A1 Refereed original research article in a scientific journal
Time-Resolved Probing of the Iodobenzene C-Band Using XUV-Induced Electron Transfer Dynamics
Authors: Unwin, James; Razmus, Weronika O.; Allum, Felix; Harries, James R.; Kumagai, Yoshiaki; Nagaya, Kiyonobu; Britton, Mathew; Brouard, Mark; Bucksbaum, Philip; Fushitani, Mizuho; Gabalski, Ian; Gejo, Tatsuo; Hockett, Paul; Howard, Andrew J.; Iwayama, Hiroshi; Kukk, Edwin; Lam, Chow-shing; McManus, Joseph; Minns, Russell S.; Niozu, Akinobu; Nishimuro, Sekito; Niskanen, Johannes; Owada, Shigeki; Pickering, James D.; Rolles, Daniel; Somper, James; Ueda, Kiyoshi; Wada, Shin-ichi; Walmsley, Tiffany; Woodhouse, Joanne L.; Forbes, Ruaridh; Burt, Michael; Warne, Emily M.
Publisher: American Chemical Society
Publication year: 2024
Journal: ACS Physical Chemistry Au
Journal name in source: ACS Physical Chemistry Au
eISSN: 2694-2445
DOI: https://doi.org/10.1021/acsphyschemau.4c00036
Web address : https://doi.org/10.1021/acsphyschemau.4c00036
Self-archived copy’s web address: https://research.utu.fi/converis/portal/detail/Publication/457536795
Time-resolved extreme ultraviolet spectroscopy was used to investigate photodissociation within the iodobenzene C-band. The carbon–iodine bond of iodobenzene was photolyzed at 200 nm, and the ensuing dynamics were probed at 10.3 nm (120 eV) over a 4 ps range. Two product channels were observed and subsequently isolated by using a global fitting method. Their onset times and energetics were assigned to distinct electron transfer dynamics initiated following site-selective ionization of the iodine photoproducts, enabling the electronic states of the phenyl fragments to be identified using a classical over-the-barrier model for electron transfer. In combination with previous theoretical work, this allowed the corresponding neutral photochemistry to be assigned to (1) dissociation via the 7B2, 8A2, and 8B1 states to give ground-state phenyl, Ph(X), and spin–orbit excited iodine and (2) dissociation through the 7A1 and 8B2 states to give excited-state phenyl, Ph(A), and ground-state iodine. The branching ratio was determined to be 87 ± 4\% Ph(X) and 13 ± 4\% Ph(A). Similarly, the corresponding amount of energy deposited into the internal phenyl modes in these channels was determined to be 44 ± 10 and 65 ± 21\%, respectively, and upper bounds to the channel rise times were found to be 114 ± 6 and 310 ± 60 fs.
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Funding information in the publication:
The experiment was performed at SACLA with the approval ofJASRI and the program review committee (proposal No.2022B8048). M.Bu. and E.W. thank the technical and scientificstaff of SACLA for their hospitality and support before andduring the beamtime as well as R.F. and F.A. for initiating thescientific collaboration that originally made these experimentspossible. M.Bu., J.S., J.U., E.W., and T.W. are also grateful toEPSRC for support from EP/S028617/1 and to the Universityof Oxford for a Covid Rebuilding Research Momentum award.J.U. additionally thanks the States of Jersey for studentshipfunding, and T.W. thanks EPSRC for studentship funding aswell as Jesus College, Oxford for a partial fee scholarship. R.F.and F.A. gratefully acknowledge support from the LinacCoherent Light Source, SLAC National Accelerator Labo-ratory, which is supported by the US Department of Energy,Office of Science, Office of Basic Energy Sciences, undercontract no. DE-AC02-76SF00515. R.S.M. thanks the EPSRC(EP/R010609/1) and Leverhulme Trust (RPG-2021-257) forfinancial support. W.O.R. thanks the UK XFEL hub forphysical sciences and the University of Southampton for aStudentship. C.-S.L., J.W.M., and M.Bro. gratefully acknowl-edge the support of EPSRC Programme grant EP/V026690/1. D.R. was supported by the Chemical Sciences, Geosciences,and Biosciences Division, Office of Basic Energy Sciences,Office of Science, US Department of Energy under grant no.DE-FG02-86ER13491. P.H.B., A.J.H., and M.Bri. weresupported by the National Science Foundation. J.N. acknowl-edges Academy of Finland funding via project 331234. Y.K.acknowledges support from the Nikki-Saneyoshi (JGC-S)Scholarship Foundation. M.F. acknowledges support fromJSPS KAKENHI (Grants No. 20K05549). A CC-BY license isapplied to the author accepted manuscript arising from thissubmission, in accordance with UKRI open access conditions.
