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突破超快衍射的极限:成像孤立分子中的量子相干性。

Pushing the limits of ultrafast diffraction: Imaging quantum coherences in isolated molecules.

作者信息

Tang Zilong, Jarupula Ramesh, Yong Haiwang

机构信息

Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, CA 92093, USA.

Program in Materials Science and Engineering, University of California, San Diego, La Jolla, CA 92093, USA.

出版信息

iScience. 2024 Aug 10;27(9):110705. doi: 10.1016/j.isci.2024.110705. eCollection 2024 Sep 20.

DOI:10.1016/j.isci.2024.110705
PMID:39262780
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11388184/
Abstract

Quantum coherence governs the outcome and efficiency of photochemical reactions and ultrafast molecular dynamics. Recent ultrafast gas-phase X-ray scattering and electron diffraction have enabled the observation of femtosecond nuclear dynamics driven by vibrational coherence. However, probing attosecond electron dynamics and coupled electron-nuclear dynamics remains challenging. This article discusses advances in ultrafast X-ray scattering and electron diffraction, highlighting their potential to resolve attosecond charge migration and vibronic coupling at conical intersections. Novel techniques, such as X-ray scattering with orbital angular momentum beams and combined X-ray and electron diffraction, promise to selectively probe coherence contributions and visualize charge migration in real-space. These emerging methods could further our understanding of coherence effects in chemical reactions.

摘要

量子相干控制着光化学反应和超快分子动力学的结果与效率。近期的超快气相X射线散射和电子衍射使得对由振动相干驱动的飞秒核动力学的观测成为可能。然而,探测阿秒电子动力学以及耦合的电子-核动力学仍然具有挑战性。本文讨论了超快X射线散射和电子衍射的进展,突出了它们在锥形交叉点解析阿秒电荷迁移和振子耦合的潜力。诸如利用轨道角动量光束进行X射线散射以及联合X射线和电子衍射等新技术,有望选择性地探测相干贡献并在实空间中可视化电荷迁移。这些新兴方法能够增进我们对化学反应中相干效应的理解。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/edc4/11388184/a9dfeba853be/gr4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/edc4/11388184/d9b1c10c4597/fx1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/edc4/11388184/9b7c61aa43e6/gr1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/edc4/11388184/005e13bc357f/gr2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/edc4/11388184/ced6963347c5/gr3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/edc4/11388184/a9dfeba853be/gr4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/edc4/11388184/d9b1c10c4597/fx1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/edc4/11388184/9b7c61aa43e6/gr1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/edc4/11388184/005e13bc357f/gr2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/edc4/11388184/ced6963347c5/gr3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/edc4/11388184/a9dfeba853be/gr4.jpg

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本文引用的文献

1
A comparative review of time-resolved x-ray and electron scattering to probe structural dynamics.用于探测结构动力学的时间分辨X射线和电子散射的比较综述。
Struct Dyn. 2024 May 1;11(3):031301. doi: 10.1063/4.0000249. eCollection 2024 May.
2
Femtosecond Electronic and Hydrogen Structural Dynamics in Ammonia Imaged with Ultrafast Electron Diffraction.用超快电子衍射成像法观测氨中的飞秒级电子与氢结构动力学
Phys Rev Lett. 2023 Oct 6;131(14):143001. doi: 10.1103/PhysRevLett.131.143001.
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Open questions in attochemistry.原子化学中的开放性问题。
Commun Chem. 2023 Sep 4;6(1):184. doi: 10.1038/s42004-023-00989-0.
4
Rehybridization dynamics into the pericyclic minimum of an electrocyclic reaction imaged in real-time.电环化反应的周环最小势能点的实时成像中的再杂交动力学。
Nat Commun. 2023 May 18;14(1):2795. doi: 10.1038/s41467-023-38513-6.
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Exploiting chemistry and molecular systems for quantum information science.利用化学和分子系统实现量子信息科学
Nat Rev Chem. 2020 Sep;4(9):490-504. doi: 10.1038/s41570-020-0200-5. Epub 2020 Jul 7.
6
Real-time observation of a correlation-driven sub 3 fs charge migration in ionised adenine.对电离腺嘌呤中关联驱动的亚3飞秒电荷迁移的实时观测
Commun Chem. 2021 May 20;4(1):73. doi: 10.1038/s42004-021-00510-5.
7
Novel Ultrafast Molecular Imaging Based on the Combination of X-ray and Electron Diffraction.基于 X 射线和电子衍射结合的新型超快分子成像。
J Phys Chem A. 2023 Jan 26;127(3):835-841. doi: 10.1021/acs.jpca.2c08024. Epub 2023 Jan 17.
8
Attosecond Charge Migration in Molecules Imaged by Combined X-ray and Electron Diffraction.通过结合X射线和电子衍射成像的分子中的阿秒电荷迁移
J Am Chem Soc. 2022 Nov 16;144(45):20710-20716. doi: 10.1021/jacs.2c07997. Epub 2022 Nov 1.
9
Direct Monitoring of Conical Intersection Passage via Electronic Coherences in Twisted X-Ray Diffraction.通过扭曲X射线衍射中的电子相干直接监测锥形交叉通道
Phys Rev Lett. 2022 Sep 2;129(10):103001. doi: 10.1103/PhysRevLett.129.103001.
10
Multichannel photodissociation dynamics in CS studied by ultrafast electron diffraction.利用超快电子衍射研究CS中的多通道光解离动力学。
Phys Chem Chem Phys. 2022 Jun 29;24(25):15416-15427. doi: 10.1039/d2cp01268e.