Controlling Chiral Spin States of a Triangular-Lattice Magnet by Cooling in a Magnetic Field

Magnetic materials with a non-collinear and non-coplanar arrangement of magnetic moments hosting a nonzero scalar spin-chirality exhibit unique magnetic and spin-dependent electronic transport properties. The spin chirality often occurs in materials where competing exchange interactions lead to geometrical frustrations between magnetic moments and to a strong coupling between the crystal lattice and the magnetic structure. These characteristics are particularly strong in Mn-based antiperovskites where the interactions and chirality can be tuned by substitutional modifications of the crystalline lattice. This study presents evidence for the formation of two unequal chiral spin states in magnetically ordered Mn3.338Ni0.651N antiperovskite based on density functional theory calculations and supported by magnetization measurements after cooling in a magnetic field. The existence of two scalar spin-chiralities of opposite sign and different magnitude is demonstrated by a vertical shift of the magnetic-field dependent magnetization and Hall effect at low fields and from an asymmetrical magnetoresistivity when the applied magnetic field is oriented parallel or antiparallel to the direction of the cooling field. This opens up the possibility of manipulating the spin chirality for potential use in the emerging field of chiral spintronics.