Abstract
Two-dimensional (2D) magnetic materials offer a promising platform for nanoscale spintronics and for exploration of novel physical phenomena. Here, we predict a diverse range of magnetic orders in cobalt-based 2D single septuple layers CoX2Y4, namely, CoBi2Te4, CoBi2Se2Te2, CoBi2Se4, and CoSb2Te4. Notably, CoBi2Te4 presents intrinsic non-collinear antiferromagnetism (AFM), while the others display collinear AFM. The emergence of AFM in all CoX2Y4 materials is attributed to the antiferromagnetic 90° Co-Te(Se)-Co superexchange coupling. The origin of non-collinear/collinear orders lies in competing Heisenberg exchange interactions within the Co triangular lattice. A pivotal factor governing the non-collinear order of CoBi2Te4 is the vanishingly small ratio of exchange coupling between next-nearest neighbour Co and the nearest neighbour Co (J2/J1 ∼ 0.01). Furthermore, our investigation into strain effects on CoX2Y4 lattices demonstrates the tunability of the magnetic state of CoSb2Te4 from collinear to non-collinear. Our prediction of the unique non-collinear AFM in 2D suggests the potential for observing extraordinary magnetic phenomena in 2D, including non-collinear scattering and magnetic domain walls.
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