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动量分配在协方差离子成像分析中的作用。

The Role of Momentum Partitioning in Covariance Ion Imaging Analysis.

作者信息

Walmsley Tiffany, McManus Joseph W, Kumagai Yoshiaki, Nagaya Kiyonobu, Harries James, Iwayama Hiroshi, Ashfold Michael N R, Britton Mathew, Bucksbaum Philip H, Downes-Ward Briony, Driver Taran, Heathcote David, Hockett Paul, Howard Andrew J, Lee Jason W L, Liu Yusong, Kukk Edwin, Milesevic Dennis, Minns Russell S, Niozu Akinobu, Niskanen Johannes, Orr-Ewing Andrew J, Owada Shigeki, Robertson Patrick A, Rolles Daniel, Rudenko Artem, Ueda Kiyoshi, Unwin James, Vallance Claire, Brouard Mark, Burt Michael, Allum Felix, Forbes Ruaridh

机构信息

Chemistry Research Laboratory, Department of Chemistry, University of Oxford, Oxford OX1 3TA, U.K.

Department of Applied Physics, Tokyo University of Agriculture and Technology, Tokyo 184-8588, Japan.

出版信息

J Phys Chem A. 2024 Jun 6;128(22):4548-4560. doi: 10.1021/acs.jpca.4c00999. Epub 2024 May 7.

DOI:10.1021/acs.jpca.4c00999
PMID:38713032
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11163424/
Abstract

We present results from a covariance ion imaging study, which employs extensive filtering, on the relationship between fragment momenta to gain deeper insight into photofragmentation dynamics. A new data analysis approach is introduced that considers the momentum partitioning between the fragments of the breakup of a molecular polycation to disentangle concurrent fragmentation channels, which yield the same ion species. We exploit this approach to examine the momentum exchange relationship between the products, which provides direct insight into the dynamics of molecular fragmentation. We apply these techniques to extensively characterize the dissociation of 1-iodopropane and 2-iodopropane dications prepared by site-selective ionization of the iodine atom using extreme ultraviolet intense femtosecond laser pulses with a photon energy of 95 eV. Our assignments are supported by classical simulations, using parameters largely obtained directly from the experimental data.

摘要

我们展示了一项协方差离子成像研究的结果,该研究采用了广泛的滤波技术,以探究碎片动量之间的关系,从而更深入地了解光解离动力学。引入了一种新的数据分析方法,该方法考虑分子聚阳离子分解碎片之间的动量分配,以解开产生相同离子种类的并发解离通道。我们利用这种方法来研究产物之间的动量交换关系,这为分子解离动力学提供了直接的见解。我们应用这些技术广泛地表征了通过使用光子能量为95 eV的极紫外强飞秒激光脉冲对碘原子进行位点选择性电离制备的1-碘丙烷和2-碘丙烷二价阳离子的解离。我们的归属得到了经典模拟的支持,模拟参数大多直接从实验数据中获得。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2ef4/11163424/fcaa786ac596/jp4c00999_0009.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2ef4/11163424/2cacb0a49318/jp4c00999_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2ef4/11163424/88bce3ac7dc2/jp4c00999_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2ef4/11163424/0086e5b90d62/jp4c00999_0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2ef4/11163424/fcaa786ac596/jp4c00999_0009.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2ef4/11163424/f8954a77f463/jp4c00999_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2ef4/11163424/495ac5a2549f/jp4c00999_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2ef4/11163424/95fff0e17a78/jp4c00999_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2ef4/11163424/2cacb0a49318/jp4c00999_0006.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2ef4/11163424/fcaa786ac596/jp4c00999_0009.jpg

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本文引用的文献

1
Characterizing the multi-dimensional reaction dynamics of dihalomethanes using XUV-induced Coulomb explosion imaging.
J Chem Phys. 2023 Oct 14;159(14). doi: 10.1063/5.0172749.
2
Time-Resolved X-ray Photoelectron Spectroscopy: Ultrafast Dynamics in CS Probed at the S 2p Edge.时间分辨X射线光电子能谱:在S 2p边缘探测CS中的超快动力学
J Phys Chem Lett. 2023 Aug 10;14(31):7126-7133. doi: 10.1021/acs.jpclett.3c01447. Epub 2023 Aug 3.
3
Multiparticle Cumulant Mapping for Coulomb Explosion Imaging.多粒子关联映射在库仑爆炸成像中的应用。
Phys Rev Lett. 2023 Mar 3;130(9):093001. doi: 10.1103/PhysRevLett.130.093001.
4
Energy-dependent timescales in the dissociation of diiodothiophene dication.二碘噻吩二阳离子离解的能量相关时间尺度。
Phys Chem Chem Phys. 2023 Feb 15;25(7):5795-5807. doi: 10.1039/d2cp05309h.
5
A localized view on molecular dissociation via electron-ion partial covariance.基于电子-离子部分协方差对分子解离的局部视角。
Commun Chem. 2022 Mar 28;5(1):42. doi: 10.1038/s42004-022-00656-w.
6
Disentangling sequential and concerted fragmentations of molecular polycations with covariant native frame analysis.利用协变天然框架分析解析分子聚阳离子的顺序和协同碎片化过程。
Phys Chem Chem Phys. 2022 Sep 28;24(37):22699-22709. doi: 10.1039/d2cp03029b.
7
Cumulant mapping as the basis of multi-dimensional spectrometry.累积映射作为多维光谱法的基础。
Phys Chem Chem Phys. 2022 Sep 14;24(35):20776-20787. doi: 10.1039/d2cp02365b.
8
Predicting Coulomb explosion fragment angular distributions using molecular ground-state vibrational motion.
Phys Chem Chem Phys. 2022 May 18;24(19):11636-11645. doi: 10.1039/d2cp01114j.
9
Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy.分子超快 X 射线光电子能谱中的激发态化学位移。
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J Phys Chem Lett. 2021 Sep 2;12(34):8302-8308. doi: 10.1021/acs.jpclett.1c02481. Epub 2021 Aug 24.