Covalency, correlations, and interlayer interactions governing the magnetic and electronic structure of Mn3Si2Te6

This work establishes the spectroscopic fingerprints of ferrimagnetic Mn${}_{3}$Si${}_{2}$Te${}_{6}$, providing a comprehensive understanding of the electronic states underpinning its magnetic interactions. The authors show the pivotal role played by covalency, which weakens the electronic correlations and influences the magnetic frustrations and anisotropic exchange, leading to the onset of the long-range ferrimagnetic order in this compound. The approach of combining spectroscopic experiments with state-of-the-art first-principles theory will have widespread applicability across the families of layered and quasilayered magnetic materials.