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Published on: July 4, 2016
Supramolecular Ion-Channel Engineering of Spin-Charge Coexistence in a [Ni(dmit)2] Conductor Hosting Mixed-Valence Mn
Daisuke Ishikawa1, Jun Manabe1, Masato Haneda1
1Department of Chemistry, Graduate School of Advanced Science and Engineering, Hiroshima University, 1-3-1, Kagamiyama, Higashi-hiroshima, Hiroshima 739-8526, Japan.
Abstract:
The interplay between electrical conduction and magnetism offers a powerful means to elucidate emergent mechanisms and control properties; however, realizing this in Ni(dmit)2 crystals has been challenging due to undesirable reactions among their components. Mn1.83([18]crown-6)3[Ni(dmit)2]11(H2O)7.33(CH3CN)2 (1) is prepared in the present study, integrating one-dimensional [18]crown-6 ion channels hosting mixed-valence Mn2+/Mn3+ with conducting [Ni(dmit)2] layers. Subsequently, a structure-driven mechanism of conductivity is clarified. In the crystal, [Ni(dmit)2] forms one-dimensional dimer-dimer-trimer-dimer-dimer stacks; weak interchain contacts generate two-dimensional sheets alternating with supramolecular channel layers. Mn ions occupy two partially populated sites and adopt seven-coordinate environments with two axial aqua ligands and five equatorial crown-ether oxygen. Magnetometry indicates Mn moments are effectively decoupled from the conducting [Ni(dmit)2] sublattice: the Mn sublattice follows Curie-Weiss behavior with an exceptionally small Weiss temperature, while the [Ni(dmit)2] stacks form S = 1/2 one-dimensional Heisenberg antiferromagnetic chains. Compound 1 exhibits high conductivity at 300 K and one-dimensional variable-range hopping, attributable to thermal fluctuations of the supramolecular channels that modulate intracolumn transfer integrals and promote carrier localization. To our knowledge, 1 is the first system combining transition-metal-ion [18]crown-6 channels with conducting [Ni(dmit)2] layers, establishing a supramolecular route to tune spin-charge coexistence via host design.
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