Long-range antiferromagnetic interactions in Ni-Co-Mn-Ga metamagnetic Heusler alloys: A two-step ordering studied by neutron diffraction

We report on the experimental observation of a long-range antiferromagnetic structure in the metamagnetic Ni-Co-Mn-Ga Heusler alloys. The accurate magnetic symmetry analysis based on experimental neutron diffraction data, exploiting the Shubnikov theory, allows the determination of the correct magnetic space group of the system. A two-step process, featuring the ordering of the Ni and Mn sublattices at different temperatures, leads to the antiferromagnetic structure in martensite. A perfect, constrained by the symmetry, antiferromagnetic ordering of the Ni sublattice in the "paramagnetic gap" is observed, followed by the ordering of the Mn sublattice at lower temperatures. The observation of such antiferromagnetic structure clarifies the current debate on the presence of antiferromagnetic interactions in the (Ni,Co)-Mn-X (X=Ga, Sn, Sb, and In) ferromagnetic shape memory alloys and yields new insights in understanding the magnetostructural properties of this relevant class of materials.