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

Abstract

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 degrees) 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 propose general strategies to realize them in 2D magnets. Our work not only uncovers a series of intriguing NLMO phenomena, but also paves the way for both fundamental research and device applications of ultra-thin NLMO materials.

arXiv comment10 pages,5 figures, npj Computational Materials accepted

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Cited by in corpus (5)

• Spin-chirality-driven second-harmonic generation in two-dimensional magnet CrSBr
• Reversing Neel Vector in PT-Antiferromagnets by Nonreciprocal Light Scattering
• Light-induced ultrafast magnetization dynamics in van der Waals antiferromagnetic CrSBr
• Temporal modulation of second harmonic generation in ferroelectrics by a pulsed electric field
• Advancements in Entangled Photon Pairs in 2D Van der Waals Materials for On-chip Quantum Applications