Time-resolved momentum imaging of UV photodynamics in structural isomers of iodopropane probed by site-selective XUV ionization
Journal Article
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· Physical Chemistry Chemical Physics. PCCP
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- Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Institute (PULSE); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
- Tokyo Univ. of Agriculture and Technology (Japan); Nara Women's Univ. (Japan)
- Kyoto Univ. (Japan)
- National Institutes for Quantum Science and Technology (QST) (Japan)
- Inst. for Molecular Science (Japan); Sokendai (Japan)
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Institute (PULSE)
- Univ. of Oxford (United Kingdom); Trent Univ., Peterborough, ON (Canada)
- Univ. of Oxford (United Kingdom)
- Univ. of Southampton (United Kingdom)
- National Research Council of Canada, Ottawa, ON (Canada)
- Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
- Univ. of Turku (Finland)
- Hiroshima Univ. (Japan)
- Univ. of Bristol (United Kingdom)
- RIKEN SPring-8 Center, Sayo (Japan); Japan Synchrotron Radiation Research Institute, Sayo, Hyogo (Japan)
- Univ. of Oxford (United Kingdom); Univ. of Nottingham (United Kingdom)
- Kansas State Univ., Manhattan, KS (United States)
- Tohoku Univ., Sendai (Japan)
The photodynamics of 1- and 2-iodopropane (1 and 2-IP) were studied in a time-resolved scheme incorporating ultraviolet (UV) excitation and extreme ultraviolet (XUV) probing, which initiates photoionization selectively from the I 4d core orbital. UV absorption in the A-band of both isomers leads to prompt C–I bond fission, with significant disposal of internal energy into the propyl radical product. Site-selective ionization enables a range of charge transfer (CT) processes between the nascent highly charged iodine ions and neutral propyl radicals, dependent on the interfragment distance at the instant of ionization. Subtle differences in the dynamics of these CT processes between the two isomers are observed. In 1-IP, the kinetic energies of iodine ions produced by UV photodissociation and subsequent XUV multiple ionization increased notably over the first few hundred femtoseconds, which could be understood in terms of differing gradients along the photodissociation coordinates of the neutral and polycationic states involved in the pump and probe steps, respectively. Led by a recent report of HI elimination in UV photoexcited 2-IP [Todt et al., Phys. Chem. Chem. Phys., 22(46), 27338 (2020)], we also model the most likely signatures of this process in the present experiment, and can identify signal in the 2-IP data (that is absent or significantly weaker in the data from the unbranched 1-IP isomer) that is consistent with such a process occurring on ultrafast timescales.
- Research Organization:
- Kansas State Univ., Manhattan, KS (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
- Grant/Contract Number:
- AC02-76SF00515; FG02-86ER13491
- OSTI ID:
- 3003090
- Journal Information:
- Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 38 Vol. 27; ISSN 1463-9076; ISSN 1463-9084
- Publisher:
- Royal Society of ChemistryCopyright Statement
- Country of Publication:
- United States
- Language:
- English
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