2025/07/05 by De Vita, Alessandro, Stavrić, Srdjan, Sant, Roberto +8
#FOS: Physical sciences #Materials Science (cond-mat.mtrl-sci) #Strongly Correlated Electrons (cond-mat.str-el)
paper · doi:10.48550/arxiv.2507.04144
Recent years have seen a vast increase in research into van der Waals magnetic materials. In many of these systems, magnetism is introduced via light 3d-transition metal elements, combined with chalcogenides or halogens. Despite the high technological promise in the field of spintronics, the connection between the d-orbital configuration and the occurrence of low-dimensional magnetic order is currently unclear. Here we address the prototypical two-dimensional ferromagnet CrI\textsubscript3, via complementary spectroscopies and density functional theory calculations. We reveal the electronic structure and orbital character of bulk CrI\textsubscript3 in the paramagnetic and ferromagnetic phases, describing the couplings underpinning its energy diagram, and providing a robust experimental demonstration that the mechanism of stabilization of ferromagnetism is attributable to orbital mixing between I p and Cr \textite\textsubscriptg states. These findings reveal the microscopic connection between orbital and spin degrees of freedom, providing fundamental insights into the behavior of low-dimensional magnetic materials.