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

Abstract

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, opening up ample opportunities for novel device functionalities. Here, we discovered 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 (e.g. MoS2). We showed 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 revealed the underlying C2h symmetry, and thus monoclinic stacking order in CrI3 bilayers, providing crucial structural information for the microscopic origin of layered antiferromagnetism. Our results highlight SHG as a highly sensitive probe that can reveal subtle magnetic order and open novel nonlinear and nonreciprocal optical device possibilities based on 2D magnets.

References in corpus (22)

• Layer-dependent Ferromagnetism in a van der Waals Crystal down to the Monolayer Limit
• Discovery of intrinsic ferromagnetism in 2D van der Waals crystals
• Gate-tunable Room-temperature Ferromagnetism in Two-dimensional Fe${}_3$GeTe${}_2$
• Two-Dimensional Itinerant Ising Ferromagnetism in Atomically thin Fe3GeTe2
• Electrical Control of 2D Magnetism in Bilayer CrI3
• Giant Tunneling Magnetoresistance in Spin-Filter van der Waals Heterostructures
• Controlling magnetism in 2D CrI3 by electrostatic doping
• Ising-Type Magnetic Ordering in Atomically Thin FePS3
• Probing magnetism in 2D van der Waals crystalline insulators via electron tunneling
• Electric-field switching of two-dimensional van der Waals magnets
• Room Temperature Intrinsic Ferromagnetism in Epitaxial Manganese Selenide Films in the Monolayer Limit
• Second harmonic microscopy of monolayer MoS2
• Stacking-Dependent Magnetism in Bilayer CrI${}_3$
• Very Large Tunneling Magnetoresistance in Layered Magnetic Semiconductor CrI${}_3$
• Electrical Control of Second-Harmonic Generation in a WSe2 Monolayer Transistor
• Antiferromagnetic opto-spintronics: Part of a collection of reviews on antiferromagnetic spintronics
• Stacking tunable interlayer magnetism in bilayer CrI3
• Ligand-field helical luminescence in a 2D ferromagnetic insulator
• Skyrmions in the moiré of van der Waals 2D magnets
• Interplay between interlayer exchange and stacking in CrI${}_3$ bilayers
• Microscopic understanding of magnetic interactions in bilayer CrI${}_3$
• Optical Selection Rule based on Valley-Exciton Locking for 2D Valleytronics

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