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

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.