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Structural Evolution of One-dimensional Spin Ladder Compounds Sr14-xCaxCu24O41 with Ca doping and Related Hole Redistribution Evidence

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 Added by Guochu Deng
 Publication date 2011
  fields Physics
and research's language is English




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Incommensurate crystal structures of spin ladder series Sr14-xCaxCu24O41 (x=3, 7, 11, 12.2) were characterized by powder neutron scattering method and refined using the superspace group Xmmm(00{gamma})ss0 (equivalent to superspace group Fmmm(0,0,1+{gamma})ss0); X stands for non-standard centering (0,0,0,0), (0,1/2,1/2,1/2), (1/2,1/2,0,0), (1/2,0,1/2,1/2)) with a modulated structure model. The Ca doping effects on the lattice parameters, atomic displacement, Cu-O distances, Cu-O bond angles and Cu bond valence sum were characterized. The refined results show that the CuO4 planar units in both chain and ladder sublattices become closer to square shape with an increase of Ca doping. The Cu bond valence sum calculation provided new evidence for the charge transfer from the chains to ladders (approximately 0.16 holes per Cu from x=0 to 12.2). The charge transfer was attributed to two different mechanisms: (a) the Cu-O bond distance shrinkage on the ladder; (b) increase of the interaction between two sublattices, resulting in Cu-O bonding between the chains and ladders. The low temperature structural refinement resulted in the similar conclusion, with a slight charge backflow to the chains.



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The spin ladder is a reduced-dimensional analogue of the high temperature superconductors that was predicted to exhibit both superconductivity and an electronic charge density wave or hole crystal (HC). Both phenomena have been observed in the doped spin ladder system Sr14-xCaxCu24O41 (SCCO), which at x=0 exhibits a HC which is commensurate at all temperatures. To investigate the effects of discommensuration we used resonant soft x-ray scattering (RSXS) to study SCCO as a function of doped hole density, d. The HC forms only with the commensurate wave vectors L_L = 1/5 and L_L = 1/3 and exhibits a simple temperature scaling T_(1/3) / T_(1/5) = 5/3. For irrational wave vectors the HC melts, perhaps through the motion of topological defects carrying fractional charge.
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We report the results of a ^63Cu and ^17O NMR study of the nuclear quadrupole interaction tensor, ^(17,63)nu_{Q,alpha}, in the hole doped spin ladder system Sr_(14-x)Ca_xCu_24O_41 (x = 0 and 12) performed under ambient and high pressures. NMR data show that the hole density in the Cu_2O_3 ladder layer grows with temperature, Ca content and an applied pressure. We have derived the hole occupation of Cu 3d and O 2p orbitals at the different ion sites in the Cu_2O_3 ladder as a function of the temperature, Ca substitution and pressure. We also suggest that the most important role of high pressure for the stabilization of a superconducting ground state in Ca-rich two-leg ladders is an increase of the hole concentration in the conducting Cu_2O_3 planes. We have obtained an estimate of 0.10 hole per Cu1 for the hole concentration at low temperature in Ca12 under 32 kbar when this compound undergoes a superconducting transition at 5K. Such a value fits fairly well with the doping phase diagram of cuprate superconductors.
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