高电荷态离子碰撞诱导氟甲烷分子三价离子解离

谭旭; 房凡; 张煜; 孙德昊; 吴怡娇; 殷浩; 孟天鸣; 屠秉晟; 魏宝仁

doi:10.7498/aps.74.20251099

摘要

研究分子的碎裂机制以及碎片的动能分布, 有助于理解其在等离子体物理、生物组织的辐射损伤和星际化学等方面的重要作用. 本文利用冷靶反冲离子动量谱仪开展了3 keV/u的Ar⁸⁺离子束与氟甲烷气体分子束的碰撞实验, 聚焦CH₃F³⁺离子C—F键和C—H键断裂后形成H⁺+$ {\mathrm{C}\mathrm{H}}_{2}^{+} $+F⁺这一三体碎裂通道, 测得3个碎片离子的三维动量. 借助离子-离子动能谱、Newton图和Dalitz图展示碎片的动能与动量关联, 分析了H⁺+$ {\mathrm{C}\mathrm{H}}_{2}^{+} $+F⁺通道的解离机制. 研究发现, 该通道存在协同碎裂以及通过中间体CH₂F²⁺顺序碎裂两种解离方式, 其中协同碎裂占主导地位. 此外, 实验上观测到两种不同动力学特征的协同碎裂过程, 表明CH₃F³⁺离子中H原子可以具有不同的化学环境. 这可能是由于分子异构化产生不同分子构型或者Jahn-Teller效应使得分子产生不同C—H键所致.

关键词:

Abstract

Investigating molecular fragmentation mechanisms and the kinetic energy distributions of fragments can offer crucial insights into their roles in plasma physics, radiation-induced damage in biological tissues, and interstellar chemistry. In this study, we conduct the experiments on collision between 3 keV/u ${\rm Ar}^{8+} $ ions and CH₃F molecules by using a cold target recoil ion momentum spectrometer (COLTRIMS).We focus on the three-body fragmentation channel H⁺+$ {\mathrm{C}\mathrm{H}}_{2}^{+} $+F⁺ resulting from C—F and C—H bond cleavage in CH₃F³⁺ ions, and measure the three-dimensional momentum vectors of all fragment ions. The fragmentation mechanism involved is analyzed using ion-ion kinetic energy correlation spectra, Newton diagrams, Dalitz plots, and other correlation spectra.Our results reveal two different dissociation mechanisms for the H⁺+$ {\mathrm{C}\mathrm{H}}_{2}^{+} $+F⁺ channel, i.e. concerted fragmentation and sequential fragmentation, with the former one being dominant. In the sequential fragmentation process, H⁺ and the intermediate CH₂F²⁺ are firstly formed, followed by further fragmentation of the intermediates into $ {\mathrm{C}\mathrm{H}}_{2}^{+} $ and F⁺. No sequential pathways involving HF²⁺ or $ {\mathrm{C}\mathrm{H}}_{3}^{2+} $ intermediates are identified. Furthermore, we observe two types of concerted fragmentation processes with different dynamical characteristics, suggesting that hydrogen atoms in CH₃F³⁺ may occupy different chemical environments. This phenomenon can originate from either molecular isomerization producing different structural geometries or the Jahn-Teller effect leading to inequivalent C—H bonds. This study reveals the three-body dissociation dynamics of CH₃F³⁺ induced by highly charged ion collisions, highlighting the significant role of the Jahn-Teller effect or molecular isomerization in the ionic dissociation of polyatomic molecules.

Keywords:

fluoromethane /
dissociative ionization /
three-body fragmentation /
cold target recoil ion momentum spectrometer

作者及机构信息

1.
复旦大学现代物理研究所, 核物理与离子束应用教育部重点实验室, 上海　200433

2.
嘉兴大学机械工程学院, 嘉兴　314001

通信作者: 张煜, zyclay@outlook.com ; 魏宝仁, brwei@fudan.edu.cn

基金项目: 国家自然科学基金(批准号: 12374227, 12104185)、国家重点研发计划(批准号: 2022YFA1602504)和嘉兴市青年科技人才专项(批准号: 2024AY40007)资助的课题.

Authors and contacts

1.
Key Laboratory of Nuclear Physics and Ion Beam Application of the Ministry of Education, Institute of Modern Physics, Fudan University, Shanghai 200433, China

2.
College of Mechanical Engineering, Jiaxing University, Jiaxing 314001, China

Corresponding author: ZHANG Yu, zyclay@outlook.com ; WEI Baoren, brwei@fudan.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 12374227, 12104185), the National Key R&D Program of China (Grant No. 2022YFA1602504), and the Young Sci-Tech Talent Special Program of Jiaxing, China (Grant No. 2024AY40007).

文章全文

参考文献

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施引文献

图 1 CH₃F³⁺离子解离的三离子TOF符合谱

Fig. 1. Coincidence TOF map of CH₃F³⁺ dissociation involving three ionic fragments.

下载: 全尺寸图片幻灯片

图 2 H⁺+$ {\mathrm{C}\mathrm{H}}_{2}^{+} $+F⁺通道的Newton图

Fig. 2. Newton diagrams of H⁺+$ {\mathrm{C}\mathrm{H}}_{2}^{+} $+F⁺ channel.

下载: 全尺寸图片幻灯片

图 3 $ {\mathrm{C}\mathrm{H}}_{2}^{+} $离子和F⁺离子的动能关联谱

Fig. 3. Kinetic energy correlation spectra of $ {\mathrm{C}\mathrm{H}}_{2}^{+} $ ions and F⁺ ions.

下载: 全尺寸图片幻灯片

图 4 H⁺+$ {\mathrm{C}\mathrm{H}}_{2}^{+} $+F⁺通道的Dalitz图, 其中(a), (b), (c)分别为图3中A, B和C区域中的碎裂事件

Fig. 4. Dalitz diagrams of H⁺+$ {\mathrm{C}\mathrm{H}}_{2}^{+} $+F⁺ channel, (a), (b), (c) corresponding to fragmentation events in regions A, B, and C of Fig. 3, respectively.

下载: 全尺寸图片幻灯片

图 5 H⁺+$ {\mathrm{C}\mathrm{H}}_{2}^{+} $+F⁺通道所有事件以及图3中不同区域事件的KER谱

Fig. 5. KER spectra for all events of H⁺+$ {\mathrm{C}\mathrm{H}}_{2}^{+} $+F⁺ channel and events in different regions of Fig. 3.

下载: 全尺寸图片幻灯片

图 6 $ {\mathrm{K}\mathrm{E}\mathrm{R}}_{{\mathrm{H}\mathrm{F}}^{2+}} $和$ {\theta }_{{\mathrm{C}\mathrm{H}}_{2}^{+}, {\mathrm{H}}^{+}} $的关联谱

Fig. 6. Correlation spectrum of $ {\mathrm{K}\mathrm{E}\mathrm{R}}_{{\mathrm{H}\mathrm{F}}^{2+}} $and $ {\theta }_{{\mathrm{C}\mathrm{H}}_{2}^{+}, {\mathrm{H}}^{+}} $.

下载: 全尺寸图片幻灯片

下载: 全尺寸图片幻灯片

[1]	Thissen R, Witasse O, Dutuit O, Wedlund C S, Gronoff G, Lilensten J 2011 Phys. Chem. Chem. Phys. 13 18264 Google Scholar
[2]	Reiter D, Janev R K 2010 Contrib. Plasma Phys. 50 986 Google Scholar
[3]	Wheatley A K, Juno J A, Wang J J, Selva K J, Reynaldi A, Tan H X, Lee W S, Wragg K M, Kelly H G, Esterbauer R, Davis S K, Kent H E, Mordant F L, Schlub T E, Gordon D L, Khoury D S, Subbarao K, Cromer D, Gordon T P, Chung A W, Davenport M P, Kent S J 2021 Nat. Commun. 12 1162 Google Scholar
[4]	Ren X G, Wang E L, Skitnevskaya A D, Trofimov A B, Gokhberg K, Dorn A 2018 Nat. Phys. 14 1062 Google Scholar
[5]	Price S D, Roithová J 2011 Phys. Chem. Chem. Phys. 13 18251 Google Scholar
[6]	Matsika S, Spanner M, Kotur M, Weinacht T C 2013 J. Phys. Chem. A 117 12796 Google Scholar
[7]	Ren B H, Ma P F, Zhang Y, Wei L, Han J, Xia Z H, Wang J R, Meng T M, Yu W D, Zou Y M, Yang C L, Wei B R 2022 Phys. Rev. A 106 012805 Google Scholar
[8]	Lin K, Hu X Q, Pan S Z, Chen F, Ji Q Y, Zhang W B, Li H X, Qiang J J, Sun F H, Gong X C, Li H, Lu P F, Wang J G, Wu Y, Wu J 2020 J. Phys. Chem. Lett. 11 3129 Google Scholar
[9]	张紫琪, 闫顺成, 陶琛玉, 余璇, 张少锋, 马新文 2025 物理学报 74 063401 Google Scholar Zhang Z Q, Yan S C, Tao C Y, Yu X, Zhang S F, Ma X W 2025 Acta Phys. Sin. 74 063401 Google Scholar
[10]	Das R, Bhojani A K, Madhusudhan P, Nimma V, Bhardwaj P, Singh D K, Kushawaha R K 2025 J. Phys. B: At. Mol. Opt. Phys. 58 045603 Google Scholar
[11]	Wang E L, Shan X, Chen L, Pfeifer T, Chen X J, Ren X G, Dorn A 2020 J. Phys. Chem. A 124 2785 Google Scholar
[12]	Zhang Y, Jiang T, Wei L, Luo D, Wang X, Yu W, Hutton R, Zou Y, Wei B 2018 Phys. Rev. A 97 022703 Google Scholar
[13]	Wei B, Zhang Y, Wang X, Lu D, Lu G C, Zhang B H, Tang Y J, Hutton R, Zou Y 2014 J. Chem. Phys. 140 124303 Google Scholar
[14]	Wang B, Han J, Zhu X L, Wei L, Ren B H, Zhang Y, Yu W D, Yan S C, Ma X W, Zou Y M, Chen L, Wei B R 2021 Phys. Rev. A 103 042810 Google Scholar
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[17]	Hishikawa A, Matsuda A, Takahashi E J, Fushitani M 2008 J. Chem. Phys. 128 084302 Google Scholar
[18]	Müller H S P, Schlöder F, Stutzki J, Winnewisser G 2005 J. Mol. Struct. 742 215 Google Scholar
[19]	Das R, Pandey D K, Soumyashree S, Madhusudhan P, Nimma V, Bhardwaj P, Muhammed S K M, Singh D K, Kushawaha R K 2022 Phys. Chem. Chem. Phys. 24 18306 Google Scholar
[20]	Townsend D, Lahankar S A, Lee S K, Chambreau S D, Suits A G, Zhang X, Rheinecker J, Harding L B, Bowman J M 2004 Science 306 1158 Google Scholar
[21]	Nakai K, Kato T, Kono H, Yamanouchi K 2013 J. Chem. Phys. 139 181103 Google Scholar
[22]	Castrovilli M C, Trabattoni A, Bolognesi P, O’Keeffe P, Avaldi L, Nisoli M, Calegari F, Cireasa R 2018 J. Phys. Chem. Lett. 9 6012 Google Scholar
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[24]	Kokkonen E, Vapa M, Bučar K, Jänkälä K, Cao W, Žitnik M, Huttula M 2016 Phys. Rev. A 94 033409 Google Scholar
[25]	Masuoka T, Koyano I 1991 J. Chem. Phys. 95 909 Google Scholar
[26]	Ma P F, Wang J R, Zhang Z X, Meng T M, Xia Z H, Ren B H, Wei L, Yao K, Xiao J, Zou Y M, Tu B S, Wei B R 2023 Nucl. Sci. Tech. 34 156 Google Scholar
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[29]	Zhou J Q, Li Y T, Wang Y Y, Jia S K, Xue X R, Yang T, Zhang Z, Dorn A, Ren X G 2021 Phys. Rev. A 104 032807 Google Scholar
[30]	Ma C, Xu S Y, Zhao D M, Guo D L, Yan S C, Feng W T, Zhu X L, Ma X W 2020 Phys. Rev. A 101 052701 Google Scholar
[31]	Yan S, Zhu X L, Zhang P, Ma X, Feng W T, Gao Y, Xu S, Zhao Q S, Zhang S F, Guo D L, Zhao D M, Zhang R T, Huang Z K, Wang H B, Zhang X J 2016 Phys. Rev. A 94 032708 Google Scholar
[32]	Pearson R G 1975 Proc. Nat. Acad. Sci. USA 72 2104 Google Scholar
[33]	Bersuker I B 2001 Chem. Rev. 101 1067 Google Scholar
[34]	Bersuker I B 2021 Chem. Rev. 121 1463 Google Scholar
[35]	Wörner H J, Merkt F 2009 Angew. Chem. Int. Ed. 48 6404 Google Scholar
[36]	Jahn H A, Teller E 1937 Proc. R. Soc. London Ser. A 161 220 Google Scholar
[37]	Matselyukh D, Svoboda V, Wörner H J 2025 Nat. Commun. 16 6540 Google Scholar
[38]	Wang J G, Dong B W, Zhang M, Deng Y K, Jian X P, Li Z, Liu Y Q 2024 J. Am. Chem. Soc. 146 10443 Google Scholar
[39]	Kugel' K I, Khomskiĭ D I 1982 Sov. Phys. Usp. 25 231 Google Scholar
[40]	O’Brien M C, Chancey C C 1993 Am. J. Phys. 61 688 Google Scholar
[41]	Zhou J Q, Wu L, Belina M, Skitnevskaya A D, Jia S K, Xue X R, Hao X T, Zeng Q R, Ma Q B, Zhao Y T, Li X K, He L H, Luo S Z, Zhang D D, Wang C C, Trofimov A B, Slavíček P, Ding D J, Ren X G 2025 Nat. Commun. 16 5838 Google Scholar
[42]	Zhao X N, Zhang X Y, Liu H, Ma P, Li X K, Wang C C, Luo S Z, Ding D J 2025 Phys. Rev. A 111 053106 Google Scholar
[43]	Zhou J Q, Belina M, Jia S K, Xue X R, Hao X T, Ren X G, Slavíček P 2022 J. Phys. Chem. Lett. 13 10603 Google Scholar
[44]	Yuan H, Gao Y, Yang B, Gu S F, Lin H, Guo D L, Liu J L, Zhang S F, Ma X W, Xu S Y 2024 Phys. Rev. Lett. 133 193002 Google Scholar
[45]	Duflot D, Robbe J M, Flament J P 1995 J. Chem. Phys. 103 10571 Google Scholar
[46]	Matsubara T 2023 J. Phys. Chem. A 127 4801 Google Scholar

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高电荷态离子碰撞诱导氟甲烷分子三价离子解离