Cong Wang1, Xieyu Zhou1, Yuhao Pan1, Jingsi Qiao1, Xianghua Kong1, Chao-Cheng Kaun2, Wei Ji1,*
1Beijing Key Laboratory of Optoelectronic Functional Materials & Micro-Nano Devices, Department of Physics, Renmin University of China, Beijing 100872, P.R. China
2Research Center for Applied Sciences, Academia Sinica, Taipei 11529, Taiwan, R. China
DOI:10.1103/PhysRevB.97.245409 Publication Date:
Interlayer coupling is of vital importance for manipulating physical properties, e.g. electronic bandgap, 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 CrS2 mono- and few-layers are tunable between striped antiferromagnetic (sAFM) and ferromagnetic (FM) orders by manipulating charge transfer between Cr t2g and eg 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 Cr4+ to Cr3+, 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 -10 meV, an order of magnitude stronger than available results of interlayer magnetic coupling. It addition, the charge doping could tune CrS2 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.