Giant and nonreciprocal second harmonic generation from layered antiferromagnetism in bilayer CrI₃

Layered antiferromagnetism is the spatial arrangement of ferromagnetic layers with antiferromagnetic interlayer coupling. Recently, the van der Waals magnet, chromium triiodide (CrI₃), emerged as the first layered antiferromagnetic insulator in its few-layer form. In this talk, we present an emergent nonreciprocal second-order nonlinear optical effect in bilayer CrI₃. The observed second-harmonic generation (SHG) is giant: several orders of magnitude larger than known magnetization induced SHG and comparable to SHG in the best 2D nonlinear optical materials studied so far. We show that while the parent lattice of bilayer CrI₃ is centrosymmetric and thus does not contribute to the SHG signal, the observed nonreciprocal SHG originates purely from the layered antiferromagnetic order, which breaks both spatial inversion and time reversal symmetries. Furthermore, polarization-resolved measurements reveal the underlying C_2h symmetry, and thus monoclinic stacking order in CrI₃ bilayers, providing key structural information for the microscopic origin of layered antiferromagnetism. Our results indicate that SHG is a highly sensitive probe of subtle magnetic orders and open up possibilities for the use of two-dimensional magnets in nonlinear and nonreciprocal optical devices.