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説明:

Controlling spin states at the single-molecule level is a crucial step toward functional molecular spintronic devices. Au porphyrins, as efficient electron acceptors, are highly sensitive to charge transfer on surfaces and offer a promising route to investigate spin-state modulation in single-molecule magnets. Here, we report the synthesis of phenalenyl-expanded Au porphyrins via cyclodehydrogenation on Au(111). The atomic-scale structures, electronic properties, and spin states of the products were investigated in detail with a combination of noncontact atomic force microscopy, scanning tunneling microscopy, scanning tunneling spectroscopy, as well as density functional theory and multireference quantum chemistry calculations. Although the structures are nearly identical, the spin states of the porphyrins are significantly affected by the charge state of the Au complex. Our findings show that the role of the molecule–substrate interactions and the resulting charge transfer of the gold complex tune the spin and electronic properties of the extended porphyrins, establishing them as versatile molecular platforms for investigating charge-transfer-driven spin switches and guiding the design of molecular spintronic devices.

権利情報:

• Creative Commons BY Attribution 4.0 International
  

キーワード: scanning tunneling microscopy, noncontact atomic force microscopy, single-molecule spintronics, Au porphrins, spin-state modulation, molecule magnets, density functional theory

刊行年月日: 2026-04-08

出版者: American Chemical Society (ACS)

掲載誌:

• Journal of the American Chemical Society (ISSN: 00027863) vol. 148 issue. 13 p. 13863-13870

研究助成金:

• Japan Society for the Promotion of Science 24K21721
• Japan Society for the Promotion of Science 24KF0269
• Japan Society for the Promotion of Science 25H00422
• Japan Society for the Promotion of Science JP20H05863
• Japan Society for the Promotion of Science JP23K17951
• Japan Society for the Promotion of Science JP23K23335
• MEYS CR(LM2023051) GACR25-17866X
• the European Union under the Marie Sklodowska-Curie Actions Grant Agreement No. 101203634
• TERAFIT project CZ.02.01.01/00/22_008/0004594

原稿種別: 出版者版 (Version of record)

MDR DOI:

公開URL: https://doi.org/10.1021/jacs.5c21710

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更新時刻: 2026-04-09 15:00:14 +0900

MDRでの公開時刻: 2026-04-09 16:22:30 +0900