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

Among chromium trihalides, a specific group of layered van der Waals magnetic materials, chromium trichloride (CrCl3) is the only system relatively stable under ambient conditions. This is also observed in reduced dimensionality where the emergence of extrinsic long-range ordered oxidized and Cl-vacancy-defective CrCl3 phases is experimentally reported. In this work, the magnetic properties of such two-dimensional (2D) systems are studied using density functional theory (DFT) calculations, including the electron-electron (U) repulsion interactions, and Monte Carlo (MC) simulations. Once the Cl vacancies are introduced, the results indicate that the monolayer CrCl3 has a magnetic moment that is enhanced linearly (up to 3.14 mu ( B )/Cr) in the (1%-10%) vacancy concentration range. This determines a strengthening of the ferromagnetic state and a two-fold increase of the Curie temperature (up to 146 K) as valuated from MC simulations. More interestingly, once oxygen extrinsic impurities are considered, the monolayer CrCl3 structure is hybridized forming a stable ordered phase (O-CrCl3) with oxygen atoms allocated on the Cr atomic layer in the center of the honeycomb ring formed by Cr atoms. The magnetic moments of the O-CrCl3 system are localized on both Cr and O atoms, with oxygen antiferromagnetically coupled to chromium, resulting in a 2D ferrimagnetic hexagonal lattice system with an average magnetic moment of 2.14 mu ( B )/Cr and a high magnetic ordering temperature (110 K) predicted with DFT in the mean field approach.

Automated summary

In this study, the magnetic properties of two-dimensional CrCl3 systems were investigated using density functional theory and Monte Carlo simulations. It was found that the introduction of Cl vacancies leads to a linear increase in magnetic moment, strengthening the ferromagnetic state and increasing the Curie temperature. Additionally, the presence of oxygen impurities results in the formation of a stable ordered phase, with antiferromagnetic coupling between chromium and oxygen atoms, giving rise to a two-dimensional ferrimagnetic hexagonal lattice system with a high magnetic ordering temperature.