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Register a new userFormation of partial energy gap below the structural phase transition and the rare-earth element substitution effect on infrared phonons in ReFeAsO (Re=La, Nd, and Sm)
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Single crystals of LaFeAsO, NdFeAsO, and SmFeAsO have been prepared by means of a NaAs flux growth technique and studied by optical spectroscopy measurements. We show that the spectral features corresponding to the partial energy gaps in the spin-density-wave (SDW) state are present below the structural phase transition. This indicates that the electronic state below the structural phase transition is already very close to that in the SDW state. We also show that in-plane infrared phonon modes display systematic shifts towards high frequency upon rare-earth element substitutions for La, suggesting a strong enhancement of the bonding strength. Furthermore, an asymmetric line-shape of the in-plane phonon mode is observed, implying the presence of an electron-phonon coupling effect in Fe-pnictides.
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We synthesized bulk polycrystalline samples of RECoAsO (RE=La, Nd and Sm) by solid state reaction route in an evacuated sealed quartz tube. All these compounds are crystallized in a tetragonal structure with space group P4/nmm. The Co, in these compounds is in itinerant ferromagnetic state with its paramagnetic moment above 1.5 microB and the same orders ferromagnetically (FM) with small saturation moment of around 0.20 microB below say 80K. This bulk intrinsic magnetism of Co changes dramatically when nonmagnetic La is changed by magnetic Sm and Nd. Although the itinerant ferromagnetism occurs below 80-100K with small saturation moment, typical anti-ferromagnetic (AFM) transitions (TN1, TN2) are observed at 57K and 45K for Sm and at 69K and 14K for Nd. The transition of Co spins from FM to AFM, for magnetic Sm and Nd in RECoAsO is both field and temperature dependent. For applied fields below 100Oe, both TN1 and TN2 are seen, with intermediate fields below 1-2kOe only TN1 and above say 5kOe the AFM transition is not observed. This is evidenced in isothermal magnetization (MH) plots as well. It is clear that Sm/Nd magnetic moments interact with the ordered Co spins in adjacent layer and thus transforms the FM ordering to AFM. All the studied compounds are metallic in nature, and their magneto-transport R(T)H follows the temperature and field dependent FM-AFM transition of ordered Co spins.
We present results of transport and magnetic properties and heat capacity measurements on polycrystalline CeFeAsO, PrFeAsO, and NdFeAsO. These materials undergo structural phase transitions, spin density wave-like magnetic ordering of small moments on iron, and antiferromagnetic ordering of rare earth moments. The temperature dependence of the electrical resistivity, Seebeck coefficient, thermal conductivity, Hall coefficient, and magnetoresistance are reported. The magnetic behavior of the materials have been investigated using Mossbauer spectroscopy and magnetization measurements. Transport and magnetic properties are affected strongly by the structural and magnetic transitions, suggesting significant changes in the band structure and/or carrier mobilities occur, and phonon-phonon scattering is reduced upon transformation to the low temperature structure. Results are compared to recent reports for LaFeAsO, and systematic variations in properties as the identity of Ln is changed are observed and discussed. As Ln progresses across the rare-earth series from La to Nd, an increase in the hole contributions to Seebeck coefficient, and increases in magnetoresistance and the Hall coefficient are observed in the low temperature phase. Analysis of hyperfine fields at the iron nuclei determined from Mossbauer spectra indicates that the moment on Fe in the orthorhombic phase is nearly independent of the identity of Ln, in apparent contrast to reports of powder neutron diffraction refinements.
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.
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.
A new crystal growth technique for single-crystals of REFeAsO (RE = La, Ce, Pr, Nd, Sm, Gd, and Tb) using NaI/KI as flux is presented. Crystals with a size up to 300 $mu$m were isolated for single-crystal X-ray diffraction measurements. Lattice parameters were determined by LeBail fits of X-ray powder data against LaB6 standard. A consistent set of structural data is obtained and interpreted in a hard-sphere model. Effective radii for the rare-earth metal atoms for REFeAsO are deduced. The relation of the intra- and inter-plane distances of the arsenic atoms is identified as limiter of the phase formation, and its influence on Tc is discussed.
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