Unconventional ferrimagnetism and enhanced magnetic ordering temperature in monolayer CrCl3 by introducing O impurities and Cl vacancies

Abstract Among chromium trihalides, a specific group of layered van der Waals magnetic materials, trichloride (CrCl 3 ) is the only system relatively stable under ambient conditions. This also observed in reduced dimensionality where emergence extrinsic long-range ordered oxidized and Cl-vacancy-defective CrCl phases experimentally reported. In this work, properties such two-dimensional (2D) systems are studied using density functional theory (DFT) calculations, including electron-electron (U) repulsion interactions, Monte Carlo (MC) simulations. Once Cl vacancies introduced, results indicate that monolayer has moment enhanced linearly (up to 3.14 µ B /Cr) (1%–10%) vacancy concentration range. determines strengthening ferromagnetic state two-fold increase Curie temperature 146 K) as valuated from MC More interestingly, once oxygen impurities considered, structure hybridized forming phase (O–CrCl with atoms allocated on Cr atomic layer center honeycomb ring formed by atoms. The moments O–CrCl localized both O atoms, antiferromagnetically coupled chromium, resulting 2D ferrimagnetic hexagonal lattice an average 2.14 /Cr high ordering (110 predicted DFT mean field approach.