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Time-Resolved X-ray Photoelectron Spectroscopy: Ultrafast Dynamics in CS(2) Probed at the S 2p Edge
[Image: see text] 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 TRX...
Autores principales: | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2023
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10431593/ https://www.ncbi.nlm.nih.gov/pubmed/37534743 http://dx.doi.org/10.1021/acs.jpclett.3c01447 |
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author | Gabalski, Ian Allum, Felix Seidu, Issaka Britton, Mathew Brenner, Günter Bromberger, Hubertus Brouard, Mark Bucksbaum, Philip H. Burt, Michael Cryan, James P. Driver, Taran Ekanayake, Nagitha Erk, Benjamin Garg, Diksha Gougoula, Eva Heathcote, David Hockett, Paul Holland, David M. P. Howard, Andrew J. Kumar, Sonu Lee, Jason W. L. Li, Siqi McManus, Joseph Mikosch, Jochen Milesevic, Dennis Minns, Russell S. Neville, Simon Atia-Tul-Noor Papadopoulou, Christina C. Passow, Christopher Razmus, Weronika O. Röder, Anja Rouzée, Arnaud Simao, Alcides Unwin, James Vallance, Claire Walmsley, Tiffany Wang, Jun Rolles, Daniel Stolow, Albert Schuurman, Michael S. Forbes, Ruaridh |
author_facet | Gabalski, Ian Allum, Felix Seidu, Issaka Britton, Mathew Brenner, Günter Bromberger, Hubertus Brouard, Mark Bucksbaum, Philip H. Burt, Michael Cryan, James P. Driver, Taran Ekanayake, Nagitha Erk, Benjamin Garg, Diksha Gougoula, Eva Heathcote, David Hockett, Paul Holland, David M. P. Howard, Andrew J. Kumar, Sonu Lee, Jason W. L. Li, Siqi McManus, Joseph Mikosch, Jochen Milesevic, Dennis Minns, Russell S. Neville, Simon Atia-Tul-Noor Papadopoulou, Christina C. Passow, Christopher Razmus, Weronika O. Röder, Anja Rouzée, Arnaud Simao, Alcides Unwin, James Vallance, Claire Walmsley, Tiffany Wang, Jun Rolles, Daniel Stolow, Albert Schuurman, Michael S. Forbes, Ruaridh |
author_sort | Gabalski, Ian |
collection | PubMed |
description | [Image: see text] 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 CS(2), 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. |
format | Online Article Text |
id | pubmed-10431593 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-104315932023-08-17 Time-Resolved X-ray Photoelectron Spectroscopy: Ultrafast Dynamics in CS(2) Probed at the S 2p Edge Gabalski, Ian Allum, Felix Seidu, Issaka Britton, Mathew Brenner, Günter Bromberger, Hubertus Brouard, Mark Bucksbaum, Philip H. Burt, Michael Cryan, James P. Driver, Taran Ekanayake, Nagitha Erk, Benjamin Garg, Diksha Gougoula, Eva Heathcote, David Hockett, Paul Holland, David M. P. Howard, Andrew J. Kumar, Sonu Lee, Jason W. L. Li, Siqi McManus, Joseph Mikosch, Jochen Milesevic, Dennis Minns, Russell S. Neville, Simon Atia-Tul-Noor Papadopoulou, Christina C. Passow, Christopher Razmus, Weronika O. Röder, Anja Rouzée, Arnaud Simao, Alcides Unwin, James Vallance, Claire Walmsley, Tiffany Wang, Jun Rolles, Daniel Stolow, Albert Schuurman, Michael S. Forbes, Ruaridh J Phys Chem Lett [Image: see text] 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 CS(2), 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. American Chemical Society 2023-08-03 /pmc/articles/PMC10431593/ /pubmed/37534743 http://dx.doi.org/10.1021/acs.jpclett.3c01447 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by-nc-nd/4.0/Permits non-commercial access and re-use, provided that author attribution and integrity are maintained; but does not permit creation of adaptations or other derivative works (https://creativecommons.org/licenses/by-nc-nd/4.0/). |
spellingShingle | Gabalski, Ian Allum, Felix Seidu, Issaka Britton, Mathew Brenner, Günter Bromberger, Hubertus Brouard, Mark Bucksbaum, Philip H. Burt, Michael Cryan, James P. Driver, Taran Ekanayake, Nagitha Erk, Benjamin Garg, Diksha Gougoula, Eva Heathcote, David Hockett, Paul Holland, David M. P. Howard, Andrew J. Kumar, Sonu Lee, Jason W. L. Li, Siqi McManus, Joseph Mikosch, Jochen Milesevic, Dennis Minns, Russell S. Neville, Simon Atia-Tul-Noor Papadopoulou, Christina C. Passow, Christopher Razmus, Weronika O. Röder, Anja Rouzée, Arnaud Simao, Alcides Unwin, James Vallance, Claire Walmsley, Tiffany Wang, Jun Rolles, Daniel Stolow, Albert Schuurman, Michael S. Forbes, Ruaridh Time-Resolved X-ray Photoelectron Spectroscopy: Ultrafast Dynamics in CS(2) Probed at the S 2p Edge |
title | Time-Resolved
X-ray Photoelectron Spectroscopy:
Ultrafast Dynamics in CS(2) Probed at the S 2p Edge |
title_full | Time-Resolved
X-ray Photoelectron Spectroscopy:
Ultrafast Dynamics in CS(2) Probed at the S 2p Edge |
title_fullStr | Time-Resolved
X-ray Photoelectron Spectroscopy:
Ultrafast Dynamics in CS(2) Probed at the S 2p Edge |
title_full_unstemmed | Time-Resolved
X-ray Photoelectron Spectroscopy:
Ultrafast Dynamics in CS(2) Probed at the S 2p Edge |
title_short | Time-Resolved
X-ray Photoelectron Spectroscopy:
Ultrafast Dynamics in CS(2) Probed at the S 2p Edge |
title_sort | time-resolved
x-ray photoelectron spectroscopy:
ultrafast dynamics in cs(2) probed at the s 2p edge |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10431593/ https://www.ncbi.nlm.nih.gov/pubmed/37534743 http://dx.doi.org/10.1021/acs.jpclett.3c01447 |
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