Antiferromagnetism in trigonal SrMn2As2 and CaMn2As2 single crystals

Abstract: Crystallographic, electronic transport, thermal and magnetic properties are reported for SrMn2As2 and CaMn2As2 single crystals grown using Sn flux. Rietveld refinements of powder x-ray diffraction data show that the two compounds are isostructural and crystallize in the trigonal CaAl2Si2-type structure (space group P-3m1), in agreement with the literature. Electrical resistivity rho versus temperature T measurements demonstrate insulating ground states for both compounds with activation energies of 85 meV for SrMn2As2 and 61 meV for CaMn2As2. In a local-moment picture, the Mn^{+2} 3d^5 ions are expected to have high-spin S = 5/2 with spectroscopic splitting factor g = 2. Magnetic susceptibility chi and heat capacity measurements versus T reveal antiferromagnetic (AFM) transitions at TN = 120(2) K and 62(3) K for SrMn2As2 and CaMn2As2, respectively. The anisotropic chi(T < TN) data indicate that the hexagonal c axis is the hard axis and hence that the ordered Mn moments are aligned in the ab plane. The chi(T) for both compounds and Cp(T) data for SrMn2As2 show strong dynamic short-range AFM correlations from TN up to at least 900 K, likely associated with quasi-two-dimensional connectivity of strong AFM exchange interactions between the Mn spins within the corrugated honeycomb Mn layers parallel to the ab plane.