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Antiferromagnets are promising materials for future opto-spintronicapplications since they show spin dynamics in the THz range and no netmagnetization. Recently, layered van der Waals (vdW) antiferromagnets have beenreported, which combine low-dimensional excitonic properties with complexspin-structure. While various methods for the fabrication of vdW 2D crystalsexist, formation of large area and continuous thin films is challenging becauseof either limited scalability, synthetic complexity, or low opto-spintronicquality of the final material. Here, we fabricate centimeter-scale thin filmsof the van der Waals 2D antiferromagnetic material NiPS3, which we prepareusing a crystal ink made from liquid phase exfoliation (LPE). We performstatistical atomic force microscopy (AFM) and scanning electron microscopy(SEM) to characterize and control the lateral size and number of layers throughthis ink-based fabrication. Using ultrafast optical spectroscopy at cryogenictemperatures, we resolve the dynamics of photoexcited excitons. We findantiferromagnetic spin arrangement and spin-entangled Zhang-Rice multipletexcitons with lifetimes in the nanosecond range, as well as ultranarrowemission linewidths, despite the disordered nature of our films. Thus, ourfindings demonstrate scalable thin-film fabrication of high-quality NiPS3,which is crucial for translating this 2D antiferromagnetic material intospintronic and nanoscale memory devices and further exploring its complexspin-light coupled states.

Solution-processed NiPS3 thin films from Liquid Exfoliated Inks with Long-Lived Spin-Entangled Excitons