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The magnetic state of the single-component molecular compound, [Cu(tmdt)], is investigated by means of H-NMR. An abrupt spectral broadening below 13 K and a sharp peak in nuclear spin-lattice relaxation rate, , at 13 K are observed as clear manifestations of a second-order antiferromagnetic transition, which is consistent with the previously reported magnetic susceptibility and EPR measurement. The ordered moment is estimated at /molecule. The temperature-dependence of above the transition temperature indicates one-dimensional spin dynamics and supports that the spins are on the central part of the molecule differently from other isostructural compounds.

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