniel M Neumark1

  • 1Department of Chemistry, University of California, Berkeley, California 94720, United States.

The Journal of Physical Chemistry. A
|April 6, 2026
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Summary

This study reports high-resolution photoelectron spectra of cryogenically cooled vanadium oxide hydride anions (VO3H2-). The research provides key insights into the electronic structure and vibrational frequencies of neutral VO(OH)2.

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Area of Science:

  • Physical Chemistry
  • Spectroscopy
  • Computational Chemistry

Background:

  • Vanadium oxide hydride anions (VO3H2-) are relevant in understanding metal-oxide-water interactions.
  • Previous studies on similar adducts like TiO3H2- highlight the importance of electronic structure.
  • Characterizing the electronic and vibrational properties of these anions is crucial for chemical insights.

Purpose of the Study:

  • To obtain high-resolution photoelectron spectra of cryogenically cooled VO3H2- anions.
  • To determine the electron affinity and vibrational frequencies of the neutral VO(OH)2 species.
  • To investigate the role of Herzberg-Teller coupling in the observed spectral features.

Main Methods:

  • Cryogenic Slow Electron Velocity-Map Imaging (cryo-SEVI) was employed to obtain photoelectron spectra.
  • Density Functional Theory (DFT) calculations were performed for theoretical comparison.
  • Franck-Condon (FC) simulations were used to analyze spectral transitions.

Main Results:

  • High-resolution spectra confirmed the formation of the cis-VO(OH)2- dissociative adduct.
  • The electron affinity of neutral VO(OH)2 was determined to be 1.857(1) eV.
  • Several vibrational frequencies for the neutral species were identified, with some attributed to FC-forbidden transitions via Herzberg-Teller coupling.

Conclusions:

  • The study successfully characterized the electronic and vibrational properties of VO3H2- and its neutral counterpart.
  • Herzberg-Teller coupling plays a significant role in the observed spectral complexity, involving nontotally symmetric vibrational modes.
  • Comparison with TiO3H2- adducts provides a foundation for exploring the impact of additional valence electrons in related systems.