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Register a new userA common behavior of thermoelectric layered cobaltites: incommensurate spin density wave states in [Ca$_2$Co$_{4/3}$Cu$_{2/3}$O$_4$]$_{0.62}$[CoO$_2$] and [Ca$_2$CoO$_3$]$_{0.62}$[CoO$_2$]
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Magnetism of a misfit layered cobaltite [Ca$_2$Co$_{4/3}$Cu$_{2/3}$O$_4$]$_x^{rm RS}$[CoO$_2$] ($x sim$ 0.62, RS denotes a rocksalt-type block) was investigated by a positive muon spin rotation and relaxation ($mu^+$SR) experiment. A transition to an incommensurate ({sf IC}) spin density wave ({sf SDW}) state was found below 180 K (= $T_{rm C}^{rm on}$); and a clear oscillation due to a static internal magnetic field was observed below 140 K (= $T_{rm C}$). Furthermore, an anisotropic behavior of the zero-field $mu^+$SR experiment indicated that the {sf IC-SDW} propagates in the $a$-$b$ plane, with oscillating moments directed along the c axis. These results were quite similar to those for the related compound [Ca$_2$CoO$_3$]$_{0.62}^{rm RS}$[CoO$_2$], {sl i.e.}, Ca$_3$Co$_4$O$_9$. Since the {sf IC-SDW} field in [Ca$_2$Co$_{4/3}$Cu$_{2/3}$O$_4$]$_{0.62}^{rm RS}$[CoO$_2$] was approximately same to those in pure and doped [Ca$_2$CoO$_3$]$_{0.62}^{rm RS}$[CoO$_2$], it was concluded that the {sf IC-SDW} exist in the [CoO$_2$] planes.
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[Ca$_2$CoO$_3$]$_{0.62}$[CoO$_2$], a two dimensional misfit metallic compound, is famous for its rich phases accessed by temperature, $i.e.$ high temperature spin-state transition, metal-insulator transition (MIT) at intermediate temperature ($sim$ 100 K) and low temperature spin density wave (SDW). It enters into SDW phase below T$_{MIT}$ which becomes long range at 27 K. Information on the independent role of misfit layers (rocksalt/Ca$_2$CoO$_3$ & triangular/CoO$_2$) in these phases is scarce. By combining a set of complementary macroscopic (DC magnetization and resistivity) and microscopic (neutron diffraction and X-ray absorption fine structure spectroscopy) measurements on pure (CCO) and Tb substituted in the rocksalt layer of CCO (CCO1), magnetic correlations in both subsystems of this misfit compound are unraveled. CCO is found to exhibit glassiness, as well as exchange bias (EB) effects, while CCO1 does not exhibit glassiness, albeit it shows weaker EB effect. By combining local structure investigations from extended X-ray absorption fine structure (EXAFS) spectroscopy and neutron diffraction results on CCO, we confirm that the SDW arises in the CoO$_2$ layer. Our results show that the magnetocrystalline anisotropy associated with the rocksalt layer acts as a source of pinning, which is responsible for EB effect. Ferromagnetic clusters in the Ca$_2$CoO$_3$ affects SDW in CoO$_2$ and ultimately glassiness arises.
Layered misfit cobaltate [Ca$_2$CoO$_3$]$_{0.62}$[CoO$_2$], which emerged as an important thermoelectric material~[A. C. Masset et al. Phys. Rev. B, 62, 166 (2000)], has been explored extensively in the last decade for the exact mechanism behind its high Seebeck coefficient. Its complex crystal and electronic structures have inhibited consensus among such investigations. This situation has arisen mainly due to difficulties in accurate identification of the chemical state, spin state, and site symmetries in its two subsystems (rocksalt [Ca$_2$CoO$_3$] and triangular [CoO$_2$]). By employing resonant photoemission spectroscopy and x-ray absorption spectroscopy along with charge transfer multiplet simulations (at the Co ions), we have successfully identified the site symmetries, valencies and spin states of the Co in both layers. Our site-symmetry observations explain the experimental value of the high Seebeck coefficient and also confirm that the carriers hop within the rocksalt layer, which is in contrast to earlier reports where hopping within triangular CoO$_2$ layer has been held responsible for the large Seebeck coefficient.
Transport property is investigated in [Ca$_{2}$CoO$_{3-delta}$]$_{0.62}$[CoO$_{2}$] single crystals obtained by varying annealing conditions. The $rho_{ab}(T)$ exhibits a resistivity minimum, and the temperature corresponding to this minimum increases with the loss of oxygen content, indicative of the enhancement of spin density wave (SDW). Large negative magnetoresistance (MR) was observed in all single crystals [Ca$_{2}$CoO$_{3-delta}$]$_{0.62}$[CoO$_{2}$], while a magnetic-field-driven insulator-to-metal (IM) transition in oxygen annealed samples. These results suggest a ferromagnetic correlation in system enhanced by oxygen content. In addition, a low temperature thermal activation resistivity induced by fields was observed in single crystals annealed in oxygen atmosphere.
The single electron tunneling spectroscopy on superconductor Na$_{x}$CoO$_2$$cdot$ yH$_2$O and its starting compound Na$_{x}$CoO$_2$ has been studied with point-contact method. The spectra of Na$_{x}$CoO$_2$ have two types of distinct shapes at different random locations, this is attributed to the non-uniformly distributed sodium escaped from the inner part of the sample. While all the measured spectra of the superconducting samples Na$_{x}$CoO$_2$$cdot$ yH$_2$O have a good spatial reproducibility, and show a remarkable zero bias conductance depression appearing below an onset temperature which associates very well with the resistance upturn at around 45 K. The latter behavior resembles in some way the pseudogap feature in high-T$_c$ cuprate uperconductors.
With x-ray absorption spectroscopy we investigated the orbital reconstruction and the induced ferromagnetic moment of the interfacial Cu atoms in YBa$_2$Cu$_3$O$_{7}$/La$_{2/3}$Ca$_{1/3}$MnO$_3$ (YBCO/LCMO) and La$_{2-x}$Sr$_{x}$CuO$_4$/La$_{2/3}$Ca$_{1/3}$MnO$_3$ (LSCO/LCMO) multilayers. We demonstrate that these electronic and magnetic proximity effects are coupled and are common to these cuprate/manganite multilayers. Moreover, we show that they are closely linked to a specific interface termination with a direct Cu-O-Mn bond. We furthermore show that the intrinsic hole doping of the cuprate layers and the local strain due to the lattice mismatch between the cuprate and manganite layers are not of primary importance. These findings underline the central role of the covalent bonding at the cuprate/manganite interface in defining the spin-electronic properties.
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