Observation of giant surface second harmonic generation coupled to nematic orders in the van der Waals antiferromagnet FePS${}_3$

Abstract

Second harmonic generation has been applied to study lattice, electronic and magnetic proprieties in atomically thin materials. However, inversion symmetry breaking is usually required for the materials to generate a large signal. In this work, we report a giant second-harmonic generation that arises below the Néel temperature in few-layer centrosymmetric FePS${}_3$. Layer-dependent study indicates the detected signal is from the second-order nonlinearity of the surface. The magnetism-induced surface second-harmonic response is two orders of magnitude larger than those reported in other magnetic systems, with the surface nonlinear susceptibility reaching 0.08--0.13 nm${}^2$/V in 2 L--5 L samples. By combing linear dichroism and second harmonic generation experiments, we further confirm the giant second-harmonic generation is coupled to nematic orders formed by the three possible Zigzag antiferromagnetic domains. Our study shows that the surface second-harmonic generation is also a sensitive tool to study antiferromagnetic states in centrosymmetric atomically thin materials.

to appear in Nano Letters

References in corpus (8)

• Ising-Type Magnetic Ordering in Atomically Thin FePS3
• Coupling the valley degree of freedom to antiferromagnetic order
• Magnetoelectric MnPS3 thiophosphate as a new candidate for ferrotoroidicity
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• Possible persistence of multiferroic order down to bilayer limit of van der Waals material NiI${}_2$
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• On-site and inter-site Hubbard corrections in magnetic monolayers: The case of FePS${}_3$ and CrI${}_3$
• Exciton-magnon splitting in van der Waals antiferromagnet MnPS${}_3$ unveiled by second-harmonic generation
• Giant Magneto-Optical Schäfer-Hubert Effect in Two-Dimensional van der Waals Antiferromagnets \textit{M}PS${}_3$ (\textit{M}=Mn, Fe, Ni)
• Regularized lattice theory for spatially dispersive nonlinear optical conductivities
• Floquet formulation of the dynamical Berry-phase approach to non-linear optics in extended systems
• Advancements in Entangled Photon Pairs in 2D Van der Waals Materials for On-chip Quantum Applications
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