X-ray induced Coulomb explosion imaging of transient excited-state structural rearrangements in CS2

Unwin, James; Allum, Felix; Britton, Mathew; Gabalski, Ian; Bromberger, Hubertus; Brouard, Mark; Bucksbaum, Philip H.; Driver, Taran; Ekanayake, Nagitha; Garg, Diksha; Gougoula, Eva; Heathcote, David; Howard, Andrew J.; Hockett, Paul; Holland, David M. P.; Kumar, Sonu; Lam, Chow-shing; Lee, Jason W. L.; McManus, Joseph; Mikosch, Jochen; Milesevic, Dennis; Minns, Russell S.; Papadopoulou, Christina C.; Passow, Christopher; Razmus, Weronika O.; Röder, Anja; Rouzée, Arnaud; Schuurman, Michael; Simao, Alcides; Stolow, Albert; Tul-Noor, Atia; Vallance, Claire; Walmsley, Tiffany; Rolles, Daniel; Erk, Benjamin; Burt, Michael; Forbes, Ruaridh

doi:10.1038/s42005-023-01414-7

Title: X-ray induced Coulomb explosion imaging of transient excited-state structural rearrangements in CS2

Journal Article · 20 October 2023 · Communications Physics

DOI: https://doi.org/10.1038/s42005-023-01414-7 · OSTI ID:2203129

;

; Britton, Mathew; Gabalski, Ian;

;

; Bucksbaum, Philip H.; Driver, Taran;

; Garg, Diksha; Gougoula, Eva;

;

; Lam, Chow-shing;

; McManus, Joseph; Mikosch, Jochen more »

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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Sponsoring Organization:: USDOE

OSTI ID:: 2203129

Journal Information:: Communications Physics, Journal Name: Communications Physics Journal Issue: 1 Vol. 6; ISSN 2399-3650

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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