Exploring the ultrafast and isomer-dependent photodissociation of iodothiophenes via site-selective ionization

doi:10.1039/d3cp06079a

	Exploring the ultrafast and isomer-dependent photodissociation of iodothiophenes via site-selective ionization
	Razmus, Weronika O.1; Allum, Felix 2,3,4; Harries, James 5; Kumagai, Yoshiaki 6; Nagaya, Kiyonobu 7; Bhattacharyya, Surjendu 8; Britton, Mathew 3; Brouard, Mark 2; Bucksbaum, Philip H.3; Cheung, Kieran 2; Crane, Stuart W.9; Fushitani, Mizuho 10; Gabalski, Ian 3,12; Gejo, Tatsuo 11; Ghrist, Aaron 3,4,12; Heathcote, David 2; Hikosaka, Yasumasa 13; Hishikawa, Akiyoshi 10,14; Hockett, Paul 15; Jones, Ellen 2; Kukk, Edwin 16; Iwayama, Hiroshi 17; Lam, Huynh V. S.8; McManus, Joseph W.2; Milesevic, Dennis 2; Mikosch, Jochen 18; Minemoto, Shinichirou 19; Niozu, Akinobu 20; Orr-Ewing, Andrew J.21; Owada, Shigeki 22,23; Rolles, Daniel 8; Rudenko, Artem 8; Townsend, Dave 9; Ueda, Kiyoshi24,25 ; Unwin, James 2; Vallance, Claire 2; Venkatachalam, Anbu 8; Wada, Shin-Ichi 20; Walmsley, Tiffany 2; Warne, Emily M.2; Woodhouse, Joanne L.1; Burt, Michael 2; Ashfold, Michael N. R.21; Minns, Russell S.1; Forbes, Ruaridh 4
	2024-04-05
发表期刊	PHYSICAL CHEMISTRY CHEMICAL PHYSICS (IF:2.9[JCR-2023],3.0[5-Year])
ISSN	1463-9076
EISSN	1463-9084
卷号	26 期号:16 页码:12725-12737
发表状态	已发表
DOI	10.1039/d3cp06079a
摘要	C-I bond extension and fission following ultraviolet (UV, 262 nm) photoexcitation of 2- and 3-iodothiophene is studied using ultrafast time-resolved extreme ultraviolet (XUV) ionization in conjunction with velocity map ion imaging. The photoexcited molecules and eventual I atom products are probed by site-selective ionization at the I 4d edge using intense XUV pulses, which induce multiple charges initially localized to the iodine atom. At C-I separations below the critical distance for charge transfer (CT), charge can redistribute around the molecule leading to Coulomb explosion and charged fragments with high kinetic energy. At greater C-I separations, beyond the critical distance, CT is no longer possible and the measured kinetic energies of the charged iodine atoms report on the neutral dissociation process. The time and momentum resolved measurements allow determination of the timescales and the respective product momentum and kinetic energy distributions for both isomers, which are interpreted in terms of rival ‘direct’ and ‘indirect’ dissociation pathways. The measurements are compared with a classical over the barrier model, which reveals that the onset of the indirect dissociation process is delayed by ∼1 ps relative to the direct process. The kinetics of the two processes show no discernible difference between the two parent isomers, but the branching between the direct and indirect dissociation channels and the respective product momentum distributions show isomer dependencies. The greater relative yield of indirect dissociation products from 262 nm photolysis of 3-iodothiophene (cf. 2-iodothiophene) is attributed to the different partial cross-sections for (ring-centred) π∗ ← π and (C-I bond localized) σ∗ ← (n/π) excitation in the respective parent isomers. © 2024 The Royal Society of Chemistry
关键词	Atoms Binary alloys Charge transfer Computerized tomography Ground state Iodine Ionization Kinetic energy Kinetics Molecules Momentum Photodissociation Photolysis Plants (botany) Bond extension Bond fissions Dissociation process Iodine atoms Localised Photo-excitations Selective ionization Site selective Time-resolved Ultra-fast
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收录类别	EI ; SCI
语种	英语
资助项目	Linac Coherent Light Source["DE-AC02-76SF00515","DE-FG02-86ER13491"] ; School of Chemistry at the University of Southampton[RPG-2021-257] ; Leverhulme trust[EP/S028617/1] ; State of Jersey[EP/T021675/1] ; EPSRC Programme Grant[20K14427] ; University of Bristol[EP/V026690/1] ; EPSRC[101003142] ; European Research Council (ERC) under the European Union[EP/P001459/1]
WOS研究方向	Chemistry ; Physics
WOS类目	Chemistry, Physical ; Physics, Atomic, Molecular & Chemical
WOS记录号	WOS:001203703900001
出版者	Royal Society of Chemistry
EI入藏号	20241615945818
EI主题词	Isomers
EI分类号	631.1 Fluid Flow, General ; 723.5 Computer Applications ; 801.4 Physical Chemistry ; 802.2 Chemical Reactions ; 804 Chemical Products Generally ; 931 Classical Physics ; Quantum Theory ; Relativity ; 931.1 Mechanics ; 931.3 Atomic and Molecular Physics
原始文献类型	Journal article (JA)
引用统计	正在获取...
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/370141
专题	物质科学与技术学院大科学中心
通讯作者	Minns, Russell S.; Forbes, Ruaridh
作者单位	1.School of Chemistry, University of Southampton, Highfield, Southampton; SO17 1BJ, United Kingdom 2.Chemistry Research Laboratory, Department of Chemistry, University of Oxford, Oxford; OX1 3TA, United Kingdom 3.PULSE Institute, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park; CA; 94025, United States 4.Linac Coherent Light Source, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park; CA; 94025, United States 5.QST, SPring-8, Kouto 1-1-1, Hyogo, Sayo, Japan 6.Department of Applied Physics, Tokyo University of Agriculture and Technology, Tokyo, Japan 7.Department of Physics, Kyoto University, Kyoto; 606-8502, Japan 8.J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan; KS; 66506, United States 9.Institute of Photonics and Quantum Sciences, Heriot-Watt University, Edinburgh; EH14 4AS, United Kingdom 10.Department of Chemistry, Graduate School of Science, Nagoya University, Furo-cho, Chikusa, Aichi, Nagoya; 464-8602, Japan 11.Graduate School of Material Science, University of Hyogo, Kuoto 3-2-1, Kamigori-cho, Ako-gun, Hyogo; 678-1297, Japan 12.Department of Applied Physics, Stanford University, Stanford; CA; 94305, United States 13.Institute of Liberal Arts and Sciences, University of Toyama, Toyama; 930-0194, Japan 14.Research Center for Materials Science, Nagoya University, Furo-cho, Chikusa, Aichi, Nagoya; 464-8602, Japan 15.National Research Council of Canada, 100 Sussex Dr, Ottawa; ON; K1A 0R6, Canada 16.Department of Physics and Astronomy, University of Turku, Turku; FI-20014, Finland 17.Institute for Molecular Science, Okazaki; 444-8585, Japan 18.Department of Physics, University of Kassel, Heinrich-Plett-Strasse 40, Kassel; 34132, Germany 19.Department of Physics, Graduate School of Science, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo; 113-0033, Japan 20.Graduate School of Advanced Science and Engineering, Hiroshima University, Higashi-Hiroshima; 739-8526, Japan 21.School of Chemistry, University of Bristol, Cantock's Close, Bristol; BS8 1TS, United Kingdom 22.RIKEN SPring-8 Center, Hyogo, Sayo; 679-5148, Japan 23.Japan Synchrotron Radiation Research Institute, Hyogo, Japan 24.Department of Chemistry, Tohoku University, Sendai; 980-8578, Japan 25.Department of Condensed Matter Physics and Photon Science, School of Physical Science and Technology, ShanghaiTech University, Shanghai; 201210, China
推荐引用方式 GB/T 7714	Razmus, Weronika O.,Allum, Felix,Harries, James,et al. Exploring the ultrafast and isomer-dependent photodissociation of iodothiophenes via site-selective ionization[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2024,26(16):12725-12737.
APA	Razmus, Weronika O..,Allum, Felix.,Harries, James.,Kumagai, Yoshiaki.,Nagaya, Kiyonobu.,...&Forbes, Ruaridh.(2024).Exploring the ultrafast and isomer-dependent photodissociation of iodothiophenes via site-selective ionization.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,26(16),12725-12737.
MLA	Razmus, Weronika O.,et al."Exploring the ultrafast and isomer-dependent photodissociation of iodothiophenes via site-selective ionization".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 26.16(2024):12725-12737.