Role of the Environment in Quenching the Production of H3+ from Dicationic Clusters of Methanol
Role of the Environment in Quenching the Production of H3+ from Dicationic Clusters of Methanol
复制标题
环境在淬灭甲醇双阳离子簇生成 H3 中的作用
DOI：
10.1103/physrevlett.126.103402
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发表时间：
2021
影响因子：
8.6
通讯作者：
er Dorn
中科院分区：
文献类型：
--
作者：
Enliang Wang;Xueguang Ren;Alex;er Dorn
有机分子的电离和随后的异构化被认为是外层空间三氢阳离子的重要来源。对这类反应的高度兴趣引发了对各种分子的许多实验和理论研究。在这里，我们报告测量以及ab initiomolecular动力学模拟的碎片双阳离子甲醇单体和集群电离的低能（90 eV）电子。在实验上，对于双阳离子单体，观察到与阳离子化同时形成的断裂通道。模拟结果表明，在第一步中形成了一个中间中性粒子，它在双阳离子周围漫游，最终形成了。整个反应大约需要100-500 fs。计算的离子对动能释放与实验结果符合得很好.相反，对于双阳离子团簇，由于两个电荷分布在不同分子上的可能性，出现了几个快速解离通道，抑制了离子的漫游和离子的形成。本信表明，化学环境对形成的猝灭是有机分子双阳离子簇中的普遍现象。
Ionization and subsequent isomerization of organic molecules has been suggested as an important source of trihydrogencations in outer space. The high interest in such reactions has initiated many experimental and theoretical studies for various molecules. Here, we report measurements as well asab initiomolecular dynamics simulations on the fragmentation of dicationic methanol monomers and clusters ionized by low-energy (90 eV) electrons. Experimentally, for dicationic monomers, a fragmentation channel for the formation ofin coincidence with acation is observed. The simulations show that an intermediate neutralis formed in the first step, and its roaming around the dication ends in the formation of. The entire reaction takes about 100–500 fs. The calculated kinetic energy release for theion pair is in excellent agreement with the experimental result. In contrast, for the dicationic clusters, due to the possibility of distributing the two charges onto different molecules, several fast dissociation channels occur and suppress the roaming ofand formation of. The present Letter suggests that the quenching offormation by the chemical environment is a general phenomenon in dicationic clusters of organic molecules.