TAN Xu; FANG Fan; ZHANG Yu; SUN Dehao; WU Yijiao; YIN Hao; MENG Tianming; TU Bingsheng; WEI Baoren

doi:10.7498/aps.74.20251099

Abstract
Investigating molecular fragmentation mechanisms and the kinetic energy distributions of fragments provides crucial insights into their roles in plasma physics, radiation-induced damage in biological tissues, and interstellar chemistry. In this study, we conducted collision experiments between 3 keV/u Ar⁸⁺ ions and CH₃F molecules using a cold target recoil ion momentum spectrometer. We focused on the three-body fragmentation channel H⁺ + CH²⁺ + F⁺ resulting from C-F and C-H bond cleavage in CH₃F³⁺ ions, and measured the three-dimensional momentum vectors of all fragment ions. The fragmentation mechanism involved was analyzed using ion-ion kinetic energy correlation spectra, Newton diagrams, Dalitz plots and other correlation spectra.
Our results reveal two distinct dissociation mechanisms for the H⁺ + CH²⁺ + F⁺ channel, i.e., concerted 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 CH²⁺ and F⁺. No sequential pathways involving HF²⁺ or CH₃²⁺ intermediates were identified. Furthermore, we observed two types of concerted fragmentation processes with different dynamical characteristics, suggesting that hydrogen atoms in CH₃F³⁺ may occupy different chemical environments. This phenomenon could 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 /

COLTRIMS
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