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Register a new userInterplay of Rare Earth and Iron magnetism in RFeAsO with R = La, Ce, Pr, and Sm: A muon spin relaxation study and symmetry analysis
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Hans-Henning Klauss
Publication date
2009
fields
Physics
and research's language is
English
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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.
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We present measurements of the thermal expansion coefficient $alpha$ of polycrystalline RFeAsO (R = La,Ce,Pr,Sm,Gd). Anomalies at the magnetic ordering transitions indicate a significant magneto-elastic coupling and a negative pressure dependence of $T_{rm N}$ . The structural transitions are associated by large anomalies in $alpha$. Rare earth magnetic ordering in CeFeAsO, PrFeAsO, and SmFeAsO yields large positive anomalies at low temperatures.
The tetragonal-to-orthorhombic structural phase transition (SPT) in LaFeAsO (La-1111) and SmFeAsO (Sm-1111) single crystals measured by high resolution x-ray diffraction is found to be sharp while the RFeAsO (R=La, Nd, Pr, Sm) polycrystalline samples show a broad continuous SPT. Comparing the polycrystalline and the single crystal 1111 samples, the critical exponents of the SPT are found to be the same while the correlation length critical exponents are found to be very different. These results imply that the lattice fluctuations in 1111 systems change in samples with different surface to volume ratio that is assigned to the relieve of the temperature dependent superlattice misfit strain between active iron layers and the spacer layers in 1111 systems. This phenomenon that is missing in the AFe2As2 (A=Ca, Sr, Ba) 122 systems, with the same electronic structure but different for the thickness and the elastic constant of the spacer layers, is related with the different maximum superconducting transition temperature in the 1111 (55 K) versus 122 (35 K) systems and implies the surface reconstruction in 1111 single crystals.
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.
We have studied the magnetism of the Pr3+ ions in PrFeAsO_1-xF_x (x = 0; 0.15) and its interaction with the Fe magnetic order (for x = 0). Specific heat data confirm the presence of a first excited crystal electric field (CEF) level around 3.5 meV in the undoped compound PrFeAsO. This finding is in agreement with recent neutron scattering experiments. The doped compound is found to have a much lower first CEF splitting of about 2.0 meV. The Pr ordering in PrFeAsO gives rise to large anomalies in the specific heat and the thermal expansion coefficient. In addition, a field-induced transition is found at low temperatures that is most pronounced for the magnetostriction coefficient. This transition, which is absent in the doped compound, is attributed to a reversal of the Fe spin canting as the antiferromagnetic Pr order is destroyed by the external magnetic field.
The Pr-rich end of the alloy series Pr$_{1-x}$Nd$_x$Os$_4$Sb$_{12}$ has been studied using muon spin rotation and relaxation. The end compound PrOs$_4$Sb$_{12}$ is an unconventional heavy-fermion superconductor, which exhibits a spontaneous magnetic field in the superconducting phase associated with broken time-reversal symmetry. No spontaneous field is observed in the Nd-doped alloys for x $>$ 0.05. The superfluid density is insensitive to Nd concentration, and no Nd$^{3+}$ static magnetism is found down to the lowest temperatures of measurement. Together with the slow suppression of the superconducting transition temperature with Nd doping, these results suggest anomalously weak coupling between Nd spins and conduction-band states.
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