Unravelling nonclassical beam damage mechanisms in metal-organic frameworks by low-dose electron microscopy
Abstract Recent advances in direct electron detectors and low-dose imaging techniques have opened up captivating possibilities for real-space visualization of radiation-induced structural dynamics. This has significantly contributed to our understanding of electron-beam radiation damage in materials...
Saved in:
| Main Authors: | , , , , , , , , , , , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2025-01-01
|
| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-55632-w |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1841559230674370560 |
|---|---|
| author | Xiaoqiu Xu Liwei Xia Changlin Zheng Yikuan Liu Dongyang Yu Jingjing Li Shigui Zhong Cuiyu Li Huijun Song Yunzhou Liu Tulai Sun Yonghe Li Yu Han Jia Zhao Qiang Lin Xiaonian Li Yihan Zhu |
| author_facet | Xiaoqiu Xu Liwei Xia Changlin Zheng Yikuan Liu Dongyang Yu Jingjing Li Shigui Zhong Cuiyu Li Huijun Song Yunzhou Liu Tulai Sun Yonghe Li Yu Han Jia Zhao Qiang Lin Xiaonian Li Yihan Zhu |
| author_sort | Xiaoqiu Xu |
| collection | DOAJ |
| description | Abstract Recent advances in direct electron detectors and low-dose imaging techniques have opened up captivating possibilities for real-space visualization of radiation-induced structural dynamics. This has significantly contributed to our understanding of electron-beam radiation damage in materials, serving as the foundation for modern electron microscopy. In light of these developments, the exploration of more precise and specific beam damage mechanisms, along with the development of associated descriptive models, has expanded the theoretical framework of radiation damage beyond classical mechanisms. We unravel, in this work, the nonclassical beam damage mechanisms of an open-framework material, i.e. UiO-66(Hf) metal-organic framework, by integrating low-dose electron microscopy and ab initio simulations of radiation induced structural dynamics. The physical origins of radiation damage phenomena, spanning across multiple scales including morphological, lattice, and molecular levels, have been unequivocally unveiled. Based on these observations, potential alternative mechanisms including reversible radiolysis and radiolysis-enhanced knock-on displacement are proposed, which account for their respective dynamic crystalline-to-amorphous interconversion and site-specific ligand knockout events occurring during continuous beam radiation. The current study propels the fundamental understanding of beam damage mechanisms from dynamic and correlated perspectives. Moreover, it fuels technical innovations, such as low-dose ultrafast electron microscopy, enabling imaging of beam-sensitive materials with uncompromised spatial resolution. |
| format | Article |
| id | doaj-art-a061f8af3daa4a8fa4af58a2b068ea39 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-a061f8af3daa4a8fa4af58a2b068ea392025-01-05T12:40:27ZengNature PortfolioNature Communications2041-17232025-01-0116111510.1038/s41467-024-55632-wUnravelling nonclassical beam damage mechanisms in metal-organic frameworks by low-dose electron microscopyXiaoqiu Xu0Liwei Xia1Changlin Zheng2Yikuan Liu3Dongyang Yu4Jingjing Li5Shigui Zhong6Cuiyu Li7Huijun Song8Yunzhou Liu9Tulai Sun10Yonghe Li11Yu Han12Jia Zhao13Qiang Lin14Xiaonian Li15Yihan Zhu16State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology and College of Chemical Engineering, Center for Electron Microscopy, Institute for Frontier and Interdisciplinary Sciences, Zhejiang University of TechnologyState Key Laboratory Breeding Base of Green Chemistry Synthesis Technology and College of Chemical Engineering, Center for Electron Microscopy, Institute for Frontier and Interdisciplinary Sciences, Zhejiang University of TechnologyState Key Laboratory of Surface Physics and Department of Physics, Fudan UniversityState Key Laboratory Breeding Base of Green Chemistry Synthesis Technology and College of Chemical Engineering, Center for Electron Microscopy, Institute for Frontier and Interdisciplinary Sciences, Zhejiang University of TechnologyZhejiang Provincial Key Laboratory of Quantum Precision Measurement, College of Physics, Zhejiang University of TechnologyState Key Laboratory Breeding Base of Green Chemistry Synthesis Technology and College of Chemical Engineering, Center for Electron Microscopy, Institute for Frontier and Interdisciplinary Sciences, Zhejiang University of TechnologyState Key Laboratory Breeding Base of Green Chemistry Synthesis Technology and College of Chemical Engineering, Center for Electron Microscopy, Institute for Frontier and Interdisciplinary Sciences, Zhejiang University of TechnologyState Key Laboratory Breeding Base of Green Chemistry Synthesis Technology and College of Chemical Engineering, Center for Electron Microscopy, Institute for Frontier and Interdisciplinary Sciences, Zhejiang University of TechnologyState Key Laboratory Breeding Base of Green Chemistry Synthesis Technology and College of Chemical Engineering, Center for Electron Microscopy, Institute for Frontier and Interdisciplinary Sciences, Zhejiang University of TechnologyState Key Laboratory Breeding Base of Green Chemistry Synthesis Technology and College of Chemical Engineering, Center for Electron Microscopy, Institute for Frontier and Interdisciplinary Sciences, Zhejiang University of TechnologyState Key Laboratory Breeding Base of Green Chemistry Synthesis Technology and College of Chemical Engineering, Center for Electron Microscopy, Institute for Frontier and Interdisciplinary Sciences, Zhejiang University of TechnologyState Key Laboratory Breeding Base of Green Chemistry Synthesis Technology and College of Chemical Engineering, Center for Electron Microscopy, Institute for Frontier and Interdisciplinary Sciences, Zhejiang University of TechnologyCenter for Electron Microscopy, South China University of TechnologyState Key Laboratory Breeding Base of Green Chemistry Synthesis Technology and College of Chemical Engineering, Center for Electron Microscopy, Institute for Frontier and Interdisciplinary Sciences, Zhejiang University of TechnologyZhejiang Provincial Key Laboratory of Quantum Precision Measurement, College of Physics, Zhejiang University of TechnologyState Key Laboratory Breeding Base of Green Chemistry Synthesis Technology and College of Chemical Engineering, Center for Electron Microscopy, Institute for Frontier and Interdisciplinary Sciences, Zhejiang University of TechnologyState Key Laboratory Breeding Base of Green Chemistry Synthesis Technology and College of Chemical Engineering, Center for Electron Microscopy, Institute for Frontier and Interdisciplinary Sciences, Zhejiang University of TechnologyAbstract Recent advances in direct electron detectors and low-dose imaging techniques have opened up captivating possibilities for real-space visualization of radiation-induced structural dynamics. This has significantly contributed to our understanding of electron-beam radiation damage in materials, serving as the foundation for modern electron microscopy. In light of these developments, the exploration of more precise and specific beam damage mechanisms, along with the development of associated descriptive models, has expanded the theoretical framework of radiation damage beyond classical mechanisms. We unravel, in this work, the nonclassical beam damage mechanisms of an open-framework material, i.e. UiO-66(Hf) metal-organic framework, by integrating low-dose electron microscopy and ab initio simulations of radiation induced structural dynamics. The physical origins of radiation damage phenomena, spanning across multiple scales including morphological, lattice, and molecular levels, have been unequivocally unveiled. Based on these observations, potential alternative mechanisms including reversible radiolysis and radiolysis-enhanced knock-on displacement are proposed, which account for their respective dynamic crystalline-to-amorphous interconversion and site-specific ligand knockout events occurring during continuous beam radiation. The current study propels the fundamental understanding of beam damage mechanisms from dynamic and correlated perspectives. Moreover, it fuels technical innovations, such as low-dose ultrafast electron microscopy, enabling imaging of beam-sensitive materials with uncompromised spatial resolution.https://doi.org/10.1038/s41467-024-55632-w |
| spellingShingle | Xiaoqiu Xu Liwei Xia Changlin Zheng Yikuan Liu Dongyang Yu Jingjing Li Shigui Zhong Cuiyu Li Huijun Song Yunzhou Liu Tulai Sun Yonghe Li Yu Han Jia Zhao Qiang Lin Xiaonian Li Yihan Zhu Unravelling nonclassical beam damage mechanisms in metal-organic frameworks by low-dose electron microscopy Nature Communications |
| title | Unravelling nonclassical beam damage mechanisms in metal-organic frameworks by low-dose electron microscopy |
| title_full | Unravelling nonclassical beam damage mechanisms in metal-organic frameworks by low-dose electron microscopy |
| title_fullStr | Unravelling nonclassical beam damage mechanisms in metal-organic frameworks by low-dose electron microscopy |
| title_full_unstemmed | Unravelling nonclassical beam damage mechanisms in metal-organic frameworks by low-dose electron microscopy |
| title_short | Unravelling nonclassical beam damage mechanisms in metal-organic frameworks by low-dose electron microscopy |
| title_sort | unravelling nonclassical beam damage mechanisms in metal organic frameworks by low dose electron microscopy |
| url | https://doi.org/10.1038/s41467-024-55632-w |
| work_keys_str_mv | AT xiaoqiuxu unravellingnonclassicalbeamdamagemechanismsinmetalorganicframeworksbylowdoseelectronmicroscopy AT liweixia unravellingnonclassicalbeamdamagemechanismsinmetalorganicframeworksbylowdoseelectronmicroscopy AT changlinzheng unravellingnonclassicalbeamdamagemechanismsinmetalorganicframeworksbylowdoseelectronmicroscopy AT yikuanliu unravellingnonclassicalbeamdamagemechanismsinmetalorganicframeworksbylowdoseelectronmicroscopy AT dongyangyu unravellingnonclassicalbeamdamagemechanismsinmetalorganicframeworksbylowdoseelectronmicroscopy AT jingjingli unravellingnonclassicalbeamdamagemechanismsinmetalorganicframeworksbylowdoseelectronmicroscopy AT shiguizhong unravellingnonclassicalbeamdamagemechanismsinmetalorganicframeworksbylowdoseelectronmicroscopy AT cuiyuli unravellingnonclassicalbeamdamagemechanismsinmetalorganicframeworksbylowdoseelectronmicroscopy AT huijunsong unravellingnonclassicalbeamdamagemechanismsinmetalorganicframeworksbylowdoseelectronmicroscopy AT yunzhouliu unravellingnonclassicalbeamdamagemechanismsinmetalorganicframeworksbylowdoseelectronmicroscopy AT tulaisun unravellingnonclassicalbeamdamagemechanismsinmetalorganicframeworksbylowdoseelectronmicroscopy AT yongheli unravellingnonclassicalbeamdamagemechanismsinmetalorganicframeworksbylowdoseelectronmicroscopy AT yuhan unravellingnonclassicalbeamdamagemechanismsinmetalorganicframeworksbylowdoseelectronmicroscopy AT jiazhao unravellingnonclassicalbeamdamagemechanismsinmetalorganicframeworksbylowdoseelectronmicroscopy AT qianglin unravellingnonclassicalbeamdamagemechanismsinmetalorganicframeworksbylowdoseelectronmicroscopy AT xiaonianli unravellingnonclassicalbeamdamagemechanismsinmetalorganicframeworksbylowdoseelectronmicroscopy AT yihanzhu unravellingnonclassicalbeamdamagemechanismsinmetalorganicframeworksbylowdoseelectronmicroscopy |