Time-resolved X-ray photoelectron spectroscopy: ultrafast dynamics in CS2 probed at the S 2p edge
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 we...
| Main Authors: | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
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| Format: | Journal article |
| Language: | English |
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American Chemical Society
2023
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| Subjects: |
| _version_ | 1797110939702525952 |
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| author | Gabalski, I Allum, F Seidu, I Britton, M Brenner, G Bromberger, H Brouard, M Bucksbaum, PH Burt, M Cryan, JP Driver, T Ekanayake, N Erk, B Garg, D Gougoula, E Heathcote, D Hockett, P Holland, DMP Howard, AJ Kumar, S Lee, JWL Li, S McManus, J Mikosch, J Milesevic, D Minns, RS Neville, S Atia-Tul-Noor Papadopoulou, CC Passow, C Razmus, WO Röder, A Rouzée, A Simao, A Unwin, J Vallance, C Walmsley, T Wang, J Rolles, D Stolow, A Schuurman, MS Forbes, R |
| author_facet | Gabalski, I Allum, F Seidu, I Britton, M Brenner, G Bromberger, H Brouard, M Bucksbaum, PH Burt, M Cryan, JP Driver, T Ekanayake, N Erk, B Garg, D Gougoula, E Heathcote, D Hockett, P Holland, DMP Howard, AJ Kumar, S Lee, JWL Li, S McManus, J Mikosch, J Milesevic, D Minns, RS Neville, S Atia-Tul-Noor Papadopoulou, CC Passow, C Razmus, WO Röder, A Rouzée, A Simao, A Unwin, J Vallance, C Walmsley, T Wang, J Rolles, D Stolow, A Schuurman, MS Forbes, R |
| author_sort | Gabalski, I |
| collection | OXFORD |
| description | 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<sub>2</sub>, 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 <i>ab initio</i> 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. |
| first_indexed | 2024-03-07T08:01:37Z |
| format | Journal article |
| id | oxford-uuid:2078ac37-b22c-459f-a347-2f7519055b7e |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-07T08:01:37Z |
| publishDate | 2023 |
| publisher | American Chemical Society |
| record_format | dspace |
| spelling | oxford-uuid:2078ac37-b22c-459f-a347-2f7519055b7e2023-10-04T17:37:31ZTime-resolved X-ray photoelectron spectroscopy: ultrafast dynamics in CS2 probed at the S 2p edgeJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:2078ac37-b22c-459f-a347-2f7519055b7ePhotodissociationDissociationSulfurIonizationUltrafast phenomenaEnglishSymplectic ElementsAmerican Chemical Society2023Gabalski, IAllum, FSeidu, IBritton, MBrenner, GBromberger, HBrouard, MBucksbaum, PHBurt, MCryan, JPDriver, TEkanayake, NErk, BGarg, DGougoula, EHeathcote, DHockett, PHolland, DMPHoward, AJKumar, SLee, JWLLi, SMcManus, JMikosch, JMilesevic, DMinns, RSNeville, SAtia-Tul-NoorPapadopoulou, CCPassow, CRazmus, WORöder, ARouzée, ASimao, AUnwin, JVallance, CWalmsley, TWang, JRolles, DStolow, ASchuurman, MSForbes, RRecent 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<sub>2</sub>, 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 <i>ab initio</i> 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. |
| spellingShingle | Photodissociation Dissociation Sulfur Ionization Ultrafast phenomena Gabalski, I Allum, F Seidu, I Britton, M Brenner, G Bromberger, H Brouard, M Bucksbaum, PH Burt, M Cryan, JP Driver, T Ekanayake, N Erk, B Garg, D Gougoula, E Heathcote, D Hockett, P Holland, DMP Howard, AJ Kumar, S Lee, JWL Li, S McManus, J Mikosch, J Milesevic, D Minns, RS Neville, S Atia-Tul-Noor Papadopoulou, CC Passow, C Razmus, WO Röder, A Rouzée, A Simao, A Unwin, J Vallance, C Walmsley, T Wang, J Rolles, D Stolow, A Schuurman, MS Forbes, R Time-resolved X-ray photoelectron spectroscopy: ultrafast dynamics in CS2 probed at the S 2p edge |
| title | Time-resolved X-ray photoelectron spectroscopy: ultrafast dynamics in CS2 probed at the S 2p edge |
| title_full | Time-resolved X-ray photoelectron spectroscopy: ultrafast dynamics in CS2 probed at the S 2p edge |
| title_fullStr | Time-resolved X-ray photoelectron spectroscopy: ultrafast dynamics in CS2 probed at the S 2p edge |
| title_full_unstemmed | Time-resolved X-ray photoelectron spectroscopy: ultrafast dynamics in CS2 probed at the S 2p edge |
| title_short | Time-resolved X-ray photoelectron spectroscopy: ultrafast dynamics in CS2 probed at the S 2p edge |
| title_sort | time resolved x ray photoelectron spectroscopy ultrafast dynamics in cs2 probed at the s 2p edge |
| topic | Photodissociation Dissociation Sulfur Ionization Ultrafast phenomena |
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