Emergence of inhomogeneous moments from spin liquid in the triangular-lattice Mott insulator κ\kappa-(ET)2_2Cu2_2(CN)3_3

The static and dynamic local spin susceptibility of the organic Mott insulator $\kappa$-(ET)$_2$Cu$_2$(CN)$_3$, a model material of the spin- 1/2 triangular lattice, is studied by $^{13}$C NMR spectroscopy from room temperature down to 20 mK. We observe an anomalous field-dependent spectral broadening with the continuous and bipolar shift distribution, appearing without the critical spin fluctuations. It is attributable to spatially nonuniform magnetizations induced in the spin liquid under magnetic fields. The amplitude of the magnetization levels off below 1 K, while the low-lying spin fluctuations survive toward the ground state, as indicated by the temperature profile of the relaxation rates.Comment: 4 pages, 4 figure

Spin Liquid State in an Organic Mott Insulator with Triangular Lattice

$^{1}$H NMR and static susceptibility measurements have been performed in an organic Mott insulator with nearly isotropic triangular lattice, $\kappa$-(BEDT-TTF)$_{2}$Cu$_{2}$(CN)$_{3}$, which is a model system of frustrated quantum spins. The static susceptibility is described by the spin $S$ = 1/2 antiferromagnetic triangular-lattice Heisenberg model with the exchange constant $J$ $\sim$ 250 K. Regardless of the large magnetic interactions, the $^{1}$H NMR spectra show no indication of long-range magnetic ordering down to 32 mK, which is four-orders of magnitude smaller than $J$. These results suggest that a quantum spin liquid state is realized in the close proximity of the superconducting state appearing under pressure.Comment: 4 pages, 4 figure

Theory of the beta-type Organic Superconductivity under Uniaxial Compression

We study theoretically the shift of the superconducting transition temperature (Tc) under uniaxial compression in beta-type organic superconductors, beta-(BEDT-TTF)2I3 and beta-(BDA-TTP)2X[X=SbF6,AsF6], in order to clarify the electron correlation, the spin frustration and the effect of dimerization. The transfer integrals are calculated by the extended Huckel method assuming the uniaxial strain and the superconducting state mediated by the spin fluctuation is solved using Eliashberg's equation with the fluctuation-exchange approximation. The calculation is carried out on both the dimerized (one-band) and nondimerized (two-band) Hubbard models. We have found that (i) the behavior of Tc in beta-(BEDT-TTF)2I3 with a stronger dimerization is well reproduced by the dimer model, while that in weakly dimerized beta-BDA-TTP salts is rather well reproduced by the two-band model, and (ii) the competition between the spin frustration and the effect induced by the fluctuation is important in these materials, which causes nonmonotonic shift of Tc against uniaxial compression.Comment: 18 pages, 16 figures, 2 tabl

Enhancing Tc in field-doped Fullerenes by applying uniaxial stress

Capitalizing on the two-dimensional nature of superconductivity in field-effect doped C60, we show that it should be possible to increase the transition temperature Tc by applying uniaxial stress perpendicular to the gate electrode. This method not only holds the promise of substantially enhancing Tc (by about 30 K per GPa), but also provides a sensitive check of the current understanding of superconductivity in the doped Fullerenes.Comment: 3 pages RevTe

Electric Conductivity of the Zero-gap Semiconducting State in Alpha-(BEDT-TTF)2I3 Salt

The electric conductivity which reveals the zero gap semiconducting (ZGS) state has been investigated as the function of temperature $T$ and life time $\tau$ in order to understand the ZGS state in quarter-filled $\alpha$-(BEDT-TTF)$_2$I$_3$ salt with four sites in the unit cell. By treating $\tau$ as a parameter and making use of the one-loop approximation, it is found that the conductivity is proportional to $T$ and $\tau$ for $k_B\gg\hbar/\tau$ and independent of $T$ and $\tau$ for $k_B T\ll\hbar/\tau$. Further the conductivity being independent of $T$ in the ZGS state is examined in terms of Born approximation for the impurity cattering.Comment: 5 pages, 4 figures, submitted to J. Phys. Soc. Jp

Multi-Orbital Molecular Compound (TTM-TTP)I_3: Effective Model and Fragment Decomposition

The electronic structure of the molecular compound (TTM-TTP)I_3, which exhibits a peculiar intra-molecular charge ordering, has been studied using multi-configuration ab initio calculations. First we derive an effective Hubbard-type model based on the molecular orbitals (MOs) of TTM-TTP; we set up a two-orbital Hamiltonian for the two MOs near the Fermi energy and determine its full parameters: the transfer integrals, the Coulomb and exchange interactions. The tight-binding band structure obtained from these transfer integrals is consistent with the result of the direct band calculation based on density functional theory. Then, by decomposing the frontier MOs into two parts, i.e., fragments, we find that the stacked TTM-TTP molecules can be described by a two-leg ladder model, while the inter-fragment Coulomb energies are scaled to the inverse of their distances. This result indicates that the fragment picture that we proposed earlier [M.-L. Bonnet et al.: J. Chem. Phys. 132 (2010) 214705] successfully describes the low-energy properties of this compound.Comment: 5 pages, 4 figures, published versio

Magnetic Fluctuations in a Charge Ordered State of the One-Dimensional Extended Hubbard Model with a Half-Filled Band

Magnetic properties in a charge ordered state are examined for the extended Hubbard model at half-filling. Magnetic excitations, magnetic susceptibilities and a nuclear spin relaxation rate are calculated with taking account of fluctuations around the mean-field solution. The relevance of the present results to the observation in the 1:1 organic conductors, (TTM-TTP)I$_3$, is discussed.Comment: 4 pages, 3 figures, to be published in J. Phys. Soc. Jpn. Vol.71 (2002) No.

Effects of Next-Nearest-Neighbor Repulsion on One-Dimensional Quarter-Filled Electron Systems

We examine effects of the next-nearest-neighbor repulsion on electronic states of a one-dimensional interacting electron system which consists of quarter-filled band and interactions of on-site and nearest-neighbor repulsion. We derive the effective Hamiltonian for the electrons around wave number \pm \kf (\kf: Fermi wave number) and apply the renormalization group method to the bosonized Hamiltonian. It is shown that the next-nearest-neighbor repulsion makes 4\kf-charge ordering unstable and suppresses the spin fluctuation. Further the excitation gaps and spin susceptibility are also evaluated.Comment: 19 pages, 8 figures, submitted to J. Phys. Soc. Jp

de Haas-van Alphen Effect in the Two-Dimensional and the Quasi-Two-Dimensional Systems

We study the de Haas-van Alphen (dHvA) oscillation in two-dimensional and quasi-two-dimensional systems. We give a general formula of the dHvA oscillation in two-dimensional multi-band systems. By using this formula, the dHvA oscillation and its temperature-dependence for the two-band system are shown. By introducing the interlayer hopping $t_z$, we examine the crossover from the two-dimension, where the oscillation of the chemical potential plays an important role in the magnetization oscillation, to the three-dimension, where the oscillation of the chemical potential can be neglected as is well know as the Lifshitz and Kosevich formula. The crossover is seen at $4 t_z \sim 8 ta b H /\phi_0$, where a and b are lattice constants, $\phi_0$ is the flux quantum and 8t is the width of the total energy band. We also study the dHvA oscillation in quasi-two-dimensional magnetic breakdown systems. The quantum interference oscillations such as $\beta-\alpha$ oscillation as well as the fundamental oscillations are suppressed by the interlayer hopping $t_z$, while the $\beta+\alpha$ oscillation gradually increases as $t_z$ increases and it has a maximum at $t_z/t\approx 0.025$. This interesting dependence on the dimensionality can be observed in the quasi-two-dimensional organic conductors with uniaxial pressure.Comment: 11 pages, 14 figure

Evidence for structural and electronic instabilities at intermediate temperatures in κ\kappa-(BEDT-TTF)2_{2}X for X=Cu[N(CN)2_{2}]Cl, Cu[N(CN)2_{2}]Br and Cu(NCS)2_{2}: Implications for the phase diagram of these quasi-2D organic superconductors

We present high-resolution measurements of the coefficient of thermal expansion $\alpha (T)=\partial \ln l(T)/\partial T$ of the quasi-twodimensional (quasi-2D) salts $\kappa$-(BEDT-TTF)$_2$X with X = Cu(NCS)$_2$, Cu[N(CN)$_2$]Br and Cu[N(CN)$_2$]Cl. At intermediate temperatures (B), distinct anomalies reminiscent of second-order phase transitions have been found at $T^\ast = 38$ K and 45 K for the superconducting X = Cu(NCS)$_2$ and Cu[N(CN)$_2$]Br salts, respectively. Most interestingly, we find that the signs of the uniaxial pressure coefficients of $T^\ast$ are strictly anticorrelated with those of $T_c$. We propose that $T^\ast$ marks the transition to a spin-density-wave (SDW) state forming on minor, quasi-1D parts of the Fermi surface. Our results are compatible with two competing order parameters that form on disjunct portions of the Fermi surface. At elevated temperatures (C), all compounds show $\alpha (T)$ anomalies that can be identified with a kinetic, glass-like transition where, below a characteristic temperature $T_g$, disorder in the orientational degrees of freedom of the terminal ethylene groups becomes frozen in. We argue that the degree of disorder increases on going from the X = Cu(NCS)$_2$ to Cu[N(CN)$_2$]Br and the Cu[N(CN)$_2$]Cl salt. Our results provide a natural explanation for the unusual time- and cooling-rate dependencies of the ground-state properties in the hydrogenated and deuterated Cu[N(CN)$_2$]Br salts reported in the literature.Comment: 22 pages, 7 figure