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乙醇二价阳离子上H形成动力学的连续机制。

Sequential mechanism in H formation dynamics on the ethanol dication.

作者信息

Gope Krishnendu, Bittner Dror M, Strasser Daniel

机构信息

Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem 9190401, Israel.

出版信息

Phys Chem Chem Phys. 2023 Mar 1;25(9):6979-6986. doi: 10.1039/d2cp03632k.

DOI:10.1039/d2cp03632k
PMID:36804659
Abstract

Two- and three-body Coulomb explosion dynamics of isolated ethanol dications are studied single-photon double-ionization with ultrafast extreme-ultraviolet pulses. The measured 3-body momentum correlations obtained 3D coincidence imaging of the ionic products provide evidence for several concerted and sequential mechanisms: (1) a concerted 3-body breakup mechanism, with dominating channels such as CH + COH + H; (2) sequential dissociation in which the ejection of a low-kinetic-energy neutral OH precedes the Coulomb explosion of CH → CH + CH; and (3) a sequential 3-body breakup mechanism that dominates H formation from the ethanol dication a mechanism that is different from the well-studied H formation in the 2-body Coulomb explosion of the methanol dication. Furthermore, we report surprising branching ratios of the competing C-O bond dissociation channels, resulting in HO, HO and OH formation.

摘要

利用超快极紫外脉冲的单光子双电离研究了孤立乙醇二价阳离子的两体和三体库仑爆炸动力学。通过对离子产物的三维符合成像获得的测量三体动量关联为几种协同和相继机制提供了证据:(1)一种协同三体分裂机制,主要通道如CH + COH + H;(2)相继解离,其中低动能中性OH的喷射先于CH → CH + CH的库仑爆炸;(3)一种相继三体分裂机制,该机制主导了乙醇二价阳离子中H的形成,这是一种不同于在甲醇二价阳离子的两体库仑爆炸中深入研究的H形成机制。此外,我们报告了竞争的C - O键解离通道令人惊讶的分支比,导致形成HO、HO和OH。

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