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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 χversus temperature T, isothermal magnetization M versus magnetic field H, specific heat Cp(T) and electrical resistivity ρ(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 ρ(T) and Cp(T) data reveal metallic character for both EuCu2As2 and EuCu1.82Sb2. Antiferromagnetic (AFM) ordering is indicated from the χ(T), Cp(T), and ρ(T) data for both EuCu2As2 (T_N = 17.5 K) and EuCu1.82Sb2 (T_N = 5.1 K). In EuCu1.82Sb2, the ordered-state χ(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 χ(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.