Layer and doping tunable ferromagnetic order in two-dimensional CrS2 layers

Interlayer coupling is of vital importance for manipulating physical properties, e.g., electronic band gap, in two-dimensional materials. However, tuning magnetic properties in these materials is yet to be addressed. Here, we found the in-plane magnetic orders of $\mathrm{Cr}{\mathrm{S}}_{2}$ mono and few layers are tunable between striped antiferromagnetic (sAFM) and ferromagnetic (FM) orders by manipulating charge transfer between Cr ${t}_{2g}$ and ${e}_{g}$ orbitals. Such charge transfer is realizable through interlayer coupling, direct charge doping, or substituting S with Cl atoms. In particular, the transferred charge effectively reduces a portion of ${\mathrm{Cr}}^{4+}$ to ${\mathrm{Cr}}^{3+}$, which, together with delocalized S $p$ orbitals and their resulting direct S-S interlayer hopping, enhances the double-exchange mechanism favoring the FM rather than sAFM order. An exceptional interlayer spin-exchange parameter was revealed over $\ensuremath{-}10\phantom{\rule{0.16em}{0ex}}\mathrm{meV}$, an order of magnitude stronger than available results of interlayer magnetic coupling. It addition, the charge doping could tune $\mathrm{Cr}{\mathrm{S}}_{2}$ between $p$- and $n$-doped magnetic semiconductors. Given these results, several prototype devices were proposed for manipulating magnetic orders using external electric fields or mechanical motion. These results manifest the role of interlayer coupling in modifying magnetic properties of layered materials and shed considerable light on manipulating magnetism in these materials.