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Temperature dependence of spherical electron transfer in a nanosized [Fe14] complex

DOI: 10.1038/s41467-019-13279-y DOI Help

Authors: Wei Huang (Changzhou University) , Shuqi Wu (Kyushu University) , Xiangwei Gu (Changzhou University) , Yao Li (Changzhou University) , Atsushi Okazawa (The University of Tokyo) , Norimichi Kojima (Toyota Physical and Chemical Research Institute) , Shinya Hayami (Kumamoto University) , Michael L. Baker (The University of Manchester) , Peter Bencok (Diamond Light Source) , Mariko Noguchi (Osaka University; Nihon University) , Yuji Miyazaki (Osaka University) , Motohiro Nakano (Osaka University) , Takumi Nakanishi (Kyushu University) , Shinji Kanegawa (Kyushu University) , Yuji Inagaki (Kyushu University) , Tatsuya Kawae (Kyushu University) , Gui-lin Zhuang (Zhejiang University of Technology) , Yoshihito Shiota (Kyushu University) , Kazunari Yoshizawa (Kyushu University) , Dayu Wu (Changzhou University) , Osamu Sato (Kyushu University)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Nature Communications , VOL 10

State: Published (Approved)
Published: December 2019
Diamond Proposal Number(s): 17723

Open Access Open Access

Abstract: The study of transition metal clusters exhibiting fast electron hopping or delocalization remains challenging, because intermetallic communications mediated through bridging ligands are normally weak. Herein, we report the synthesis of a nanosized complex, [Fe(Tp)(CN)3]8[Fe(H2O)(DMSO)]6 (abbreviated as [Fe14], Tp−, hydrotris(pyrazolyl)borate; DMSO, dimethyl sulfoxide), which has a fluctuating valence due to two mobile d-electrons in its atomic layer shell. The rate of electron transfer of [Fe14] complex demonstrates the Arrhenius-type temperature dependence in the nanosized spheric surface, wherein high-spin centers are ferromagnetically coupled, producing an S = 14 ground state. The electron-hopping rate at room temperature is faster than the time scale of Mössbauer measurements (<~10−8 s). Partial reduction of N-terminal high spin FeIII sites and electron mediation ability of CN ligands lead to the observation of both an extensive electron transfer and magnetic coupling properties in a precisely atomic layered shell structure of a nanosized [Fe14] complex.

Journal Keywords: Materials science; Organic–inorganic nanostructures; Organometallic chemistry

Subject Areas: Chemistry, Physics, Materials

Instruments: I10-Beamline for Advanced Dichroism