Spin and Orbital Effects on Asymmetric Exchange Interaction in Polar Magnets: M(IO3)2 (M = Cu and Mn).

Magnetic polar materials feature an astonishing range of physical properties, such as magnetoelectric coupling, chiral spin textures, and related new spin topology physics. This is primarily attributable to their lack of space inversion symmetry in conjunction with unpaired electrons, potentially facilitating an asymmetric Dzyaloshinskii-Moriya (DM) exchange interaction supported by spin-orbital and electron-lattice coupling. However, engineering the appropriate ensemble of coupled degrees of freedom necessary for enhanced DM exchange has remained elusive for polar magnets. Here, we study how spin and orbital components influence the capability of promoting the magnetic interaction by studying two magnetic polar materials, α-Cu(IO3)2 (2D) and Mn(IO3)2 (6S), and connecting their electronic and magnetic properties with their structures. The chemically controlled low-temperature synthesis of these complexes resulted in pure polycrystalline samples, providing a viable pathway to prepare bulk forms of transition-metal iodates. Rietveld refinements of the powder synchrotron X-ray diffraction data reveal that these materials exhibit different crystal structures but crystallize in the same polar and chiral P21 space group, giving rise to an electric polarization along the b-axis direction. The presence and absence of an evident phase transition to a possible topologically distinct state observed in α-Cu(IO3)2 and Mn(IO3)2, respectively, imply the important role of spin-orbit coupling. Neutron diffraction experiments reveal helpful insights into the magnetic ground state of these materials. While the long-wavelength incommensurability of α-Cu(IO3)2 is in harmony with sizable asymmetric DM interaction and low dimensionality of the electronic structure, the commensurate stripe AFM ground state of Mn(IO3)2 is attributed to negligible DM exchange and isotropic orbital overlapping. The work demonstrates connections between combined spin and orbital effects, magnetic coupling dimensionality, and DM exchange, providing a worthwhile approach for tuning asymmetric interaction, which promotes evolution of topologically distinct spin phases.