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Register a new userMagnetic and transport properties of the spin-state disordered oxide La0.8Sr0.2Co_{1-x}Rh_xO_{3-delta}
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We report measurements and analysis of magnetization, resistivity and thermopower of polycrystalline samples of the perovskite-type Co/Rh oxide La$_{0.8}$Sr$_{0.2}$Co$_{1-x}$Rh$_x$O$_{3-delta}$. This system constitutes a solid solution for a full range of $x$,in which the crystal structure changes from rhombohedral to orthorhombic symmetry with increasing Rh content $x$. The magnetization data reveal that the magnetic ground state immediately changes upon Rh substitution from ferromagnetic to paramagnetic with increasing $x$ near 0.25, which is close to the structural phase boundary. We find that one substituted Rh ion diminishes the saturation moment by 9 $mu_B$, which implies that one Rh$^{3+}$ ion makes a few magnetic Co$^{3+}$ ions nonmagnetic (the low spin state), and causes disorder in the spin state and the highest occupied orbital. In this disordered composition ($0.05le x le 0.75$), we find that the thermopower is anomalously enhanced below 50 K. In particular, the thermopower of $x$=0.5 is larger by a factor of 10 than those of $x$=0 and 1, and the temperature coefficient reaches 4 $mu$V/K$^2$ which is as large as that of heavy-fermion materials such as CeRu$_2$Si$_2$.
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We have demonstrated the effect of hydrostatic pressure on magnetic and transport properties, and thermal transport properties in electron-doped manganites CaMn$_{1-x}$Sb$_{x}$O$_{3}$. The substitution of Sb$^{5+}$ ion for Mn $^{4+}$site of the parent matrix causes one-electron doping with the chemical formula CaMn$^{4+}_{1-2x}$Mn$^{3+}_{x}$Sb$^{5+}_{x}$O$_{3}$ accompanied by a monotonous increase in unit cell volume as a function of $x$. Upon increasing the doping level of Sb, the magnitudes of both electrical resistivity and negative Seebeck coefficient are suppressed at high temperatures, indicating the electron doping. Anomalous diamagnetic behaviors at $x=0.05$ and 0.08 are clearly observed in field cooled dc magnetization. The effect of hydrostatic pressure on dc magnetization is in contrast to the chemical pressure effect due to Sb doping. The dynamical effect of ac magnetic susceptibility measurement points to the formation of the magnetically frustrated clusters such as FM clusters embedded in canted AFM matrix.
We present the first-principles investigation of the structural, electronic, and magnetic properties of SrCoO$_{3-delta}$ ($delta=0, 0.25, 0.5$) to understand the multivalent nature of Co ions in SrCoO$_{3-delta}$ along the line of topotactic transition between perovskite SrCoO$_{3}$ and brownmillerite SrCoO$_{2.5}$. From the on-site Coulomb interaction $U$-dependent ground state of stoichiometric SrCoO$_{3}$, we show the proximity of its metallic ferromagnetic ground state to other antiferromagnetic states. The structural and magnetic properties of SrCoO$_{3-delta}$ depending on their oxygen-content provide an interesting insight into the relationship between the Co-Co distances and the magnetic couplings so that the spin-state transition of Co spins can understood by the change of $pd$-hybridization depending on the Co-Co distances. The emph{strong} suppression of the $dpsigma$-hybridization between Co $d$ and O $p$ orbitals in brownmillerite SrCoO$_{2.5}$ brings on the high-spin state of Co$^{3+}$ $d^{6}$ and is responsible for the antiferromagnetically ordered insulating ground state. The increase of effective Co-Co distances driven by the presence of oxygen vacancies in SrCoO$_{3-delta}$ is consistent with the reduction of the effective $pd$-hybridization between Co $d$ and O $p$ orbitals. We conclude that the configuration of neighboring Co spins is shown to be crucial to their local electronic structure near the metal-to-insulator transition along the line of the topotactic transition in SrCoO$_{3-delta}$. Incidentally, we also find that the textit{I2mb} symmetry of SrCoO$_{2.5}$ is energetically stable and exhibits ferroelectricity via the ordering of CoO$_{4}$ tetrahedra, where this polar lattice can be stabilized by the presence of a large activation barrier.
Na-based osmium oxide pyrochlore was synthesized for the first time by an ion-exchange method. KOs2O6 was used as a host compound. Elelectron probe micro-analysis, synchrotron x-ray diffraction analysis, and thermo-gravimetric analysis confirmed its structure not as the beta-type but as the defect-type pyrochlore. The composition was identified as Na1.4Os2O6.H2O. Electrical resistivity, heat capacity, and magnetization measurements of the polycrystalline Na1.4Os2O6.H2O clarified absence of superconductivity above 2 K, being in contrast to what were found for the beta-pyrochlore AOs2O6 (A = Cs, Rb, K). Sommerfeld coefficient of 22 mJ K-2 mol-1 of Na1.4Os2O6.H2O was smallest among those of AOs2O6. A magnetic anomaly at ~57 K and possible associated magnetoresistance (+3.7 % at 2 K in 70 kOe) were found.
Neutron diffraction for a polycrystalline sample of LaCo$_{0.8}$Rh$_{0.2}$O$_{3}$ and synchrotron x-ray diffraction for polycrystalline samples of LaCo$_{0.9}$Rh$_{0.1}$O$_{3}$ and LaCo$_{0.8}$Rh$_{0.2}$O$_{3}$ have been carried out in order to investigate the structural properties related with the spin state of Co$^{3+}$ ions. We have found that the values of the Co(Rh)-O bond lengths in the Co(Rh)O$_{6}$ octahedron of LaCo$_{0.8}$Rh$_{0.2}$O$_{3}$ are nearly identical at 10 K. The lattice volume for the Rh$^{3+}$ substituted samples decreases with the thermal expansion coefficient similar to that of LaCoO$_{3}$ from room temperature, and ceases to decrease around 70 K. These experimental results favor a mixed state consisting of the high-spin-state and low-spin-state Co$^{3+}$ ions, and suggest that the high-spin-state Co$^{3+}$ ions are thermally excited in addition to those pinned by the substituted Rh$^{3+}$ ions.
Ba$_3$Mn$_2$O$_8$ is a geometrically frustrated spin dimer compound. We investigate the effect of site disorder on the zero field phase diagram of this material by considering the solid solution Ba$_{3}$(Mn$_{1-x}$V$_{x}$)$_{2}$O$_{8}$, where nonmagnetic V$^{5+}$ ions partially substitute magnetic Mn$^{5+}$ ions. This substitution results in unpaired $S=1$ moments for half-substituted dimers, which are ungapped and therefore susceptible to types of magnetic order not present in the parent compound. AC susceptibility measurements of compositions between $x=0.046$ and $x=0.84$ show a sharp frequency- and composition-dependent kink at temperatures below 210mK, suggesting that unpaired spins form a spin glass. The case for a glassy state is made clearer by the absence of any sharp features in the specific heat. However, Ba$_{3}$(Mn$_{1-x}$V$_{x}$)$_{2}$O$_{8}$ is not a paradigmatic spin glass. Whereas both the freezing temperature and the Weiss temperature (determined from susceptibility above 1K) vary strongly as a function of composition, the heat capacity per unpaired spin is found to be insensitive (above the glass transition) to the density of unpaired spins for the broad regime $0.18leq x leq 0.84$. This surprising result is consistent with a scenario in which nearest-neighbor unpaired spins form local, possibly fluctuating, spin-singlets prior to the eventual spin freezing. The spin glass state is only found for temperatures below the energy scale of single-ion anisotropy, suggestive this plays a significant role in determining the eventual ground state. Possible ground states in the dilute limit ($x < 0.04$ and $x > 0.9$) are also discussed.
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