Atomic Intercalation Induced Spin-Flip Transition in Bilayer CrI 3 .

The recent discovery of 2D magnets has induced various intriguing phenomena due to the modulated spin polarization by other degrees of freedoms such as phonons, interlayer stacking, and doping. The mechanism of the modulated spin-polarization, however, is not clear. In this work, we demonstrate theoretically and computationally that interlayer magnetic coupling of the CrI 3 bilayer can be well controlled by intercalation and carrier doping. Interlayer atomic intercalation and carrier doping have been proven to induce an antiferromagnetic (AFM) to ferromagnetic (FM) phase transition in the spin-polarization of the CrI 3 bilayer. Our results revealed that the AFM to FM transition induced by atom intercalation was a result of enhanced superexchange interaction between Cr atoms of neighboring layers. FM coupling induced by O intercalation mainly originates from the improved superexchange interaction mediated by Cr 3 d -O 2 p coupling. FM coupling induced by Li intercalation was found to be much stronger than that by O intercalation, which was attributed to the much stronger superexchange by electron doping than by hole doping. This comprehensive spin exchange mechanism was further confirmed by our results of the carrier doping effect on the interlayer magnetic coupling. Our work provides a deep understanding of the underlying spin exchange mechanism in 2D magnetic materials.