Crystal Structure and Magnetic Properties of an Organic Ion-Radical Salt: [3,3′-Dimethyl-2,2′-Thiazolinocyanine]2-[TCNQ]3

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A new organic ion-radical salt, [3,3′-dimethyl-2,2′-thiazolinocyanine]2-[TCNQ]3 which is simply written by [DMTzNc]2-[TCNQ]3, is synthesized and the crystallographic and magnetic properties are investigated. This salt forms triclinic crystal in the space group P\bar1 with a=9.976(3), b=16.129(5), c=8.371(2) Å, α=101.80(3), β=106.02(3), γ=77.02(3)° and Z=2. The planar TCNQ molecules are stacked face-to-face to form a column parallel to the a-axis with two unpaired electrons per three TCNQ molecules. The magnetic susceptibility and ESR are measured. The unpaired electrons on the TCNQ column form the spin-pair state with the exchange energy of 500 K below about 200 K. The localized spin-pair decouples with increasing temperature and the one-dimensional spin correlation appears on the TCNQ column accompanying with the increases in the magnetic susceptibility and the electrical conductivity.
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