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High-pressure flux growth, structural, and superconducting properties of LnFeAsO (Ln = Pr, Nd, Sm) single crystals

129   0   0.0 ( 0 )
 Added by Nikolai Zhigadlo
 Publication date 2012
  fields Physics
and research's language is English




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Single crystals of the LnFeAsO (Ln1111, Ln = Pr, Nd, and Sm) family with lateral dimensions up to 1 mm were grown from NaAs and KAs flux at high pressure. The crystals are of good structural quality and become superconducting when O is partially substituted by F (PrFeAsO1-xFx and NdFeAsO1-xFx) or when Fe is substituted by Co (SmFe1-xCoxAsO). From magnetization measurements, we estimate the temperature dependence and anisotropy of the upper critical field and the critical current density of underdoped PrFeAsO0.7F0.3 crystal with Tc = 25 K. Single crystals of SmFe1-xCoxAsO with maximal Tc up to 16.3 K for x = 0.08 were grown for the first time. From transport and magnetic measurements we estimate the critical fields and their anisotropy, and find these superconducting properties to be quite comparable to the ones in SmFeAsO1-xFx with a much higher Tc of = 50 K. The magnetically measured critical current densities are as high as 109 A/m2 at 2 K up to 7 T, with indication of the usual fishtail effect. The upper critical field estimated from resistivity measurements is anisotropic with slopes of -8.7 T/K (H // ab-plane) and -1.7 T/K (H // c-axis). This anisotropy (= 5) is similar to that in other Ln1111 crystals with various higher Tc s.



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A review of our investigations on single crystals of LnFeAsO1-xFx (Ln=La, Pr, Nd, Sm, Gd) and Ba1-xRbxFe2As2 is presented. A high pressure technique has been applied for the growth of LnFeAsO1-xFx crystals, while Ba1-xRbxFe2As2 crystals were grown using quartz ampoule method. Single crystals were used for electrical transport, structure, magnetic torque and spectroscopic studies. Investigations of the crystal structure confirmed high structural perfection and show less than full occupation of the (O, F) position in superconducting LnFeAsO1-xFx crystals. Resistivity measurements on LnFeAsO1-xFx crystals show a significant broadening of the transition in high magnetic fields, whereas the resistive transition in Ba1 xRbxFe2As2 simply shifts to lower temperature. Critical current density for both compounds is relatively high and exceeds 2x109 A/m2 at 15 K in 7 T. The anisotropy of magnetic penetration depth, measured on LnFeAsO1-xFx crystals by torque magnetometry is temperature dependent and apparently larger than the anisotropy of the upper critical field. Ba1-xRbxFe2As2 crystals are electronically significantly less anisotropic. Point-Contact Andreev-Reflection spectroscopy indicates the existence of two energy gaps in LnFeAsO1-xFx. Scanning Tunneling Spectroscopy reveals in addition to a superconducting gap, also some feature at high energy (~20 meV).
We investigate the effect of external pressure on magnetic order in undoped LnFeAsO (Ln = La, Ce, Pr, La) by using muon-spin relaxation measurements and ab-initio calculations. Both magnetic transition temperature $T_m$ and Fe magnetic moment decrease with external pressure. The effect is observed to be lanthanide dependent with the strongest response for Ln = La and the weakest for Ln = Sm. The trend is qualitatively in agreement with our DFT calculations. The same calculations allow us to assign a value of 0.68(2) $mu_B$ to the Fe moment, obtained from an accurate determination of the muon sites. Our data further show that the magnetic lanthanide order transitions do not follow the simple trend of Fe, possibly as a consequence of the different $f$-electron overlap.
We report flux free growth of superconducting FeSe single crystals by an easy and versatile high temperature melt and slow cooling method for first time. The room temperature XRD on the surface of the piece of such obtained crystals showed single 101 plane of Beta-FeSe tetragonal phase. The bulk powder XRD, being obtained by crushing the part of crystal chunk showed majority tetragonal and minority FeSe hexagonal crystalline phases. Detailed HRTEM images along with SAED (selected area electron diffraction) showed the abundance of both majority and minority FeSe phases. Both transport (RT) and magnetization (MT) exhibited superconductivity at below around 10K. Interestingly, the magnetization signal of these crystals is dominated by the magnetism of minority magnetic phase, and hence the isothermal magnetization (MH) at 4K was seen to be ferromagnetic (FM) like. Transport (R-T) measurements under magnetic field showed superconductivity onset at below 12K, and R = 0 (Tc) at 9K. Superconducting transition temperature (Tc) decreases with applied field to around 6K at 7Tesla, with dTc/dH of 0.4K/Tesla, giving rise to an Hc2 value of around 50 Tesla, 30 Tesla and 20 Tesla for Rn = 90, 50 and 10 percent respectively. FeSe single crystal activation energy is calculated from Thermally Activated Flux Flow (TAFF) model which is found to decreases with field.
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.
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.
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