Unveiling elevated curie temperature and exceptional perpendicular magnetic anisotropy in chlorinated monolayer CrI3

Due to the finite band gap and a ferromagnetic ground state, the CrI3 monolayer is attracting great research interests. However, the low Curie temperature of 46 K is one of the major obstacles for spintronics applications. Here, we have investigated the magnetic properties of chlorinated CrI3 monolayer with varying concentration of Cl. We investigated the dynamical and thermal stability by phonon dispersion and ab-initio molecular dynamic simulation. The band gap was decreasing with increasing Cl concentration and a half-metallic state is obtained at Cl concentration of 4.22 × 1014/cm2. The pristine CrI3 monolayer had perpendicular magnetic anisotropy energy of 0.84 meV/Cr. We find that this perpendicular magnetic anisotropy energy can be even enhanced twice by chlorination. Due to the hybridization of I and Cr atom, we found the spin asymmetric density of states in the iodine atom and this strong enhancement in the magnetic anisotropy originated from asymmetric spin features in iodine atom. We propose that the chlorination can increase the Curie temperature up to 204 K and this is almost four times enhanced value. Based on these finding, we propose that the chlorinated CrI3 system can be a promising material for spintronics applications.