Large Photogalvanic Spin Current by Magnetic Resonance in Bilayer Cr Trihalides

Spin current is a key to realizing various phenomena and functionalities related to spintronics. Recently, the possibility of generating spin current through a photogalvanic effect of magnons was pointed out theoretically. However, neither a candidate material nor a general formula for calculating the photogalvanic spin current in materials is known so far. In this Letter, we develop a general formula for the photogalvanic spin current through a magnetic resonance process. This mechanism involves a one-magnon excitation process in contrast to the two-particle processes studied in earlier works. Using the formula, we show that GHz and THz waves create a large photogalvanic spin current in the antiferromagnetic phase of bilayer CrI3 and CrBr3. The large spin current arises from an optical process involving two magnon bands, which is a contribution unknown to date. This spin current appears only in the antiferromagnetic ordered phase and is reversible by controlling the order parameter. These results open a route to material design for the photogalvanic effect of magnetic excitations.