Time-resolved vacuum-ultraviolet photoelectron spectroscopy of the A1Au state of acetylene
Ultrafast time-resolved photoelectron spectra are reported for the vacuum-ultraviolet (VUV) photoionization of acetylene following excitation to the Ã1Au state via UV absorption at 200 nm. The excitation energy lies above the lowest dissociation threshold to C2H X̃2Σ+ + H, as well as above the threshold for adiabatic dissociation of the Ã1Au state to form C2H (Ã2Π) + H. The time-dependent mass spectra and photoelectron spectra provide insight into the intramolecular decay processes of the Ã1Au state. In addition, photoelectron spectra of the Ã1Au state with VUV light access both the X̃2Πu and Ã2Σg+ states of the ion, as well as the predicted, but previously unobserved, 1 2Πg state, which corresponds to a two-hole, one-particle configuration that lies in close proximity to the Ã2Σg+ state. The 1 2Πg state is split into 2A2 + 2B2 and 2Ag + 2Bg states in the cis and trans configurations, respectively. Electronic structure calculations, along with trajectory calculations, reproduce the principal features of the experimental data and confirm the assignment of the 1 2Πg state.
Authors
- Oksana Plekan (ORCID: https://orcid.org/0000-0002-4692-7018)
- Antonio Prlj (ORCID: https://orcid.org/0000-0002-5589-9776)
- Carlo Spezzani (ORCID: https://orcid.org/0000-0001-5364-9047)
- Tomislav Piteša (ORCID: https://orcid.org/0000-0002-9322-3603)
- Michele Di Fraia (ORCID: https://orcid.org/0000-0001-8102-0799)
- Primož Rebernik Ribič (ORCID: https://orcid.org/0000-0002-5555-601X)
- Marco Zangrando (ORCID: https://orcid.org/0000-0001-8860-3962)
- Piero Decleva (ORCID: https://orcid.org/0000-0002-7322-887X)
- Emily M. Warne (ORCID: https://orcid.org/0000-0002-1205-6939)
- M. Danailov (ORCID: https://orcid.org/0000-0002-1888-1331)
- Michele Devetta (ORCID: https://orcid.org/0000-0002-3806-3475)
- Richard J. Squibb (ORCID: https://orcid.org/0000-0001-6708-8631)
- C. Vozzi (ORCID: https://orcid.org/0000-0002-0212-0191)
- L. Giannessi (ORCID: https://orcid.org/0000-0002-7643-9840)
- Weronika O. Razmus
- G. De Ninno (ORCID: https://orcid.org/0000-0002-4648-4413)
- Russell S. Minns (ORCID: https://orcid.org/0000-0001-6775-2977)
- Nađa Došlić (ORCID: https://orcid.org/0000-0001-6535-9020)
- D.M.P. Holland (ORCID: https://orcid.org/0000-0003-1351-605X)
- Katharine L. Reid (ORCID: https://orcid.org/0000-0002-5480-9708)
- Lorenzo Raimondi (ORCID: https://orcid.org/0000-0001-5115-2934)
- Kevin C. Prince (ORCID: https://orcid.org/0000-0002-5416-7354)
- Davide Faccialà (ORCID: https://orcid.org/0000-0002-5072-0394)
- M. Bonanomi (ORCID: https://orcid.org/0000-0003-3629-6264)
- R. Feifel (ORCID: https://orcid.org/0000-0001-5234-3935)
- S. T. Pratt (ORCID: https://orcid.org/0000-0002-8282-1026)
- Nathan A. Seifert (ORCID: https://orcid.org/0000-0002-3039-0578)
- Alexander Demidovich (ORCID: https://orcid.org/0000-0003-2355-2257)
- Carlo Callegari (ORCID: https://orcid.org/0000-0001-5491-7752)
- Ivan Powis (ORCID: https://orcid.org/0000-0002-7941-9079)
- J. Thompson (ORCID: https://orcid.org/0000-0003-2720-2692)
Institutions
- Argonne National Laboratory (US)
- University of Nottingham (GB)
- University of Trieste (IT)
- University of Nova Gorica (SI)
- Daresbury Laboratory (GB)
- Elettra-Sincrotrone Trieste S.C.p.A. (IT)
- University of New Haven (US)
- Ruđer Bošković Institute (HR)
- Istituto di Fotonica e Nanotecnologie (IT)
- Istituto Nazionale di Fisica Nucleare, Laboratori Nazionali di Frascati (IT)
- University of Southampton (GB)
- University of Gothenburg (SE)
- Politecnico di Milano (IT)
Publication Details
- Journal
- The Journal of Chemical Physics
- Published
- 2025-02-05
- DOI
- https://doi.org/10.1063/5.0241392
- Primary Topic
- Advanced Chemical Physics Studies
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- U.S. Department of Energy
- University of Chicago
- Leverhulme Trust
- University of Southampton
- Knut och Alice Wallenbergs Stiftelse
- Vetenskapsrådet
- Hrvatska Zaklada za Znanost
- Office of Science
- Engineering and Physical Sciences Research Council
- Science and Technology Facilities Council
- Basic Energy Sciences
- Chemical Sciences, Geosciences, and Biosciences Division
- Central Laser Facility, Science and Technology Facilities Council
- Argonne National Laboratory