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Time-resolved imaging and analysis of the electron beam-induced formation of an open-cage metallo-azafullerene

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Title
Time-resolved imaging and analysis of the electron beam-induced formation of an open-cage metallo-azafullerene
Author(s)
Helen Hoelzel; Sol Lee; Konstantin Yu. Amsharov; Norbert Jux; Koji Harano; Eiichi Nakamura; Dominik Lungerich
Publication Date
2023-10
Journal
Nature Chemistry, v.15, no.10, pp.1444 - 1451
Publisher
Nature Research
Abstract
The visualization of single-molecule reactions provides crucial insights into chemical processes, and the ability to do so has grown with the advances in high-resolution transmission electron microscopy. There is currently a limited mechanistic understanding of chemical reactions under the electron beam. However, such reactions may enable synthetic methodologies that cannot be accessed by traditional organic chemistry methods. Here we demonstrate the synthetic use of the electron beam, by in-depth single-molecule, atomic-resolution, time-resolved transmission electron microscopy studies, in inducing the formation of a doubly holed fullerene-porphyrin cage structure from a well-defined benzoporphyrin precursor deposited on graphene. Through real-time imaging, we analyse the hybrid’s ability to host up to two Pb atoms, and subsequently probe the dynamics of the Pb–Pb binding motif in this exotic metallo-organic cage structure. Through simulation, we conclude that the secondary electrons, which accumulate in the periphery of the irradiated area, can also initiate chemical reactions. Consequently, designing advanced carbon nanostructures by electron-beam lithography will depend on the understanding and limitations of molecular radiation chemistry. [Figure not available: see fulltext.] © 2023, The Author(s), under exclusive licence to Springer Nature Limited.
URI
https://pr.ibs.re.kr/handle/8788114/13672
DOI
10.1038/s41557-023-01261-7
ISSN
1755-4330
Appears in Collections:
Center for Nanomedicine (나노의학 연구단) > 1. Journal Papers (저널논문)
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