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快速原子离子撞击下甜菜碱中电荷迁移的时间

Timing of charge migration in betaine by impact of fast atomic ions.

作者信息

Rousseau Patrick, González-Vázquez Jesús, Piekarski Dariusz G, Kopyra Janina, Domaracka Alicja, Alcamí Manuel, Adoui Lamri, Huber Bernd A, Díaz-Tendero Sergio, Martín Fernando

机构信息

Normandie Univ, ENSICAEN, UNICAEN, CEA, CNRS, CIMAP, 14000 Caen, France.

Departamento de Química, Módulo 13, Universidad Autónoma de Madrid, 28049 Madrid, Spain.

出版信息

Sci Adv. 2021 Oct;7(40):eabg9080. doi: 10.1126/sciadv.abg9080. Epub 2021 Oct 1.

DOI:10.1126/sciadv.abg9080
PMID:34597129
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10938492/
Abstract

The way molecules break after ion bombardment is intimately related to the early electron dynamics generated in the system, in particular, charge (or electron) migration. We exploit the natural positive-negative charge splitting in the zwitterionic molecule betaine to selectively induce double electron removal from its negatively charged side by impact of fast O ions. The loss of two electrons in this localized region of the molecular skeleton triggers a competition between direct Coulomb explosion and charge migration that is examined to obtain temporal information from ion-ion coincident measurements and nonadiabatic molecular dynamics calculations. We find a charge migration time, from one end of the molecule to the other, of approximately 20 to 40 femtoseconds. This migration time is longer than that observed in molecules irradiated by ultrashort light pulses and is the consequence of charge migration being driven by adiabatic nuclear dynamics in the ground state of the molecular dication.

摘要

离子轰击后分子的断裂方式与系统中产生的早期电子动力学密切相关，特别是电荷（或电子）迁移。我们利用两性离子分子甜菜碱中天然的正负电荷分裂，通过快速O离子的撞击选择性地诱导其带负电一侧的双电子去除。分子骨架这个局部区域中两个电子的损失引发了直接库仑爆炸和电荷迁移之间的竞争，我们通过离子-离子符合测量和非绝热分子动力学计算来研究这种竞争，以获取时间信息。我们发现电荷从分子一端迁移到另一端的时间约为20到40飞秒。这个迁移时间比在超短光脉冲照射的分子中观察到的要长，这是电荷迁移由分子双阳离子基态中的绝热核动力学驱动的结果。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3b86/10938492/0990cf156e89/sciadv.abg9080-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3b86/10938492/0d2c8b71b606/sciadv.abg9080-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3b86/10938492/f12649fb582a/sciadv.abg9080-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3b86/10938492/a933524d85b6/sciadv.abg9080-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3b86/10938492/0990cf156e89/sciadv.abg9080-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3b86/10938492/0d2c8b71b606/sciadv.abg9080-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3b86/10938492/f12649fb582a/sciadv.abg9080-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3b86/10938492/a933524d85b6/sciadv.abg9080-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3b86/10938492/0990cf156e89/sciadv.abg9080-f4.jpg

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本文引用的文献

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Faraday Discuss. 2021 May 27;228(0):349-377. doi: 10.1039/d0fd00121j.
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Interatomic and Intermolecular Coulombic Decay.原子间和分子间库仑衰变。
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Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction.超快电子衍射对核和电子动力学的同时观察。
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OpenMolcas: From Source Code to Insight.OpenMolcas：从源代码到洞见。
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Nat Commun. 2019 Jan 18;10(1):337. doi: 10.1038/s41467-018-08131-8.
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Coulomb explosion imaging of CHI and CHClI photodissociation dynamics.库仑爆炸成像技术研究 CHI 和 CHClI 的光解动力学。
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