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| DOI | Resolve DOI: https://doi.org/10.1021/acs.jpclett.3c01447 |
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| Author | Search for: Gabalski, IanORCID identifier: https://orcid.org/0000-0002-6782-6566; Search for: Allum, FelixORCID identifier: https://orcid.org/0000-0002-8044-8969; Search for: Seidu, Issaka1; Search for: Britton, Mathew; Search for: Brenner, Günter; Search for: Bromberger, Hubertus; Search for: Brouard, MarkORCID identifier: https://orcid.org/0000-0003-3421-0850; Search for: Bucksbaum, Philip H.; Search for: Burt, MichaelORCID identifier: https://orcid.org/0000-0002-7317-8649; Search for: Cryan, James P.ORCID identifier: https://orcid.org/0000-0002-7776-0919; Search for: Driver, TaranORCID identifier: https://orcid.org/0000-0002-3761-6883; Search for: Ekanayake, Nagitha; Search for: Erk, BenjaminORCID identifier: https://orcid.org/0000-0001-8413-3588; Search for: Garg, Diksha; Search for: Gougoula, Eva; Search for: Heathcote, David; Search for: Hockett, Paul1; Search for: Holland, David M. P.; Search for: Howard, Andrew J.; Search for: Kumar, Sonu; Search for: Lee, Jason W. L.; Search for: Li, Siqi; Search for: McManus, JosephORCID identifier: https://orcid.org/0000-0002-7911-2042; Search for: Mikosch, Jochen; Search for: Milesevic, Dennis; Search for: Minns, Russell S.; Search for: Neville, Simon1ORCID identifier: https://orcid.org/0000-0001-8134-1883; Search for: Atia-Tul-Noor, Atia; Search for: Papadopoulou, Christina C.; Search for: Passow, Christopher; Search for: Razmus, Weronika O.; Search for: Röder, Anja; Search for: Rouzée, Arnaud; Search for: Simao, Alcides; Search for: Unwin, James; Search for: Vallance, ClaireORCID identifier: https://orcid.org/0000-0003-3880-8614; Search for: Walmsley, Tiffany; Search for: Wang, JunORCID identifier: https://orcid.org/0000-0003-1962-895X; Search for: Rolles, DanielORCID identifier: https://orcid.org/0000-0002-3965-3477; Search for: Stolow, Albert1ORCID identifier: https://orcid.org/0000-0002-8447-3678; Search for: Schuurman, Michael S.1ORCID identifier: https://orcid.org/0000-0002-0922-9034; Search for: Forbes, RuaridhORCID identifier: https://orcid.org/0000-0003-2097-5991 |
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| Affiliation | - National Research Council of Canada. Security and Disruptive Technologies
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| Funder | Search for: University of Southampton; Search for: U.S. Department of Defense; Search for: Division of Physics; Search for: Engineering and Physical Sciences Research Council; Search for: Leverhulme Trust; Search for: Helmholtz-Gemeinschaft; Search for: Basic Energy Sciences; Search for: Science and Technology Facilities Council; Search for: Max-Planck-Gesellschaft; Search for: H2020 Research Infrastructures; Search for: Jesus College, University of Oxford; Search for: Natural Sciences and Engineering Research Council of Canada; Search for: H2020 European Research Council; Search for: National Defense Science and Engineering Graduate; Search for: University of Ottawa-NRC Joint Centre for Extreme Photonics |
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| Format | Text, Article |
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| Subject | dissociation; ionization; photodissociation; sulfur; ultrafast phenomena |
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| Abstract | Recent developments in X-ray free-electron lasers have enabled a novel site-selective probe of coupled nuclear and electronic dynamics in photoexcited molecules, time-resolved X-ray photoelectron spectroscopy (TRXPS). We present results from a joint experimental and theoretical TRXPS study of the well-characterized ultraviolet photodissociation of CS₂, a prototypical system for understanding non-adiabatic dynamics. These results demonstrate that the sulfur 2p binding energy is sensitive to changes in the nuclear structure following photoexcitation, which ultimately leads to dissociation into CS and S photoproducts. We are able to assign the main X-ray spectroscopic features to the CS and S products via comparison to a first-principles determination of the TRXPS based on ab initio multiple-spawning simulations. Our results demonstrate the use of TRXPS as a local probe of complex ultrafast photodissociation dynamics involving multimodal vibrational coupling, nonradiative transitions between electronic states, and multiple final product channels. |
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| Publication date | 2023-08-03 |
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| Publisher | American Chemical Society |
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| Language | English |
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| Peer reviewed | Yes |
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| Export citation | Export as RIS |
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| Report a correction | Report a correction (opens in a new tab) |
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| Record identifier | 9b6345aa-8d54-4b34-aea4-92674949345a |
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| Record created | 2024-01-24 |
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| Record modified | 2024-02-02 |
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