Exploring unconventional ferromagnetism in hole-doped LaCrAsO: insights into charge-transfer and magnetic interactions

Itinerant ferromagnetism due to the canonical double exchange (CDE) mechanism always occurs at low doping concentrations. Here we demonstrate the occurrence of robust itinerant ferromagnetism that can persist high doping concentrations. Using experimentally synthesized LaCrAsO as an illustrative example, we study the effects of hole doping via first-principles calculations and observe that the parent G-type antiferromagnetism vanishes quickly at a low doping concentration (∼0.20) and the system becomes a ferromagnetic metal due to the CDE mechanism. As the doping concentration continues to increase, the As 4p orbitals are gradually pushed up to the Fermi level and doped with holes. These ligand holes participate in the exchange interactions and drive the system toward ferromagnetism. Therefore, itinerant ferromagnetism doesn't terminate at an intermediate doping concentration as the CDE mechanism usually predicts. Furthermore, our results reveal that both the nearest and the next-nearest ferromagnetic exchange coupling strengths keep growing with doping concentration monotonically, showing that the emergent ferromagnetism mediated by As 4p orbitals is "stronger" than that of the CDE picture. Our work unlocks a new mechanism of itinerant ferromagnetism and potentially paves the way towards novel magneto-transport properties.