Electronic State of a Conducting Single Molecule Magnet Based on Mn-salen Type and Ni-Dithiolene Complexes

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  • Kazuya Kubo
    Department of Chemistry, Graduate School of Science, Tohoku University, 6-3, Aramaki-Aza-Aoba, Aoba-Ku, Sendai, 980-8578 Miyagi, Japan
  • Takuya Shiga
    Department of Chemistry, Graduate School of Science, Tohoku University, 6-3, Aramaki-Aza-Aoba, Aoba-Ku, Sendai, 980-8578 Miyagi, Japan
  • Takashi Yamamoto
    Department of Chemistry, Graduate school of Science, Osaka University, 1-1, Machikaneyama, Toyonaka, 560-0043 Osaka, Japan
  • Akiko Tajima
    RIKEN, 2-1, Hirosawa, Wako-shi, Saitama 351-0198, Japan
  • Taro Moriwaki
    JASRI/SPring-8, 1-1-1, Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5198, Japan
  • Yuka Ikemoto
    JASRI/SPring-8, 1-1-1, Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5198, Japan
  • Masahiro Yamashita
    Department of Chemistry, Graduate School of Science, Tohoku University, 6-3, Aramaki-Aza-Aoba, Aoba-Ku, Sendai, 980-8578 Miyagi, Japan
  • Elisa Sessini
    Dipartimento di Chimica Inorganica ed Analitica, Universita di Cagliari, Cittadella di Monserrato, I-09042 Monserrato, Cagriari, Italy
  • Maria Laura Mercuri
    Dipartimento di Chimica Inorganica ed Analitica, Universita di Cagliari, Cittadella di Monserrato, I-09042 Monserrato, Cagriari, Italy
  • Paola Deplano
    Dipartimento di Chimica Inorganica ed Analitica, Universita di Cagliari, Cittadella di Monserrato, I-09042 Monserrato, Cagriari, Italy
  • Yasuhiro Nakazawa
    Department of Chemistry, Graduate school of Science, Osaka University, 1-1, Machikaneyama, Toyonaka, 560-0043 Osaka, Japan
  • Reizo Kato
    RIKEN, 2-1, Hirosawa, Wako-shi, Saitama 351-0198, Japan

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説明

The electrochemical oxidation of an acetone solution containing [Mn(III) (5-MeOsaltmen)(H(2)O)](2)(PF(6))(2) (5-MeOsaltmen(2-) = N,N'-(1,1,2,2-tetramethylethylene)bis(5-methoxysalicylideneiminate)) and (NBu(4))[Ni(dmit)(2)] (dmit(2-) = 2-thioxo-1,3-dithiole-4,5-dithiolate) afforded a hybrid material, [Mn(5-MeOsaltmen)(acetone)](2)[Ni(dmit)(2)](6) (1), in which [Mn(2)](2+) single-molecule magnets (SMMs) with an S(T) = 4 ground state and [Ni(dmit)(2)](n-) molecules in a charge-ordered state (n = 0 or 1) are assembled in a layer-by-layer structure. Compound 1 crystallizes in the triclinic space group P1 with an inversion center at the midpoint of the Mn···Mn dimer. The [Mn(2)](2+) unit has a typical nonplanar Mn(III) dimeric core and is structurally consistent with previously reported [Mn(2)] SMMs. The six [Ni(dmit)(2)](n-) (n = 0 or 1) units have a square-planar coordination geometry, and the charge ordering among them was assigned on the basis of ν(C═C) in IR reflectance spectra (1386, 1356, 1327, and 1296 cm(-1)). The [Mn(2)](2+) SMM and [Ni(dmit)(2)](n-) units aggregate independently to form hybrid frames. Electronic conductivity measurements revealed that 1 behaved as a semiconductor (ρ(rt) = 2.1 × 10(-1) Ω·cm(-1), E(a) = 97 meV) at ambient pressure and as an insulator at 1.7 GPa (ρ(1.7GPa) = 4.5 Ω·cm(-1), E(a) = 76 meV). Magnetic measurements indicated that the [Mn(2)](2+) units in 1 behaved as S(T) = 4 SMMs at low temperatures.

収録刊行物

  • Inorganic Chemistry

    Inorganic Chemistry 50 (19), 9337-9344, 2011-09-02

    American Chemical Society (ACS)

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