Possible Itinerant-Electron Canted Antiferromagnetism in Tetragonal Antiperovskite Cr3AsN

We studied the magnetic, transport, and structural properties of the tetragonally distorted antiperovskite nitride Cr3AsN. A ferromagnetic-like increase in magnetic susceptibility below the magnetic transition temperature Tm = 255 K is reported for the first time. This magnetic transition is of the second order and not associated with a structural transition, unlike that in Mn-based antiperovskites. Although the observed spontaneous moment of 0.062 μB/Cr at the lowest temperature is very small, the reduction in the magnetic scattering in resistivity and spontaneous magnetostriction below Tm indicate the existence of a magnetic moment larger than the observed spontaneous magnetization. Zero-field 53Cr and 75As NMR results below Tm reveal the presence of a static moment of ∼0.5 μB at the Cr sites and a hyperfine field lying in the c-plane at the As site. Macroscopic and microscopic observations suggest the incomplete compensation of antiferromagnetically coupled moments. Canted antiferromagnetism is propose...