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Register a new userStructural and physical properties of trilayer nickelates $R_4$Ni$_3$O$_{10}$ ($R =$ La, Pr and Nd)
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We investigate the low temperature structural and physical properties of the trilayer nickelates R4Ni3O10 (R = La, Pr and Nd) using resistivity, thermopower, thermal conductivity, specific heat, high-resolution synchrotron powder X-ray diffraction and thermal expansion experiments. We show that all three compounds crystallize with a monoclinic symmetry, and undergo a metal-to-metal (MMT) transition at 135 K (La), 156 K (Pr) and 160 K (Nd). At MMT, the lattice parameters show distinct anomalies; however, without any lowering of the lattice symmetry. Unambiguous signatures of MMT are also seen in magnetic and thermal measurements, which suggest a strong coupling between the electronic, magnetic and structural degrees of freedom in these nickelates. Analysis of thermal expansion yields hydrostatic pressure dependence of MMT in close agreement with experiments. We show that the 9-fold coordinated Pr ions in the rocksalt (RS) layers have a crystal field (CF) split doublet ground state with possible antiferromagnetic ordering at 5 K. The Pr ions located in the perovskite block (PB) layers with 12-fold coordination, however, exhibit a non-magnetic singlet ground state. The CF ground state of Nd in both RS and PB layers is a Kramers doublet. Heat capacity of R = Nd shows a Schottky-like anomaly near35 K, and an upturn below T = 10 K suggesting the presence of short-range correlations between the Nd moments. However, no signs of long-range ordering could be found down to 2 K despite a sizeable theta_p ~ -40 K. The strongly suppressed magnetic long-range ordering in both R = Pr and Nd suggests the presence of strong magnetic frustration in these compounds. The low-temperature resistivity shows a T^0.5 dependence. No evidence for the heavy fermion behavior could be found in any of the three compounds.
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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.
Single crystals of the metallic Ruddlesden-Popper trilayer nickelates R$_4$Ni$_3$O$_{10}$ (R=La, Pr) were successfully grown using an optical-image floating zone furnace under oxygen pressure (pO$_2$) of 20 bar for La$_4$Ni$_3$O$_{10}$ and 140 bar for Pr$_4$Ni$_3$O$_{10}$. A combination of synchrotron and laboratory x-ray single crystal diffraction, high-resolution synchrotron x-ray powder diffraction and measurements of physical properties revealed that R$_4$Ni$_3$O$_{10}$ (R=La, Pr) crystallizes in the monoclinic $P$2$_1$/$a$ (Z=2) space group at room temperature, and that a metastable orthorhombic phase ($Bmab$) can be trapped by post-growth rapid cooling. Both La$_4$Ni$_3$O$_{10}$ and Pr$_4$Ni$_3$O$_{10}$ crystals undergo a metal-to-metal transition (MMT) below room temperature. In the case of Pr$_4$Ni$_3$O$_{10}$, the MMT is found at ~157.6 K. For La$_4$Ni$_3$O$_{10}$, the MMT depends on the lattice symmetry: 147.5 K for $Bmab$ vs. 138.6 K for $P$2$_1$/$a$. Lattice anomalies were found at the MMT that, when considered together with the pronounced dependence of the transition temperature on subtle structural differences between $Bmab$ and $P$2$_1$/$a$ phases, demonstrates a not insignificant coupling between electronic and lattice degrees of freedom in these trilayer nickelates.
We have investigated the temperature dependence of the magnetic susceptibility $chi(T)$ of rare-earth cobaltites RCoO$_3$ (R= La, Pr, Nd, Sm, Eu) in the temperature range $4.2-300$ K and also the influence of hydrostatic pressure up to 2 kbar on their susceptibility at fixed temperatures $T=78 $ and 300 K. The specific dependence $chi(T)$ observed in LaCoO$_3$ and the anomalously large pressure effect (d ln $chi$/d$Psim -100$ Mbar$^{-1}$ for $T = 78$ K) are analyzed in the framework of a two-level model with energy levels difference $Delta$. The ground state of the system is assumed to be nonmagnetic with the zero spin of Co$^{3+}$ ions, and magnetism at a finite temperature is determined by the excited magnetic spin state. The results of the analysis, supplemented by theoretical calculations of the electronic structure of LaCoO$_3$, indicate a significant increase in $Delta$ with a decrease in the unit cell volume under the hydrostatic pressure. In the series of RCoO$_3$ (R= Pr, Nd, Sm, Eu) compounds, the volume of crystal cell decreases monotonically due to a decrease in the radius of R$^{3+}$ ions. This leads to an increase in the relative energy $Delta$ of the excited state (the chemical pressure effect), which manifests itself in a decrease in the contribution of cobalt ions to the magnetic susceptibility at a fixed temperature, and also in a decrease in the hydrostatic pressure effect on the susceptibility of RCoO$_3$ compounds, which we have observed at $T=300$ K.
We report on structural and superconducting properties of La(3-x)R(x)Ni2B2N3 where La is substituted by the magnetic rare-earth elements Ce, Pr, Nd. The compounds Pr3Ni2B2N3 and Nd3Ni2B2N3 are characterized for the first time. Powder X-ray diffraction confirmed all samples R3Ni2B2N3 with R = La, Ce, Pr, Nd and their solid solutions to crystallize in the body centered tetragonal La3Ni2B2N3 structure type. Superconducting and magnetic properties of La(3-x)R(x)Ni2B2N3 were studied by resistivity, specific heat and susceptibility measurements. While La3Ni2B2N3 has a superconducting transition temperature Tc ~ 14 K, substitution of La by Ce, Pr, and Nd leads to magnetic pair breaking and, thus, to a gradual suppression of superconductivity. Pr3Ni2B2N3 exibits no long range magnetic order down to 2 K, Nd3Ni2B2N3 shows ferrimagnetic ordering below T_C = 17 K and a spin reorientation transition to a nearly antiferromagnetic state at 10 K.
We have studied the physical properties of Nd$_2$O$_3$ with neutron diffraction, inelastic neutron scattering, heat capacity, and magnetic susceptibility measurements. Nd$_2$O$_3$ crystallizes in a trigonal structure, with Nd$^{3+}$ ions surrounded by cages of 7 oxygen anions. The crystal field spectrum consists of four excitations spanning the energy range 3-60 meV. The refined eigenfunctions indicate XY-spins in the $ab$ plane. The Curie-Weiss temperature of $theta_{CW}=-23.7(1)$ K was determined from magnetic susceptibility measurements. Heat capacity measurements show a sharp peak at 550 mK and a broader feature centered near 1.5 K. Neutron diffraction measurements show that the 550 mK transition corresponds to long-range anti-ferromagnetic order implying a frustration index of $theta_{CW}/T_Napprox43$. These results indicate that Nd$_2$O$_3$ is a structurally and chemically simple model system for frustration caused by competing interactions with moments with predominate XY anisotropy.
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