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Register a new userStudy of Crystal-field Effects in Rare-earth (RE) - Transition-metal Intermetallic Compounds and in RE-based Laser Crystals
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Nicola Magnani
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Rare-earth (RE) based compounds and alloys are of great interest both for their fundamental physical properties and for applications. In order to tailor the required compounds for a specific task, one must be able to predict the energy level structure and transition intensities for any magnetic ion in any crystalline environment. The crystal-field (CF) analysis is one of the most powerful theoretical methods to deal with the physics of magnetic ions. In the present work, this technique is used to analyze peculiar physical properties of some materials employed in the production of new-generation solid-state laser and high-performance permanent magnets.
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Different element substitution effects in transition metal oxypnictide Re(O$_{1-x}$F$_x$)TAs with Re=La, Ce, Nd, Eu, Gd, Tm, T=Fe, Ni, Ru, were studied. Similar to the La- or Ce-based systems, we found that the pure NdOFeAs shows a strong resistivity anomaly near 145 K, which was ascribed to the spin-density-wave instability. Electron doping by F increases T$_c$ to about 50 K. While in the case of Gd, the T$_c$ is reduced below 10 K. The tetragonal ZrCuSiAs-type structure could not be formed for Eu or Tm substitution in our preparing process. For Ni-based case, although both pure and F-doped LaONiAs are superconducting, no superconductivity was found when La was replaced by Ce in both cases, instead a ferromagnetic ordering transition was likely to form at low temperature in F-doped sample. We also synthesized LaO$_{1-x}$F$_x$RuAs and CeO$_{1-x}$F$_x$RuAs compounds. Metallic behavior was observed down to 4 K.
Crystal electric field states in rare earth intermetallics show an intricate entanglement with the many-body physics that occurs in these systems and that is known to lead to a plethora of electronic phases. Here, we attempt to trace different contributions to the crystal electric field (CEF) splittings in CeIrIn$_5$, a heavy-fermion compound and member of the Ce$M$In$_5$ ($M$= Co, Rh, Ir) family. To this end, we utilize high-resolution resonant angle-resolved photoemission spectroscopy (ARPES) and present a spectroscopic study of the electronic structure of this unconventional superconductor over a wide temperature range. As a result, we show how ARPES can be used in combination with thermodynamic measurements or neutron scattering to disentangle different contributions to the CEF splitting in rare earth intermetallics. We also find that the hybridization is stronger in CeIrIn$_5$ than CeCoIn$_5$ and the effects of the hybridization on the Fermi volume increase is much smaller than predicted. By providing the first experimental evidence for $4f_{7/2}^{1}$ splittings which, in CeIrIn$_5$, split the octet into four doublets, we clearly demonstrate the many-body origin of the so-called $4f_{7/2}^{1}$ state.
Systematic experimental (vibrating sample magnetometry) and theoretical (electronic structure calculations using charge and spin self-consistent Korringa-Kohn-Rostoker Green function method) studies were performed on a series of intermetallic sigma-phase Fe(100-x)Re(x) (x = 43-53) compounds. Clear evidence was found that all investigated samples exhibit magnetism with an ordering temperature ranging between 65 K for x = 43 and 23 K for x = 53. The magnetism was revealed to be itinerant and identified as a spin-glass (SG) possibly having a re-entrant character. The SG was found to be heterogeneous viz. two regimes could be distinguished as far as irreversibility in temperature dependence of magnetization is concerned: (1) of a weak irreversibility and (2) of a strong one. According to the theoretical calculations the main contribution to the magnetism comes from Fe atoms occupying all five sub lattices. Re atoms have rather small moments. However, the calculated average magnetic moments are highly (ferromagnetic ordering model) or moderately (antiparallel ordering model) overestimated relative to the experimental data.
We investigate Seebeck effect in REFeAsO (RE=rare earth)compounds as a function of temperature and magnetic field up to 30T. The Seebeck curves are characterized by a broad negative bump around 50K, which is sample dependent and strongly enhanced by the application of a magnetic field. A model for the temperature and field dependence of the magnon drag contribution to the Seebeck effect by antiferromagnetic (AFM) spin fluctuation is developed. It accounts for the magnitude and scaling properties of such bump feature in our experimental data. This analysis allows to extract precious information on the coupling between electrons and AFM spin fluctuations in these parent compound systems, with implications on the pairing mechanism of the related superconducting compounds.
Fluoride-doped iron-based oxypnictides containing rare-earth gadolinium (GdFeAsO0.8F0.2) and co-doping with yttrium (Gd0.8Y0.2FeAsO0.8F0.2) have been prepared via conventional solid state reaction at ambient pressure. The non-yttrium substituted oxypnictide show superconducting transition as high as 43.9 K from temperature dependent resistance measurements with the Meissner effect observed at a lower temperature of 40.8 K from temperature dependent magnetization measurements. By replacing a small amount of gadolinium with yttrium Tc was observed to be lowered by 10 K which might be caused by a change in the electronic or magnetic structures since the crystal structure was not altered.
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