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説明:

Synthesis of one-dimensional molecular arrays with tailored stereoisomers is challenging yet has great potential for application in molecular opto-, electronic- and magnetic-devices, where the local array structure plays a decisive role in the functional properties. Here, we demonstrate the construction and characterization of dehydroazulene isomer and diradical units in three-dimensional organometallic compounds on Ag(111) with a combination of low-temperature scanning tunneling microscopy and density functional theory calculations. Tip-induced voltage pulses firstly result in the formation of a diradical species via successive homolytic fission of two C-Br bonds in the naphthyl groups, which are subsequently transformed into chiral dehydroazulene moieties. The delicate balance of the reaction rates among the diradical and two stereoisomers, arising from an in-line configuration of tip and molecular unit, allows directional azulene-to-azulene and azulene-to-diradical local probe structural isomerization in a controlled manner. Furthermore, our theoretical calculations suggest that the diradical moiety hosts an open-shell singlet with antiferromagnetic coupling between the unpaired electrons, which can undergo an inelastic spin transition of 91 meV to the ferromagnetically coupled triplet state.

権利情報:

キーワード: local probe, isomerization, molecular array

刊行年月日: 2023-11-25

出版者: Springer Science and Business Media LLC

掲載誌:

• Nature Communications (ISSN: 20411723) vol. 14 7741

研究助成金:

• JSPS JP22H00285
• Academy of Finland 346824

原稿種別: 出版者版 (Version of record)

MDR DOI:

公開URL: https://doi.org/10.1038/s41467-023-43659-4

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更新時刻: 2024-01-05 22:11:50 +0900

MDRでの公開時刻: 2023-12-28 16:30:31 +0900