Journal Article

PUBDB-2023-06333

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png X-ray induced Coulomb explosion imaging of transient excited-state structural rearrangements in CS$_2$

Unwin, J.Extern* ; Allum, F.Extern* ; Britton, M.Extern* ; Gabalski, I. ; Bromberger, H.CFEL*XFEL.EU*DESY* ; Brouard, M.Extern*XFEL.EU* ; Bucksbaum, P. H.Extern* ; Driver, T.Extern*XFEL.EU* ; Ekanayake, N.Extern*DESY* ; Garg, D.DESY* ; Gougoula, E.DESY* ; Heathcote, D.Extern* ; Howard, A. J.Extern* ; Hockett, P.Extern*XFEL.EU* ; Holland, D. M. P.Extern* ; Kumar, S.DESY* ; Lam, C.-s.Extern* ; Lee, J. W. L.Extern*DESY* ; McManus, J.Extern*XFEL.EU* ; Mikosch, J.Extern*XFEL.EU* ; Milesevic, D.Extern* ; Minns, R. S.Extern*XFEL.EU* ; Papadopoulou, C. C.DESY* ; Passow, C.XFEL.EU*DESY* ; Razmus, W. O.Extern* ; Röder, A. ; Rouzée, A.Extern*XFEL.EU* ; Schuurman, M.Extern*XFEL.EU* ; Pinto Simao, A.Extern* ; Stolow, A.Extern* ; Tul-Noor, A.DESY* ; Vallance, C.Extern*XFEL.EU* ; Walmsley, T.Extern* ; Rolles, D.Extern* ; Erk, B.XFEL.EU*DESY* ; Burt, M.Extern* ; Forbes, R. (Corresponding author)Extern*XFEL.EU*

2023
Springer Nature London

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Please use a persistent id in citations: doi:10.1038/s42005-023-01414-7  doi:10.3204/PUBDB-2023-06333

Abstract: 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.

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Contributing Institute(s):

1. DOOR-User (DOOR ; HAS-User)
2. Spectroscopy of molecular processes (FS-SMP)
3. Experimentebetreuung FLASH (FS-FL)
4. CFEL-CMI (FS-CFEL-CMI)
5. Laser Forschung und Entwicklung (FS-LA)
6. FLASH Wissenschaftlicher Nutzerbetrieb (FS-FLASH-O)
7. FLASH Photonen-Diagnose und Steuerungen (FS-FLASH-D)

Research Program(s):

1. 631 - Matter – Dynamics, Mechanisms and Control (POF4-631) (POF4-631)
2. 6G2 - FLASH (DESY) (POF4-6G2) (POF4-6G2)
3. FS-Proposal: F-20200773 (F-20200773) (F-20200773)

Experiment(s):

1. FLASH Beamline BL1 (FLASH)

Appears in the scientific report 2023

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Database coverage:
; ; ; ; Article Processing Charges ; Clarivate Analytics Master Journal List ; Current Contents - Physical, Chemical and Earth Sciences ; DOAJ Seal ; Ebsco Academic Search ; Essential Science Indicators ; Fees ; IF >= 5 ; JCR ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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