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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Double Imaging Photoelectron Photoion Coincidence Sheds New Light on the Dissociation of State-Selected CH3F+ Ions
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Double Imaging Photoelectron Photoion Coincidence Sheds New Light on the Dissociation of State-Selected CH3F+ Ions

机译：双重成像光电子光相结合脱落在状态选择的CH3F +离子的解离

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The vacuum ultraviolet (VUV) photoionization and dissociative photoionization of methyl fluoride (CH3F) in the 12.2-19.8 eV energy range were investigated by using synchrotron radiation coupled to a double imaging photoelectron photoion coincidence (i(2)PEPICO) spectrometer. The production of several fragment ions including CH2F+, CHF+, CH3+, and CH2+ as a function of state and internal energy of CH3F+ ions was identified and analyzed, with their individual appearance energies measured through threshold photoelectron spectroscopy. Dynamical information was inferred from electron and ion kinetic energy correlation diagrams measured at chosen fixed photon energies. The detailed mechanisms governing the dissociation of state-selected CH3F+ ions prepared in the (XE)-E-2, A(2)A(1), and (BE)-E-2 low-lying electronic states as well as outside the Franck-Condon region have been inferred based on the present experimental results and existing theoretical calculations. Both the CH2F+ and CH3+ primary fragment ions have three different channels of production from different electronic states of CH3F+. The spin-orbit splitting states of the F fragment, P-2(3/2) and P-2(1/2), in the CH3+ + F dissociation channels were assigned and adiabatically correlate to the (XE)-E-2 ground state and the A(2)A(1) electronic state, respectively, with the aid of previous theoretical results. The CH3F+ ions in the high energy part of the (XE)-E-2 ground state are unstable and statistically dissociate to the CH2F+ (1(1)A(1)) and H(S-2) fragments along the potential energy curve of the (XE)-E-2 state. The A(2)A(1) electronic state is a repulsive state and exclusively dissociates to the CH3+ (1(1)A(1)') and F(P-2(1/2)) fragments. In addition, the CH2F+, CHF+, CH3+, and CH2+ fragment ions are also produced in the (BE)-E-2 state and in the Franck-Condon gap by indirect processes, such as internal conversion or dissociative autoionization.
机译：通过使用同步辐射耦合到双成像光电子光电巧合（I（2）Pepico）光谱仪，研究了在12.2-19.8 eB能量范围内的真空紫外（Vuv）光离子（CH3F）的去氟化甲基（CH3F）的去除光离子化。鉴定并分析包括CH 2 F +，CHF +，CH3 +和CH2 +的几个片段离子，包括CH3F +离子的状态和内能量的函数，其各个外观能量​​通过阈值光电子谱测量。从选择的固定光子能量测量的电子和离子动能相关图中推断动力信息。治疗在（XE）-2，A（2）A（1），（2）-2（2）-2低位电子州以及外部的（2）-2（1）中制备的状态所选CH3F +离子解离的详细机制，以及（是）基于目前的实验结果和现有的理论计算，已经推断了Franck-Condon区域。 CH2F +和CH3 +初级片段离子都具有来自CH3F +的不同电子状态的三种不同的产生通道。在CH3 + + F离解通道中的F片段，P-2（3/2）和P-2（1/2）的旋转轨道分裂状态被分配和绝热地与（XE）-E-2相关接地状态和A（2）A（1）电子状态，借助于先前的理论结果。 （XE）-2-2-2接地状态的高能部分中的CH3F +离子不稳定并且统计地解离CH2F +（1）（1））和H沿电位能曲线的碎片（XE）-E-2状态。 A（2）（1）电子状态是排斥状态，并专门解离CH3 +（1（1）（1）'）和F（P-2（1/2））片段。另外，CH 2 F +，CHF +，CH3 +和CH2 +片段离子也通过间接过程（例如内部转化或离托自动化）在FRANCK-CONDON差距中产生。

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