Giant and controllable nonlinear magneto-optical effects in two-dimensional magnets

The interplay of polarization and magnetism in materials with light can create rich nonlinear magneto-optical (NLMO) effects, and the recent discovery of two-dimensional (2D) van der Waals magnets provides remarkable control over NLMO effects due to their superb tunability. Here, based on first-principles calculations, we reported giant NLMO effects in CrI₃-based 2D magnets, including a dramatic change of second-harmonics generation (SHG) polarization direction (90°) and intensity (on/off switch) under magnetization reversal and a 100% SHG circular dichroism effect. We further revealed that these effects could not only be used to design ultra-thin multifunctional optical devices but also to detect subtle magnetic orderings. Remarkably, we analytically derived conditions to achieve giant NLMO effects and proposed general strategies to realize them in 2D magnets. Our work not only uncovers a series of intriguing and device applications of ultra-thin NLMO materials.