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Systematic Variations in the Charge-Glass-Forming Ability of Geometrically Frustrated $theta$-(BEDT-TTF)$_2X$ Organic Conductors

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 Added by Fumitaka Kagawa
 Publication date 2014
  fields Physics
and research's language is English




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The critical cooling rate $R_{rm c}$ above which charge ordering is kinetically avoided upon cooling, which results in charge-glass formation, was investigated for the geometrically frustrated system $theta$-(BEDT-TTF)$_2X$. X-ray diffraction experiments revealed that $theta$-(BEDT-TTF)$_2$TlCo(SCN)$_4$ exhibits a horizontally charge-ordered state, and kinetic avoidance of this state requires rapid cooling of faster than 150 K/min. This value is markedly higher than that reported for two other isostructural $theta$-type compounds, thus demonstrating the lower charge-glass-forming ability of $X$ $=$ TlCo(SCN)$_4$. In accounting for the systematic variations of $R_{rm c}$ among the three $theta$-(BEDT-TTF)$_2X$, we found that stronger charge frustration leads to superior charge-glass former. Our results suggest that charge frustration tends to slow the kinetics of charge ordering.

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Using the Lanczos exact-diagonalization and density-matrix renormalization group methods, we study the extended Hubbard model at quarter filling defined on the anisotropic triangular lattice. We focus on charge ordering (CO) phenomena induced by onsite and intersite Coulomb interactions. We determine the ground-state phase diagram including three CO phases, i.e., diagonal, vertical, and three-fold CO phases, based on the calculated results of the hole density and double occupancy. We also calculate the dynamical density-density correlation functions and find possible coexistence of the diagonal and three-fold charge fluctuations in a certain parameter region where the onsite and intersite interactions compete. Furthermore, the characteristic features of the optical conductivity for each CO phase are discussed.
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In the most studied family of organic superconductors kappa-(BEDT-TTF)_2X, the BEDT-TTF molecules that make up the conducting planes are coupled as dimers. For some anions X, an antiferromagnetic insulator is found at low temperatures adjacent to superconductivity. With an average of one hole carrier per dimer, the BEDT-TTF band is effectively 1/2-filled. Numerous theories have suggested that fluctuations of the magnetic order can drive superconducting pairing in these models, even as direct calculations of superconducting pairing in monomer 1/2-filled band models find no superconductivity. Here we present accurate zero-temperature Density Matrix Renormalization Group (DMRG) calculations of a dimerized lattice with one hole per dimer. While we do find an antiferromagnetic state in our results, we find no evidence for superconducting pairing. This further demonstrates that magnetic fluctuations in the effective 1/2-filled band approach do not drive superconductivity in these and related materials.
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