We report the growth of single crystals of SrCu2As2, SrCu2Sb2, SrCu2(As0.84Sb0.16)2 and BaCu2Sb2 using the self-flux technique and their structural, magnetic, thermal and transport properties that were investigated by powder x-ray diffraction (XRD), magnetic susceptibility χ, specific heat Cp and electrical resistivity ρ measurements versus temperature T from 1.8 to 350 K. Rietveld refinements of XRD patterns for crushed crystals confirm that SrCu2As2 crystallizes in the ThCr2Si2-type body-centered tetragonal structure (space group I4/mmm) and SrCu2Sb2 crystallizes in the CaBe2Ge2-type primitive tetragonal structure (space group P 4/nmm). However, as reported previously, BaCu2Sb2 is found to have a large unit cell consisting of three blocks. Here a ThCr2Si2-type block is sandwiched between two CaBe2Ge2-type blocks along the c-axis with an overall symmetry of I4/mmm, as reported, but likely with a monoclinic distortion. The χ data of all these compounds are diamagnetic and reveal nearly T -independent anisotropic behavior. The χ of SrCu2As2 is found to be larger in the ab-plane than along the c-axis, as also previously reported for pure and doped BaFe2As2, whereas the χ values of SrCu2Sb2 and BaCu2Sb2 are larger along the c-axis. This difference in anisotropy appears to arise from the differences between the crystal structures. The finite values of the Sommerfeld linear specific heat coefficients γ and the T dependences of ρ reveal metallic character of all four compounds. The electronic and magnetic properties indicate that these compounds are sp metals with Cu in the nonmagnetic 3d 10 electronic configuration corresponding to the oxidation state Cu +1 , as previously predicted theoretically for SrCu2As2 by D. J. Singh [Phys. Rev. B 79, 153102 (2009)]. We present a brief review of theoretical and experimental work on the doping character of transition metals for Fe in BaFe2As2. The As-As covalent interlayer bond distances in the collapsed-tetragonal (Ca,Sr,Ba)Cu2As2 compounds are much shorter than the nonbonding As-As distances in BaFe2As2. Thus the electronic character of the Cu and the strength of the As-As interlayer bonding are both expected to drastically change between weakly Cu-substituted BaFe2As2 and pure BaCu2As2, perhaps via a first-order lattice instability such as a miscibility gap in the Ba(Fe1−xCux)2As2 system.
The synthesis and crystallographic and physical properties of polycrystalline EuNiGe3 are reported. EuNiGe3 crystallizes in the noncentrosymmetric body-centered tetragonal BaNiSn3-type structure (space group I4mm), in agreement with previous reports, with the Eu atoms at the corners and body center of the unit cell. The physical property data consistently demonstrate that this is a metallic system in which Eu spins S = 7/2 order antiferromagnetically at a temperature TN = 13.6 K. Magnetic susceptibility χ data for T > TN indicate that the Eu atoms have spin 7/2 with g = 2, that the Ni atoms are nonmagnetic, and that the dominant interactions between the Eu spins are ferromagnetic. Thus we propose that EuNiGe3 has a collinear A-type antiferromagnetic structure, with the Eu ordered moments in the ab-plane aligned ferromagnetically and with the moments in adjacent planes along the c-axis aligned antiferromagnetically. A fit of χ(T ≤ TN) by our molecular field theory is consistent with a collinear magnetic structure. Electrical resistivity ρ data from TN to 350 K are fitted by the Bloch-Grüneisen model for electron-phonon scattering, yielding a Debye temperature of 265(2) K. A strong decrease in ρ occurs below TN due to loss of spin-disorder scattering. Heat capacity data at 25 K ≤ T ≤ 300 K are fitted by the Debye model, yielding the same Debye temperature 268(2) K as found from ρ(T ). The extracted magnetic heat capacity is consistent with S = 7/2 and shows that significant short-range dynamical spin correlations occur above TN. The magnetic entropy at TN = 13.6 K is 83% of the expected asymptotic high-T value, with the remainder recovered by 30 K.
Polycrystalline samples of Lu1−xScxMnSi (x = 0, 0.25, 0.5) are studied using powder x-ray diffraction, heat capacity Cp, magnetization, magnetic susceptibility χ, and electrical resistivity ρ measurements versus temperature T and magnetic field H. This system crystallizes in the primitive orthorhombic TiNiSi-type structure (space group Pnma) as previously reported. The ρ(T ) data indicate metallic behavior. The Cp(T ), χ(T ), and ρ(T ) measurements consistently indicate longrange antiferromagnetic (AF) transitions with AF ordering temperatures TN = 246, 215 and 188 K for x = 0, 0.25 and 0.5, respectively. A second transition is observed at somewhat lower T for each sample from the χ(T ) and ρ(T ) measurements, which we speculate are due to spin reorientation transitions; these second transitions are completely suppressed in H = 5.5 T. The Cp data below 10 K for each composition indicate an enhanced Sommerfeld electronic heat capacity coefficient for the series in the range γ = 24-29 mJ/mol K 2 . The χ(T ) measurements up to 1000 K were fitted by local-moment Curie-Weiss behaviors which indicate a low Mn spin S ∼ 1. The χ data below TN are analyzed using the Weiss molecular field theory for a planar noncollinear cycloidal AF structure with a composition-dependent pitch, following the previous neutron diffraction work of Venturini et al. [J. Alloys Compd. 256, 65 (1997)]. Within this model, the fits indicate a turn angle between Mn ordered moments along the cycloid axis of ∼ 100• or ∼ 145• , either of which indicate dominant AF interactions between the Mn spins in the Lu1−xScxMnSi series of compounds.
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