Antiferromagnetism in EuCu2As2 and EuCu1.82Sb2 Single Crystals

Single crystals of EuCu2As2 and EuCu2Sb2 were grown from CuAs and CuSb self-flux, respectively. The crystallographic, magnetic, thermal and electronic transport properties of the single crystals were investigated by room-temperature x-ray diffraction (XRD), magnetic susceptibility \chi versus temperature T, isothermal magnetization M versus magnetic field H, specific heat Cp(T) and electrical resistivity \rho(T) measurements. EuCu2As2 crystallizes in the body-centered tetragonal ThCr2Si2-type structure (space group I4/mmm), whereas EuCu2Sb2 crystallizes in the related primitive tetragonal CaBe2Ge2-type structure (space group P4/nmm). The energy-dispersive x-ray spectroscopy and XRD data for the EuCu2Sb2 crystals showed the presence of vacancies on the Cu sites, yielding the actual composition EuCu1.82Sb2. The \rho(T) and Cp(T) data reveal metallic character for both EuCu2As2 and EuCu1.82Sb2. Antiferromagnetic (AFM) ordering is indicated from the \chi(T), Cp(T), and \rho(T) data for both EuCu2As2 (T_N = 17.5 K) and EuCu1.82Sb2 (T_N = 5.1 K). In EuCu1.82Sb2, the ordered-state \chi(T) and M(H) data suggest either a collinear A-type AFM ordering of Eu+2 spins S=7/2 or a planar noncollinear AFM structure, with the ordered moments oriented in the tetragonal ab plane in either case. This ordered-moment orientation for the A-type AFM is consistent with calculations with magnetic dipole interactions. The anisotropic \chi(T) and isothermal M(H) data for EuCu2As2, also containing Eu+2 spins S=7/2, strongly deviate from the predictions of molecular field theory for collinear AFM ordering and the AFM structure appears to be both noncollinear and noncoplanar.Comment: 21 pages, 22 figures, 4 Table

Metallic behavior induced by potassium doping of the trigonal antiferromagnetic insulator EuMn2As2

We report magnetic susceptibility \chi, isothermal magnetization M, heat capacity C_p and electrical resistivity \rho measurements on undoped EuMn2As2 and K-doped Eu0.96K0.04Mn2As2 and Eu0.93K0.07Mn2As2 single crystals with the trigonal CaAl2Si2-type structure as a function of temperature T and magnetic field H. EuMn2As2 has an insulating ground state with an activation energy of 52 meV and exhibits antiferromagnetic (AFM) ordering of the Eu+2 spins S=7/2 at T_N1 = 15 K from C_p(T) and \chi(T) data with a likely spin-reorientation transition at T_N2 = 5.0 K. The Mn+2 3d5 spins-5/2 exhibit AFM ordering at T_N = 142 K from all three types of measurements. The M(H) isotherm and \chi(T) data indicate that the Eu AFM structure is both noncollinear and noncoplanar. The AFM structure of the Mn spins is also unclear. A 4% substitution of K for Eu in Eu0.96K0.04Mn2As2 is sufficient to induce a metallic ground state. Evidence is found for a difference in the AFM structure of the Eu moments in the metallic crystals from that of undoped EuMn2As2 versus both T and H. For metallic Eu0.96K0.04Mn2As2 and Eu0.93K0.07Mn2As2, an anomalous S-shape T dependence of \rho related to the Mn magnetism is found. Upon cooling from 200 K, \rho exhibits a strong negative curvature, reaches maximum positive slope at the Mn T_N ~ 150 K, and then continues to decrease but more slowly below T_N. This suggests that dynamic short-range AFM order of the Mn spins above the Mn T_N strongly suppresses the resistivity, contrary to the conventional decrease of \rho that is only observed upon cooling below T_N of an antiferromagnet.Comment: 21 pages, 22 figures, 4 Table

Physical properties of EuPd2As2 single crystals

The physical properties of self-flux grown EuPd2As2 single crystals have been investigated by magnetization M, magnetic susceptibility chi, specific heat Cp, and electrical resistivity rho measurements versus temperature T and magnetic field H. The crystal structure was determined by powder x-ray diffraction measurements, which confirmed the ThCr2Si2-type body-centered tetragonal structure (space group I4/mmm) reported previously. The rho(T) data indicate that state of EuPd2As2 is metallic. Long-range antiferromagnetic (AFM) ordering is apparent from the chi(T), Cp(T), and rho(T) measurements. For H \parallel c the chi(T) indicates two transitions at TN1 = 11.0 K and TN2 = 5.5 K, whereas for H \perp c only one transition is observed at TN1 = 11.0 K. Between TN1 and TN2 the anisotropic chi(T) data suggest a planar noncollinear AFM structure, whereas at T < TN2 the chi(T) and M(H,T) data suggest a spin reorientation transition in which equal numbers of spins cant in opposite directions out of the ab plane. We estimate the critical field at 2 K at which all Eu moments become aligned with the field to be about 22 T. The magnetic entropy at 25 K estimated from the Cp(T) measurements is about $11\%$ smaller than expected, possibly due to an inaccuracy in the lattice heat capacity contribution. An upturn in rho at T < TN1 suggests superzone energy gap formation below TN1. This behavior of rho(T < TN1) is not sensitive to applied magnetic fields up to H = 12 T.Comment: 11 pages, 10 figures, 2 tables and 52 references; To appear in J. Phys.: Condens. Matte

Investigations of the effect of nonmagnetic Ca substitution for magnetic Dy on spin-freezing in Dy2Ti2O7

Physical properties of partially Ca substituted hole-doped Dy2Ti2O7 have been investigated by ac magnetic susceptibility \chi_ac(T), dc magnetic susceptibility \chi(T), isothermal magnetization M(H) and heat capacity C_p(T) measurements on Dy1.8Ca0.2Ti2O7. The spin-ice system Dy2Ti2O7 exhibits a spin-glass type freezing behavior near 16 K. Our frequency dependent \chi_ac(T) data of Dy1.8Ca0.2Ti2O7 show that the spin-freezing behavior is significantly influenced by Ca substitution. The effect of partial nonmagnetic Ca2+ substitution for magnetic Dy3+ is similar to the previous study on nonmagnetic isovalent Y3+ substituted Dy2-xYxTi2O7 (for low levels of dilution), however the suppression of spin-freezing behavior is substantially stronger for Ca than Y. The Cole-Cole plot analysis reveals semicircular character and a single relaxation mode in Dy1.8Ca0.2Ti2O7 as for Dy2Ti2O7. No noticeable change in the insulating behavior of Dy2Ti2O7 results from the holes produced by 10% Ca2+ substitution for Dy3+ ions.Comment: 9 pages, 7 figures, 1 tabl

Superconductivity and Physical Properties of CaPd2Ge2 Single Crystals

We present the superconducting and normal state properties of CaPd2Ge2 single crystal investigated by magnetic susceptibility \chi, isothermal magnetization M, heat capacity C_p, in-plane electrical resistivity \rho and London penetration depth \lambda versus temperature T and magnetic field H measurements. Bulk superconductivity is inferred from the \rho(T) and C_p(T) data. The \rho(T) data exhibit metallic behavior and undergoes a superconducting transition with T_c onset = 1.98 K and zero resistivity state at T_c 0 = 1.67 K. The \chi(T) reveal the onset of superconductivity at 2.0 K. For T>2.0 K, the \chi(T) and M(H) are weakly anisotropic paramagnetic with \chi_ab > \chi_c. The C_p(T) confirm the bulk superconductivity below T_c = 1.69(3) K. The superconducting state electronic heat capacity is analyzed within the framework of a single-band \alpha-model of BCS superconductivity and various normal and superconducting state parameters are estimated. Within the \alpha-model, the C_p(T) data and the ab plane \lambda(T) data consistently indicate a moderately anisotropic s-wave gap with \Delta(0)/k_B T_c ~ 1.6, somewhat smaller than the BCS value of 1.764. The relationship of the heat capacity jump at T_c and the penetration depth measurement to the anisotropy in the s-wave gap is discussed.Comment: 12 pages, 9 figures, 2 Tables; Submitted to PR

Crystal field states of Kondo lattice heavy fermions CeRuSn3 and CeRhSn3

Inelastic neutron scattering experiments have been carried out to determine the crystal field states of the Kondo lattice heavy fermions CeRuSn3 and CeRhSn3. Both the compounds crystallize in LaRuSn3-type cubic structure (space group Pm-3n) in which the Ce atoms occupy two distinct crystallographic sites with cubic (m-3) and tetragonal (-4m.2) point symmetries. The INS data of CeRuSn3 reveal the presence of a broad excitation centered around 6-8 meV which is accounted by a model based on crystal electric field (CEF) excitations. On the other hand, the INS data of isostructural CeRhSn3 reveal three CEF excitations around 7.0, 12.2 and 37.2 meV. The neutron intensity sum rule indicates that the Ce ions at both cubic and tetragonal Ce sites are in Ce3+ state in both CeRuSn3 and CeRhSn3. The CEF level schemes for both the compounds are deduced. We estimate the Kondo temperature T_K = 3.1(2) K for CeRuSn3 from neutron quasielastic linewidth in excellent agreement with that determined from the scaling of magnetoresistance which gives T_K = 3.2(1) K. For CeRhSn3 the neutron quasielastic linewidth gives T_K = 4.6 K. For both CeRuSn3 and CeRhSn3, the ground state of Ce3+ turns out to be a quartet for the cubic site and a doublet for the tetragonal site.Comment: 12 pages, 13 figures, 2 tables, to appear in Phys. Rev.