Imaging Thermally Fluctuating Neel Vectors in van der Waals Antiferromagnet NiPS3

Studying antiferromagnetic domains is essential for fundamental physics and potential spintronics applications. Despite their importance, few systematic studies have been performed on antiferromagnet (AFM) domains with high spatial resolution in van der Waals (vdW) materials, and direct probing of the Neel vectors remains challenging. In this work, we found multidomain states in the vdW AFM NiPS3, a material extensively investigated for its unique magnetic exciton. We employed photoemission electron microscopy combined with the X-ray magnetic linear dichroism (XMLD-PEEM) to image the NiPS3's magnetic structure. The nanometer-spatial resolution of XMLD-PEEM allows us to determine local Neel vector orientations and discover thermally fluctuating Neel vectors that are independent of the crystal symmetry even at 65 K, well below the T-N of 155 K. We demonstrate that an in-plane orbital moment of the Ni ion is responsible for the weak magnetocrystalline anisotropy. The observed thermal fluctuations of the antiferromagnetic domains may explain the broadening of magnetic exciton peaks at higher temperatures.