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The magnetic state of the single-component molecular compound, [Cu(tmdt)$_{2}$], is investigated by means of $^{1}$H-NMR. An abrupt spectral broadening below 13 K and a sharp peak in nuclear spin-lattice relaxation rate, $T_{1}^{-1}$, at 13 K are obs erved 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 $0.22-0.45$ ${mu}_{rm B}$/molecule. The temperature-dependence of $T_{1}^{-1}$ 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.
We report a $^{13}$C-NMR study on the ambient-pressure metallic phase of the layered organic conductor $theta$-(BEDT-TTF)$_{2}$I$_{3}$ [BEDT-TTF: bisethylenedithio-tetrathiafulvalene], which is expected to connect the physics of correlated electrons and Dirac electrons under pressure. The orientation dependence of the NMR spectra shows that all BEDT-TTF molecules in the unit cell are to be seen equivalent from a microscopic point of view. This feature is consistent with the orthorhombic symmetry of the BEDT-TTF sublattice and also indicates that the monoclinic $I_{3}$ sublattice, which should make three molecules in the unit cell nonequivalent, is not practically influential on the electronic state in the conducting BEDT-TTF layers at ambient pressure. There is no signature of charge disproportionation in opposition to most of the $theta$-type BEDT-TTF salts. The analyses of NMR Knight shift, $K$, and the nuclear spin-lattice relaxation rate, $1/T_{1}$, revealed that the degree of electron correlation, evaluated by the Korringa ratio [$varpropto 1/(T_{1}TK^{2}$)], is in an intermediate regime. However, NMR relaxation rate $1/T_{1}$ is enhanced above $sim$ 200K, which possibly indicates that the system enters into a quantum critical regime of charge-order fluctuations as suggested theoretically.
The conducting state of the quasi-two-dimensional organic conductor, $alpha$-(BEDT-TTF)$_2$I$_3$, at ambient pressure is investigated with $^{13}$C NMR measurements, which separate the local electronic states at three nonequivalent molecular sites (A , B, and C). The spin susceptibility and electron correlation effect are revealed in a locally resolved manner. While there is no remarkable site-dependence around room temperature, the local spin susceptibility gradually disproportionates among the nonequivalent sites with decreasing temperature. The disproportionation-ratio yields 5:4:6 for A:B:C molecules at 140 K. Distinct site- and temperature-dependences are also observed in the Korringa ratio, $mathcal{K}_i propto (1/T_{1}T)_iK^{-2}_i$ ($i$ = A, B, and C), which is a measure of the strength and the type of electron correlations. The values of $mathcal{K}_i$ point to sizable antiferromagnetic spin correlation. We argue the present results in terms of the theoretical prediction of the peculiar site-specific reciprocal-space ($bm{k}$-space) anisotropy on the tilted Dirac cone, and discuss the $bm{k}$-dependent profiles of the spin susceptibility and electron correlation on the cone.
We present the results of our $^{13}$C NMR study of the quasi-two-dimensional organic conductor $theta$-(BEDT-TTF)$_2$I$_{3}$ under pressure, which is suggested to be a zero-gap conductor by transport measurements. We found that NMR spin shift is pro portional to $T$ and that spin-lattice relaxation rate follows the power law $T^{alpha}$ ($alpha =3 sim 4$), where $T$ is the temperature. This behavior is consistent with the cone-like band dispersion and provides microscopic evidence for the realization of the zero-gap state in the present material under pressure.
271 - Y. Hara , K. Miyagawa , K. Kanoda 2008
We present the results of a ^{1}H NMR study of the single-component molecular conductor, [Au(tmdt)_{2}]. A steep increase in the NMR line width and a peak formation of the nuclear spin-lattice relaxation rate, 1/T_{1}, were observed at around 110 K . This behavior provides clear and microscopic evidences for a magnetic phase transition at considerably high temperature among organic conductors. The observed variation in 1/T_{1} with respect to temperature indicates the highly correlated nature of the metallic phase.
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