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説明:

The bottom-up synthesis of strained hollow cage structures, such as fullerenes, using traditional thermal or photochemical methods remains one of the most challenging tasks in organic chemistry. Here, we demonstrate the synthetic use of an electron beam by in-depth single-molecule atomic resolution time-resolved transmission electron microscopy studies to induce the formation of a doubly-holed fullerene-porphyrin cage structure from a well-defined benzoporphyrin precursor deposited on graphene. Through real-time imaging, we analyze the hybrid’s peculiar ability to host up to two Pb atoms and subsequently gain insights into the dynamics of the Pb–Pb binding motif in this exotic organometallic cage structure. With the help of density functional theory calculations and image simulations, we identify two central mechanisms responsible for the molecular transformations. Importantly, not only the fast primary electrons appear to induce chemical reactions, but also the much slower secondary electrons, which accumulate in the periphery of the irradiated area.

権利情報:

• In Copyright
  

キーワード: molecular imaging, radiation chemistry, cinematic chemistry, single-molecule dynamics, DFT-modeling, transmission electron microscopy

刊行年月日: 2023-06-29

出版者: Springer Science and Business Media LLC

掲載誌:

• Nature Chemistry (ISSN: 17554349) vol. 15 p. 1444-1451

研究助成金:

原稿種別: 著者最終稿 (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.4241

公開URL: https://doi.org/10.1038/s41557-023-01261-7

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更新時刻: 2024-01-05 22:12:51 +0900

MDRでの公開時刻: 2024-01-11 08:30:22 +0900