No Arabic abstract
Valency of Ce and Pr in LRu4P12 (L = Ce and Pr) was studied by L2,3-edge x-ray absorption near-edge structure (XANES) spectroscopy. The Ce-L3 XANES spectrum suggests that Ce is mainly trivalent, but the 4f state strongly hybridizes with ligand orbitals. The band gap of CeRu4P12 seems to be formed by strong hybridization of 4f electrons. Pr-L2 XANES spectra indicate that Pr exists in trivalent state over a wide range in temperature, 20 < T < 300 K. We find that the metal-insulator (MI) transition at TMI = 60 K in PrRu4P12 does not originate from Pr valence fluctuation.
Neutron scattering experiments have been performed on the ternary rare-earth diborocarbide Ce$^{11}$B$_2$C$_2$. The powder diffraction experiment confirms formation of a long-range magnetic order at $T_{rm N} = 7.3$ K, where a sinusoidally modulated structure is realized with the modulation vector ${bm q} = [0.167(3), 0.167(3), 0.114(3)]$. Inelastic excitation spectra in the paramagnetic phase comprise significantly broad quasielastic and inelastic peaks centered at $hbar omega approx 0, 8$ and 65 meV. Crystalline-electric-field (CEF) analysis satisfactorily reproduces the observed spectra, confirming their CEF origin. The broadness of the quasielastic peak indicates strong spin fluctuations due to coupling between localized $4f$ spins and conduction electrons in the paramagnetic phase. A prominent feature is suppression of the quasielastic fluctuations, and concomitant growth of a sharp inelastic peak in a low energy region below $T_{rm N}$. This suggests dissociation of the conduction and localized $4f$ electrons on ordering, and contrasts the presently observed incommensurate phase with spin-density-wave order frequently seen in heavy fermion compounds, such as Ce(Ru$_{1-x}$La$_x$)$_2$Si$_2$.
We report the magnetic properties strongly varying with the rare-earth elements in the newly found ternary compounds $R$Al$_{0.9}$Si$_{1.1}$, which crystallize in the tetragonal $alpha$-ThSi$_2$-type structure. For $R$ = Ce the alloy has a weak ferromagnetism below 11 K and for $R$ = Pr it orders ferromagnetically at 17 K, while for $R$ = Gd it is antiferromagnetic with $T_{rm N}$ = 30.5 K. In addition, we find no field effect on $T_{rm N}$ of $R$ = Gd because of the large internal mean field, but significant changes in the magnetic properties of $R$ = Ce and Pr.
The self-interaction-corrected local-spin-density approximation is used to describe the electronic structure of dioxides, REO$_2$, and sesquioxides, RE$_2$O$_3$, for the rare earths, RE=Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy and Ho. The valencies of the rare earth ions are determined from total energy minimization. We find Ce, Pr, Tb in their dioxides to have the tetravalent configuration, while for all the sesquioxides the trivalent groundstate configuration is found to be the most favourable. The calculated lattice constants for these valency configurations are in good agreement with experiment. Total energy considerations are exploited to show the link between oxidation and $f$-electron delocalization, and explain why, among the dioxides, only the CeO$_2$, PrO$_2$, and TbO$_2$ exist in nature. Tetravalent NdO$_2$ is predicted to exist as a metastable phase - unstable towards the formation of hexagonal Nd$_2$O$_3$.
We report zero field muon spin relaxation (muSR) measurements on RFeAsO with R = La, Ce, Pr, and Sm. We study the interaction of the FeAs and R (rare earth) electronic systems in the non superconducting magnetically ordered parent compounds of RFeAsO{1-x}Fx superconductors via a detailed comparison of the local hyperfine fields at the muon site with available Moessbauer spectroscopy and neutron scattering data. These studies provide microscopic evidence of long range commensurate magnetic Fe order with the Fe moments not varying by more than 15 % within the series RFeAsO with R = La, Ce, Pr, and Sm. At low temperatures, long range R magnetic order is also observed. Different combined Fe and R magnetic structures are proposed for all compounds using the muon site in the crystal structure obtained by electronic potential calculations. Our data point to a strong effect of R order on the iron subsystem in the case of different symmetry of Fe and R order parameters resulting in a Fe spin reorientation in the R ordered phase in PrFeAsO. Our symmetry analysis proves the absence of collinear Fe--R Heisenberg interactions in RFeAsO. A strong Fe--Ce coupling due to non--Heisenberg anisotropic exchange is found in CeFeAsO which results in a large staggered Ce magnetization induced by the magnetically ordered Fe sublattice far above T_N{Ce}. Finally, we argue that the magnetic R--Fe interaction is probably not crucial for the observed enhanced superconductivity in RFeAsO{1-x}Fx with a magnetic R ion.
We report on the use of $^{69,71}$Ga nuclear magnetic resonance to probe spin dynamics in the rare-earth kagom{e} system Pr$_3$Ga$_5$SiO$_{14}$. We find that the spin-lattice relaxation rate $^{69}1/T_1$ exhibits a maximum around 30 K, below which the Pr$^{3+}$ spin correlation time $tau$ shows novel field-dependent behavior consistent with a field-dependent gap in the excitation spectrum. The spin-spin relaxation rate $^{69}1/T_{2}$ exhibits a peak at a lower temperature (10 K) below which field-dependent power-law behavior close to $T^{2}$ is observed. These results point to field-induced formation of nanoscale magnetic clusters consistent with recent neutron scattering measurements.