X-ray induced Coulomb explosion imaging of transient excited-state structural rearrangements in CS2
Structural imaging of transient excited-state species is a key goal of molecular physics, promising to unveil rich information about the dynamics underpinning photochemical transformations. However, separating the electronic and nuclear contributions to the spectroscopic observables is challenging,...
| Main Authors: | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
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| Format: | Journal article |
| Language: | English |
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Springer Nature
2023
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| _version_ | 1797111560697544704 |
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| author | Unwin, J Allum, F Britton, M Gabalski, I Bromberger, H Brouard, M Bucksbaum, PH Driver, T Ekanayake, N Garg, D Gougoula, E Heathcote, D Howard, AJ Hockett, P Holland, DMP Kumar, S Lam, C-S Lee, JWL McManus, J Mikosch, J Milesevic, D Minns, RS Papadopoulou, CC Passow, C Razmus, WO Röder, A Rouzée, A Schuurman, M Simao, A Stolow, A Tul-Noor, A Vallance, C Walmsley, T Rolles, D Erk, B Burt, M Forbes, R |
| author_facet | Unwin, J Allum, F Britton, M Gabalski, I Bromberger, H Brouard, M Bucksbaum, PH Driver, T Ekanayake, N Garg, D Gougoula, E Heathcote, D Howard, AJ Hockett, P Holland, DMP Kumar, S Lam, C-S Lee, JWL McManus, J Mikosch, J Milesevic, D Minns, RS Papadopoulou, CC Passow, C Razmus, WO Röder, A Rouzée, A Schuurman, M Simao, A Stolow, A Tul-Noor, A Vallance, C Walmsley, T Rolles, D Erk, B Burt, M Forbes, R |
| author_sort | Unwin, J |
| collection | OXFORD |
| description | Structural imaging of transient excited-state species is a key goal of molecular physics, promising to unveil rich information about the dynamics underpinning photochemical transformations. However, separating the electronic and nuclear contributions to the spectroscopic observables is challenging, and typically requires the application of high-level theory. Here, we employ site-selective ionisation via ultrashort soft X-ray pulses and time-resolved Coulomb explosion imaging to interrogate structural dynamics of the ultraviolet photochemistry of carbon disulfide. This prototypical system exhibits the complex motifs of polyatomic photochemistry, including strong non-adiabatic couplings, vibrational mode couplings, and intersystem crossing. Immediately following photoexcitation, we observe Coulomb explosion signatures of highly bent and stretched excited-state geometries involved in the photodissociation. Aided by a model to interpret such changes, we build a comprehensive picture of the photoinduced nuclear dynamics that follows initial bending and stretching motions, as the reaction proceeds towards photodissociation. |
| first_indexed | 2024-03-07T08:10:33Z |
| format | Journal article |
| id | oxford-uuid:0f1f11e7-37c3-44a5-a084-ed5eb8016d48 |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-07T08:10:33Z |
| publishDate | 2023 |
| publisher | Springer Nature |
| record_format | dspace |
| spelling | oxford-uuid:0f1f11e7-37c3-44a5-a084-ed5eb8016d482023-11-28T11:29:09ZX-ray induced Coulomb explosion imaging of transient excited-state structural rearrangements in CS2Journal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:0f1f11e7-37c3-44a5-a084-ed5eb8016d48EnglishSymplectic ElementsSpringer Nature2023Unwin, JAllum, FBritton, MGabalski, IBromberger, HBrouard, MBucksbaum, PHDriver, TEkanayake, NGarg, DGougoula, EHeathcote, DHoward, AJHockett, PHolland, DMPKumar, SLam, C-SLee, JWLMcManus, JMikosch, JMilesevic, DMinns, RSPapadopoulou, CCPassow, CRazmus, WORöder, ARouzée, ASchuurman, MSimao, AStolow, ATul-Noor, AVallance, CWalmsley, TRolles, DErk, BBurt, MForbes, RStructural imaging of transient excited-state species is a key goal of molecular physics, promising to unveil rich information about the dynamics underpinning photochemical transformations. However, separating the electronic and nuclear contributions to the spectroscopic observables is challenging, and typically requires the application of high-level theory. Here, we employ site-selective ionisation via ultrashort soft X-ray pulses and time-resolved Coulomb explosion imaging to interrogate structural dynamics of the ultraviolet photochemistry of carbon disulfide. This prototypical system exhibits the complex motifs of polyatomic photochemistry, including strong non-adiabatic couplings, vibrational mode couplings, and intersystem crossing. Immediately following photoexcitation, we observe Coulomb explosion signatures of highly bent and stretched excited-state geometries involved in the photodissociation. Aided by a model to interpret such changes, we build a comprehensive picture of the photoinduced nuclear dynamics that follows initial bending and stretching motions, as the reaction proceeds towards photodissociation. |
| spellingShingle | Unwin, J Allum, F Britton, M Gabalski, I Bromberger, H Brouard, M Bucksbaum, PH Driver, T Ekanayake, N Garg, D Gougoula, E Heathcote, D Howard, AJ Hockett, P Holland, DMP Kumar, S Lam, C-S Lee, JWL McManus, J Mikosch, J Milesevic, D Minns, RS Papadopoulou, CC Passow, C Razmus, WO Röder, A Rouzée, A Schuurman, M Simao, A Stolow, A Tul-Noor, A Vallance, C Walmsley, T Rolles, D Erk, B Burt, M Forbes, R X-ray induced Coulomb explosion imaging of transient excited-state structural rearrangements in CS2 |
| title | X-ray induced Coulomb explosion imaging of transient excited-state structural rearrangements in CS2 |
| title_full | X-ray induced Coulomb explosion imaging of transient excited-state structural rearrangements in CS2 |
| title_fullStr | X-ray induced Coulomb explosion imaging of transient excited-state structural rearrangements in CS2 |
| title_full_unstemmed | X-ray induced Coulomb explosion imaging of transient excited-state structural rearrangements in CS2 |
| title_short | X-ray induced Coulomb explosion imaging of transient excited-state structural rearrangements in CS2 |
| title_sort | x ray induced coulomb explosion imaging of transient excited state structural rearrangements in cs2 |
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