The Electrical and Magnetic Properties of a Novel Two-Dimensional Antiferromagnet Based on BEDT–TTF: θ-(BEDT–TTF)2Cu2(CN)[N(CN)2]2

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Abstract
A crystal-structure analysis and a band calculation, as well as conductivity, thermoelectric power, ESR, and static susceptibility measurements were performed on the new BEDT–TTF salt, θ-(BEDT–TTF)2Cu2(CN)[N(CN)2]2. This salt has a unique polymerized anion comprising infinite Cu–N(CN)2–Cu double helices bridged by disordered CN groups. Although the two-dimensional arrangement of crystallographically equivalent BEDT–TTF+0.5 cations provides a two-dimensional closed Fermi surface within the tight-binding approximation, this salt is semiconductive even at room temperature, probably due to a strong electron correlation in this system. A semiconductor–semiconductor transition has been observed around 220 K. Below 220 K the electronic system is represented as a Mott insulator and a two-dimensional Heisenberg antiferromagnet. Rapid decreases in the ESR line width and spin susceptibility below 50 K indicate the existence of an additional magnetic transition.

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