Bottom-up building of two-dimensional magnetic materials with self-assembly of superatom TM@Sn12 (TM = Sc, Ti, V, Cr, Mn, Fe) clusters

Abstract

The miniaturization of electronic devices is increasingly requiring some low-dimensional magnetic materials with excellent properties, so ultra-thin two-dimensional magnetic materials have attracted extensive attention. However, most two-dimensional materials exfoliated from bulk either lack intrinsic magnetism or have low magnetic transition temperatures, which greatly limits their practical applications. Here, using magnetic superatom TM@Sn12 (TM = Sc, Ti, V, Cr, Mn, Fe) clusters as building blocks, a series of two-dimensional materials are designed and the underlying mechanism for magnetic order and stability are explained by direct exchange of outer superatom orbitals (1G, 2P and 2D). The honeycomb lattice of TM@Sn12 (TM = V, Cr, Fe) and the square lattice of Ti@Sn12 are ferromagnetic. The Cr@Sn12 honeycomb lattice has a large out-of-plane magnetic anisotropic energy of 2.21 meV and its Curie temperature reaches 162 K, while the Fe@Sn12 honeycomb lattice has a large in-plane magnetic anisotropic energy of 3.58 meV. This research provides a new avenue for developing novel magnetic materials with excellent properties.