No Arabic abstract
The ground state properties of the pure perovskite compounds PrMnO$_3$ and NdMnO$_3$ were investigated by magnetization, magnetic AC susceptibility and specific heat measurements. A strongly anisotropic behavior has been detected for temperatures below the antiferromagnetic phase transition $T_N$~100K. The susceptibility and the weak spontaneous ferromagnetic moment appear to be different in both compounds due to different anisotropic rare earth contributions. The specific heat shows strong Schottky type contributions at low temperatures, which for NdMnO$_3$ strongly depend on the magnetic field. A spin reorientation phase transition (spin-flop type) induced by a magnetic field along b axis was observed in NdMnO$_3$ at H~110kOe and T=5K. All results can consistently be explained by anisotropic contributions of the rare earth ions: In PrMnO$_3$ the electronic ground state is determined by a low lying quasidoublet split by the crystal field ~19 K. In NdMnO$_3$ the Kramers doublet is split by an exchange Nd-Mn field (~20K).
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 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.
Controlling material properties by modulating the crystalline structure has been attempted using various techniques, e.g., hydrostatic pressure, chemical pressure, and epitaxy. These techniques succeed to improve properties and achieve desired functionalities by changing the unit cell in all dimensions. In order to obtain a more detailed understanding on the relation between the crystal lattice and material properties, it is desirable to investigate the influence of a smaller number of parameters. Here, we utilize the combination of chemical pressure and epitaxy to modify a single lattice parameter of the multiferroic orthorhombic RMnO$_3$ (R = rare-earth, o-RMnO$_3$) system. By growing a series of o-RMnO$_3$ (R = Gd - Lu) films coherently on (010)-oriented YAlO$_3$ substrates, the influence of chemical pressure is reflected only along the $b$-axis. Thus, a series of o-RMnO$_3$ with $a$ ~ 5.18 {AA}, 5.77 {AA} < $b$ < 5.98 {AA}, and $c$ ~ 7.37 {AA} were obtained. Raman spectra analysis reveals that the change of the $b$-axis parameter induces a shift of the oxygen in the nominally fixed $ca$-plane. Their ferroelectric ground state is independent on the $b$-axis parameter showing polarization of ~ 1 $mu$C cm$^{-2}$ along the $a$-axis for the above-mentioned range, except for $b$ ~ 5.94 {AA} which corresponds to TbMnO$_3$ showing ~ 2 $mu$C cm$^{-2}$. This result implies that multiferroic order of o-RMnO$_3$ is almost robust against the $b$-axis parameter provided that the dimension of the $ca$-plane is fixed to 7.37 {AA} $times$ 5.18 {AA}.
The bulk magnetic properties of the lanthanide metaborates, $Ln$(BO$_2$)$_3$, $Ln$ = Pr, Nd, Gd, Tb are studied using magnetic susceptibility, heat capacity and isothermal magnetisation measurements. They crystallise in a monoclinic structure containing chains of magnetic $Ln^{3+}$ and could therefore exhibit features of low-dimensional magnetism and frustration. Pr(BO$_2$)$_3$ is found to have a non-magnetic singlet ground state. No magnetic ordering is observed down to 0.4 K for Nd(BO$_2$)$_3$. Gd(BO$_2$)$_3$ exhibits a sharp magnetic transition at 1.1 K, corresponding to three-dimensional magnetic ordering. Tb(BO$_2$)$_3$ shows two magnetic ordering features at 1.05 K and 1.95 K. A magnetisation plateau at a third of the saturation magnetisation is seen at 2 K for both Nd(BO$_2$)$_3$ and Tb(BO$_2$)$_3$ which persists in an applied field of 14 T. This is proposed to be a signature of quasi one-dimensional behaviour in Nd(BO$_2$)$_3$ and Tb(BO$_2$)$_3$.