Strongly Correlated Exciton‐Magnetization System for Optical Spin Pumping in CrBr3 and CrI3.

Abstract Ferromagnetism in van der Waals systems, preserved down to a monolayer limit, attracted attention to a class of materials with general composition CrX 3 (X=I, Br, and Cl), which are treated now as canonical 2D ferromagnets. Their diverse magnetic properties, such as different easy axes or varying and controllable character of in‐plane or interlayer ferromagnetic coupling, make them promising candidates for spintronic, photonic, optoelectronic, and other applications. Still, significantly different magneto‐optical properties between the three materials have been presenting a challenging puzzle for researchers over the last few years. Herewith, it is demonstrated that despite similar structural and magnetic configurations, the coupling between excitons and magnetization is qualitatively different in CrBr 3 and CrI 3 films. Through a combination of the optical spin pumping experiments with the state‐of‐the‐art theory describing bound excitonic states in the presence of magnetization, we concluded that the hole‐magnetization coupling has the opposite sign in CrBr 3 and CrI 3 and also between the ground and excited exciton state. Consequently, efficient spin pumping capabilities are demonstrated in CrBr 3 driven by magnetization via spin‐dependent absorption, and the different origins of the magnetic hysteresis in CrBr 3 and CrI 3 are unraveled.