Enhanced magnetic anisotropy in two-dimensional [formula omitted] by self-intercalation: A DFT study

Abstract

Searching for two-dimensional (2D) materials with strong out-of-plane magnetic anisotropy is fatal features to 2D ferromagnets with high Curie temperature. In a recent experimental work (Zhao et al. (2020)), the samples they reported seems to meet the basic requirements for inducing large magnetic anisotropy. Based on density functional theory calculations, a large out-of-plane spin anisotropy, magnetic anisotropic energy (MAE) 97meV per supercell, has been observed in the as-synthesized 2H-TaS2 bilayer. Owing to the self-intercalation of Ta atoms who see a crystal field with low symmetry, orbital motions of 5d electrons in these Ta atoms are restored, leading to large spin–orbital coupling (SOC) and a large out-of-plane spin anisotropy. Based on the calculated energy difference between states with different magnetic orders, a rather high Curie temperature for the Ta intercalated 2H-TaS2 is also estimated at nearly 865K. Our study not only demonstrates the effectiveness of such preparation strategies on enhance the strong magnetic anisotropy and Curie temperature of 2H-TaS2 bilayer, but also deepen our understanding on the magnetic anisotropy induced by intrinsic SOC of 2D materials.