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Magnetic properties of honeycomb-based spin models in verdazyl-based salts
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DOI：10.1103/PhysRevMaterials.3.064410.png)
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Abstract
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We successfully synthesized the verdazyl-based salts (m-MePy-V)(2)Fe2OCl6 and [m-MePy-V-(p-Cl)(2)](2)Fe2OCl6 center dot (CH3CN)(2) with different Fe2OCl62- structures. The exchange interactions between Fe3+ ions in the Fe2OCl62- anions were evaluated to be nearly equivalent and to form an S = 5/2 antiferromagnetic (AF) dimer in each salt. We obtained the magnetic susceptibility of S = 1/2 spins on the radical by subtracting the contribution of S = 5/2 spins in the anion from the observed magnetic susceptibility. For (m-MePy-V)(2)Fe2OCl6, ab initio molecular orbital (MO) calculations indicated that the S = 1/2 AF dimers are weakly connected by ferromagnetic interactions, thereby forming a honeycomb lattice. The experimentally measured magnetic susceptibility and specific heat indicate a corresponding nonmagnetic gapped behavior. For [m-MePy-V-(p-Cl)(2)](2)Fe2OCl6 center dot (CH3CN)(2), MO calculations indicated that four types of dominant interactions form an unconventional S = 1/2 honeycomb-based 3D spin model. The magnetic susceptibility and specific heat indicate a phase transition to a 3D order at approximately 4.8 K.
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