Enhanced Ferromagnetism of CrI3 Bilayer by Self-Intercalation*

Two-dimensional (2D) ferromagnets with high Curie temperature have long been the pursuit for electronic and spintronic applications. CrI 3 is a rising star of intrinsic 2D ferromagnets, however, it suffers from weak exchange coupling. Here we propose a general strategy of self-intercalation to achieve enhanced ferromagnetism in bilayer CrI 3 . We show that filling either Cr or I atoms into the van der Waals gap of stacked and twisted CrI 3 bilayers can induce the double exchange effect and significantly strengthen the interlayer ferromagnetic coupling. According to our first-principles calculations, the intercalated native atoms act as covalent bridge between two CrI 3 layers and lead to discrepant oxidation states for the Cr atoms. These theoretical results offer a facile route to achieve high-Curie-temperature 2D magnets for device implementation.