Layer- and doping-tunable long range ferromagnetic order-ing in two-dimensional CrS2

Interlayer coupling is of vital importance for manipulating physical properties, e.g. electronic bandgap, in two-dimensional materials. However, tuning magnetic proper-ties in these materials is yet to be addressed. Here, we found a striped antiferromag-netic (sAFM) to ferromagnetic (FM) transition undergoing from monolayer to bilayer and thicker CrS2. This transition is attributed to charge sharing of interlayer S atoms and its resulting charge transfer from Cr d eg to t2g orbitals. The transferred charge reduces a portion of Cr4+ to Cr3+, which enhances the double-exchange mechanism favoring FM rather than sAFM ordering. Doping of electrons shares the same effect with stacking induced charge sharing. Therefore, charge doping could either manip-ulate the magnetic ordering between sAFM and FM or tune CrS2 between p- and n-doped magnetic semiconductors. We also proposed several prototype devices ena-bling to use external electric field for manipulating magnetic orderings of CrS2 layers. These results manifest the role of interlayer coupling in modifying magnetic proper-ties of layered materials