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Register a new user$^{13}$C NMR Study on the Charge-Disproportionated Conducting State in the Quasi-Two-Dimensional Organic Conductor $alpha$-(BEDT-TTF)$_2$I$_3$
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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.
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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.
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 proportional 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.
To verify the effect of geometrical frustration, we artificially distort the triangular lattice of quasi-two-dimensional organic conductor $kappa$-(BEDT-TTF)$_2$Cu$_2$(CN)$_3$ [BEDT-TTF: bis(ethylenedithio)terathiofulvalene] by analogous-molecular substitution and apply $^{13}$C NMR of bulk and substituted sites, electric conductivity, and static magnetic susceptibility measurements. The results indicate that the magnetic characteristics of the substituted sample are quantitatively similar to those of the pure sample. Moreover the magnetic characteristics at the substituted sites are also the same as in the bulk. These results suggest that the observed magnetic properties may not be due to the geometrical frustration but the importance of disorder.
The ground state of $lambda$-(BEDT-TTF)$_2$GaCl$_4$, which has the same structure as the organic superconductor $lambda$-(BETS)$_2$GaCl$_4$, was investigated by magnetic susceptibility and $^{13}$C NMR measurements. The temperature dependence of the magnetic susceptibility revealed an antiferromagnetic (AF) correlation with $J/k_{rm B} simeq$ 98 K. NMR spectrum splitting and the divergence of $1/T_1$ were observed at approximately 13 K, which is associated with the AF transition. We found that the AF structure is commensurate according to discrete NMR peak splitting, suggesting that the ground state of $lambda$-(BEDT-TTF)$_2$GaCl$_4$ is an AF dimer-Mott insulating state. Our results suggest that the superconducting phase of $lambda$-type salts would be located near the AF insulating phase.
(BEDT-TFF)$_2$I$_3$ charge transfer salts are reported to show superconductivity and pressure induced quasi two-dimensional Dirac cones at the Fermi level. By performing state of the art ab initio calculations in the framework of density functional theory, we investigate the structural and electronic properties of the three structural phases $alpha$, $beta$ and $kappa$. edit{We furthermore report about the irreducible representations of the corresponding electronic band structures, symmetry of their crystal structure, and discuss the origin of band crossings. Additionally, we discuss the chemically induced strain in $kappa$-(BEDT-TTF)$_2$I$_3$ achieved by replacing the Iodine layer with other Halogens: Fluorine, Bromine and Chlorine. In the case of $kappa$-(BEDT-TTF)$_2$F$_3$, we identify topologically protected crossings within the band structure. These crossings are forced to occur due to the non-symmorphic nature of the crystal.} The calculated electronic structures presented here are added to the organic materials database (OMDB).
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