Multichannel photodissociation dynamics in CS2 studied by ultrafast electron diffraction

Minns, Russell, Razmus, Weronika, Olimpia and Warne, Emily (2022) Multichannel photodissociation dynamics in CS2 studied by ultrafast electron diffraction. Physical Chemistry Chemical Physics, 24 (25), 15416 - 15427. (doi:10.1039/d2cp01268e).

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Abstract

The structural dynamics of photoexcited gas-phase carbon disulfide (CS2) molecules are investigated using ultrafast electron diffraction. The dynamics were triggered by excitation of the optically bright 1B2(1Σu+) state by an ultraviolet femtosecond laser pulse centred at 200 nm. In accordance with previous studies, rapid vibrational motion facilitates a combination of internal conversion and intersystem crossing to lower-lying electronic states. Photodissociation via these electronic manifolds results in the production of CS fragments in the electronic ground state and dissociated singlet and triplet sulphur atoms. The structural dynamics are extracted from the experiment using a trajectory-fitting filtering approach, revealing the main characteristics of the singlet and triplet dissociation pathways. Finally, the effect of the time-resolution on the experimental signal is considered and an outlook to future experiments provided.

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Accepted/In Press date: 4 June 2022

Published date: 8 June 2022

Additional Information: Funding Information: MeV-UED is operated as part of the Linac Coherent Light Source at the SLAC National Accelerator Laboratory, supported in part by the U.S. Department of Energy (DOE) Office of Science, Office of Basic Energy Sciences, SUF Division Accelerator and Detector R&D program, the LCLS Facility, and SLAC under contract No. DE-AC02-05CH11231 and DE-AC02-76SF00515. AK acknowledges funding from the EPSRC (EP/V049240/1 and EP/V006819/1), the Leverhulme Trust (RPG-2020-208), and the Swedish Collegium for Advanced Studies supported by the Erling-Persson Family Foundation and the Knut and Alice Wallenberg Foundation. KA acknowledges an EPSRC doctoral studentship from the University of Edinburgh. WOR thanks the UK Hub for the Physical Sciences on XFELS (STFC) and the University of Southampton for a studentship. EMW gratefully acknowledges the University of Southampton for an EPSRC Doctoral Prize Scholarship (EP/T517859/1). RSM thanks the EPSRC for financial support (EP/R010609/1). TJAW was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division. JPFN, SS and MC were supported by the US Department of Energy Office of Science, Basic Energy Sciences under award no. DE-SC0014170. TW gratefully acknowledges support from the Department of Energy under Award No. DE-FG02-08ER15984. Publisher Copyright: © 2022 The Royal Society of Chemistry.

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