Time-resolved imaging and analysis of the electron beam-induced formation of an open-cage metallo-azafullerene.
Journal
Nature chemistry
ISSN: 1755-4349
Titre abrégé: Nat Chem
Pays: England
ID NLM: 101499734
Informations de publication
Date de publication:
Oct 2023
Oct 2023
Historique:
received:
04
08
2022
accepted:
26
05
2023
medline:
30
6
2023
pubmed:
30
6
2023
entrez:
29
6
2023
Statut:
ppublish
Résumé
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.
Identifiants
pubmed: 37386284
doi: 10.1038/s41557-023-01261-7
pii: 10.1038/s41557-023-01261-7
doi:
Types de publication
Journal Article
Langues
eng
Sous-ensembles de citation
IM
Pagination
1444-1451Subventions
Organisme : Institute for Basic Science (IBS)
ID : IBS-R026-Y1
Organisme : Deutsche Forschungsgemeinschaft (German Research Foundation)
ID : 1828491499
Organisme : MEXT | Japan Science and Technology Agency (JST)
ID : CREST JPMJCR20B2
Informations de copyright
© 2023. The Author(s), under exclusive licence to Springer Nature Limited.
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