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Register a new userThermoelectric properties of LaRh$_{1-x}$Ni$_x$O$_3$
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We report measurements and analyses of resistivity, thermopower, and thermal conductivity of polycrystalline samples of perovskite LaRh$_{1-x}$Ni$_x$O$_3$. The thermopower is found to be large at 800 K (185 $mu$V/K for $x=$0.3), which is ascribed to the high-temperature stability of the low-spin state of Rh$^{3+}$/Rh$^{4+}$ ions. This clearly contrasts with the thermopower of the isostructural oxide LaCoO$_3$, which rapidly decreases above 500 K owing to the spin-state transition. The spin state of the transition-metal ions is one of the most important parameters in oxide thermoelectrics.
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Ab initio calculations have been performed to unravel the origin of the recently found superlattice peaks in the trilayer nickelate La$_4$Ni$_3$O$_8$. These peaks arise from static charge ordering of Ni$^{2+}$/ Ni$^{1+}$ stripes oriented at 45$^{circ}$ to the Ni-O bonds. An insulating state originates from a combination of structural distortions and magnetic order, with the gap being formed solely within the d$_{x^2-y^2}$ manifold of states. When doped, electrons or holes would go into these states, in a similar fashion to what occurs in the cuprates. Analogous calculations suggest that checkerboard charge order should occur in the bilayer nickelate La$_3$Ni$_2$O$_6$. These results reveal a close connection between La$_4$Ni$_3$O$_8$ and La$_3$Ni$_2$O$_6$ with La$_{2-x}$Sr$_x$NiO$_4$ for x=1/3 and x=1/2, respectively.
We use a combination of the coherent potential approximation and dynamical mean field theory to study magnetic properties of the Fe$_{1-x}$Ni$_x$ alloy from a first principles. Calculated uniform magnetic susceptibilities have a Curie-Weiss-like behavior and extracted effective temperatures are in agreement with the experimental results. The individual squared magnetic moments obtained as function of nickel concentration follow the same trends as experimental data. An analysis of the ionic and spin weights shows a possibility of a high-spin to intermediate- and low-spin states transitions at high temperatures.
We have examined an isovalent Rh substitution effect on the transport properties of the thermoelectric oxide Ca$_3$Co$_{4}$O$_9$ using single-crystalline form. With increasing Rh content $x$, both the electrical resistivity and the Seebeck coefficient change systematically up to $x=0.6$ for Ca$_3$Co$_{4-x}$Rh$_{x}$O$_9$ samples. In the Fermi-liquid regime where the resistivity behaves as $rho=rho_0+AT^2$ around 120 K, the $A$ value decreases with increasing Rh content, indicating that the correlation effect is weakened by Rh $4d$ electrons with extended orbitals. We find that, in contrast to such a weak correlation effect observed in the resistivity of Rh-substituted samples, the low-temperature Seebeck coefficient is increased with increasing Rh content, which is explained with a possible enhancement of a pseudogap associated with the short-range order of spin density wave. In high-temperature range above room temperature, we show that the resistivity is largely suppressed by Rh substitution while the Seebeck coefficient becomes almost temperature-independent, leading to a significant improvement of the power factor in Rh-substituted samples. This result is also discussed in terms of the differences in the orbital size and the associated spin state between Co $3d$ and Rh $4d$ electrons.
We present combined experimental and theoretical studies on the magnetic properties of a solid solution between yttrium orthoferrite and yttrium orthochromite systems, YFe$_{1-x}$Cr$_x$O$_3$ (0 $leq$ x $leq$ 1) where Fe$^{3+}$ and Cr$^{3+}$ ions are distributed randomly at the same crystallographic site (4b). We found that all the compositions exhibit weak ferromagnetism below the Neel temperature that decreases non-linearly with increasing $x$, while certain intermediate compositions ($x = 0.4,0.5$) show a compensation point and magnetization reversal. This unusual behavior is explained based on a simple model comprising the isotropic superexchange and the antisymmetric Dzyaloshinskii-Moriya interactions. This model explains the magnetization behavior in the entire range of doping and temperature including the magnetization reversal which results from an interplay of various DM interactions such as, Fe-O-Fe, Cr-O-Cr and Fe-O-Cr.
V2O3 famously features all four combinations of paramagnetic vs antiferromagnetic, and metallic vs insulating states of matter in response to %-level doping, pressure in the GPa range, and temperature below 300 K. Using time-of-flight neutron spectroscopy combined with density functional theory calculations of magnetic interactions, we have mapped and analyzed the inelastic magnetic neutron scattering cross section over a wide range of energy and momentum transfer in the chromium stabilized antiferromagnetic and paramagnetic insulating phases (AFI & PI). Our results reveal an important magnetic frustration and degeneracy of the PI phase which is relieved by the rhombohedral to monoclinic transition at $T_N=185$ K due to a significant magneto-elastic coupling. This leads to the recognition that magnetic frustration is an inherent property of the paramagnetic phase in $rm (V_{1-x}Cr_x)_2O_3$ and plays a key role in suppressing the magnetic long range ordering temperature and exposing a large phase space for the paramagnetic Mott metal-insulator transition to occur.
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