Thickness dependence of electronic structure and optical properties of a correlated van der Waals antiferromagnet NiPS${}_3$ thin film

Abstract

We study the thickness dependence of the electronic, magnetic, and optical properties of a NiPS${}_3$ thin film, an antiferromagnetic charge-transfer insulator. Utilizing state-of-the-art advanced density functionals, we find the antiferromagnetic Zig-Zag order, the band gap, and the main peaks in the dielectric tensor are all in good agreement with the corresponding experimental values. Upon thinning, the Zig-Zag antiferromagnetic order becomes virtually degenerate with a competing Néel order, consistent with the suppression of long-range order observed by Raman spectroscopy due to strong magnetic fluctuations. Additionally, due to the robustness of the electronic band gap observed by spectroscopic ellipsometry measurements above $T_N$, we suggest that the persistence of the band gap is driven by strong electronic correlations. Other systematic changes in electronic dispersion, effective mass, and Kerr angle with thickness are also discussed. Finally, an applied external electric field is found to suppress the band gap by up to 13%, until precipitating an insulator-metal transition at a critical field value of $0.7$ eV/Å.

9 pages, 7 figures

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• Exciton-spin interactions in antiferromagnetic charge-transfer insulators
• Probing the band structure of the strongly correlated antiferromagnet NiPS3 across its phase transition
• Stabilization of zigzag order in NiPS${}_3$ via positive biquadratic interaction
• Ultrafast Dynamics of Spin-Orbit Entangled Excitons Coupled to Magnetic Ordering in van der Waals Antiferromagnet NiPS3
• Magnetic anisotropy and magnetic ordering of transition-metal phosphorus trisulfides