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从电子显微镜下的束流损伤到大规模反应放大:杜瓦苯晶体中的电离诱导链式反应

From Beam Damage to Massive Reaction Amplification under the Electron Microscope: An Ionization-Induced Chain Reaction in Crystals of a Dewar Benzene.

作者信息

Konieczny Krzysztof A, Paul Indrajit, Rodriguez Jose A, Garcia-Garibay Miguel A

机构信息

Department of Chemistry and Biochemistry, University of California at Los Angeles, Los Angeles, California 90095, United States.

Faculty of Chemistry, Wrocław University of Science and Technology, Wybrzeże Wyspiańskiego 27, 50-370 Wroclaw, Poland.

出版信息

ACS Cent Sci. 2024 Dec 6;10(12):2346-2352. doi: 10.1021/acscentsci.4c01429. eCollection 2024 Dec 25.

DOI:10.1021/acscentsci.4c01429
PMID:39735306
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11672530/
Abstract

Electron microscopy in its various forms is one of the most powerful imaging and structural elucidation methods in nanotechnology where sample information is generally limited by random chemical and structural damage. Here we show how a well-selected chemical probe can be used to transform indiscriminate chemical damage into clean chemical processes that can be used to characterize some aspects of the interactions between high-energy electron beams and soft organic matter. Crystals of a Dewar benzene exposed to a 300 keV electron beam facilitate a clean valence-bond isomerization radical-cation chain reaction where the number of chemical events per incident electron is amplified by a factor of up to ca. 90,000.

摘要

各种形式的电子显微镜是纳米技术中最强大的成像和结构解析方法之一,在纳米技术中,样本信息通常受到随机化学和结构损伤的限制。在这里,我们展示了如何使用精心挑选的化学探针将无差别化学损伤转化为可用于表征高能电子束与软有机物质之间相互作用某些方面的清洁化学过程。暴露于300 keV电子束的杜瓦苯晶体促进了一个清洁的价键异构化自由基阳离子链反应,其中每个入射电子的化学事件数量最多可放大约90,000倍。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3360/11672530/dbb78057e3a0/oc4c01429_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3360/11672530/9d2b0a695d83/oc4c01429_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3360/11672530/5b2ea85a0949/oc4c01429_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3360/11672530/279f556fc6ca/oc4c01429_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3360/11672530/726c2f6e8501/oc4c01429_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3360/11672530/dbb78057e3a0/oc4c01429_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3360/11672530/9d2b0a695d83/oc4c01429_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3360/11672530/5b2ea85a0949/oc4c01429_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3360/11672530/279f556fc6ca/oc4c01429_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3360/11672530/726c2f6e8501/oc4c01429_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3360/11672530/dbb78057e3a0/oc4c01429_0005.jpg

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本文引用的文献

1
Reaction amplification with a gain: Triplet exciton-mediated quantum chain using mixed crystals with a tailor-made triplet sensitizer.具有增益的反应放大:使用具有定制三重态敏化剂的混合晶体的三重态激子介导量子链。
Proc Natl Acad Sci U S A. 2024 Apr 2;121(14):e2401982121. doi: 10.1073/pnas.2401982121. Epub 2024 Mar 27.
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Analysis and comparison of electron radiation damage assessments in Cryo-EM by single particle analysis and micro-crystal electron diffraction.通过单颗粒分析和微晶电子衍射对冷冻电镜中电子辐射损伤评估的分析与比较
Front Mol Biosci. 2022 Oct 5;9:988928. doi: 10.3389/fmolb.2022.988928. eCollection 2022.
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Benchmarking the ideal sample thickness in cryo-EM.
在冷冻电镜中对理想样本厚度进行基准测试。
Proc Natl Acad Sci U S A. 2021 Dec 7;118(49). doi: 10.1073/pnas.2108884118.
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An Overview of Microcrystal Electron Diffraction (MicroED).微晶体电子衍射(MicroED)概述。
Annu Rev Biochem. 2021 Jun 20;90:431-450. doi: 10.1146/annurev-biochem-081720-020121.
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Radiation damage to organic and inorganic specimens in the TEM.透射电子显微镜中有机和无机标本的辐射损伤
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Analysis of Global and Site-Specific Radiation Damage in Cryo-EM.低温电子显微镜中全局和局域辐射损伤分析。
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Specimen Behavior in the Electron Beam.电子束中的样本行为
Methods Enzymol. 2016;579:19-50. doi: 10.1016/bs.mie.2016.04.010. Epub 2016 May 31.
8
Photonic amplification by a singlet-state quantum chain reaction in the photodecarbonylation of crystalline diarylcyclopropenones.晶体二芳基环丙烯酮光脱羰基反应中通过单重态量子链反应实现的光子放大。
J Am Chem Soc. 2009 Aug 19;131(32):11606-14. doi: 10.1021/ja9043449.
9
Theoretical studies of quantum amplified isomerizations for imaging systems involving hexamethyl Dewar benzene and related systems.涉及六甲基杜瓦苯及相关体系的成像系统的量子放大异构化理论研究。
J Am Chem Soc. 2006 Jun 21;128(24):7835-45. doi: 10.1021/ja060182i.
10
The Dewar benzene radical cation and its ring-opening reaction.杜瓦苯自由基阳离子及其开环反应。
J Am Chem Soc. 2006 Jun 21;128(24):7828-34. doi: 10.1021/ja060176m.