Dimensionality dependent electronic structure of the exfoliated van der Waals antiferromagnet NiPS${}_3$

Abstract

Resonant Inelastic X-ray Scattering (RIXS) was used to measure the local electronic structure in few-layer exfoliated flakes of the van der Waals antiferromagnet NiPS${}_3$. The resulting spectra show a systematic softening and broadening of $Ni{S}_6$ multiplet excitations with decreasing layer count from the bulk to three atomic layers (3L). These trends are driven by a decrease in the transition metal-ligand and ligand-ligand hopping integrals, and in the charge-transfer energy: $\Delta$ = 0.60 eV in the bulk and 0.22 eV in 3L NiPS${}_3$. Relevant intralayer magnetic exchange integrals computed from the electronic parameters exhibit a systematic decrease in the average interaction strength with thickness and place 2D NiPS${}_3$ close to the phase boundary between stripy and spiral antiferromagnetic order, which may explain the apparent vanishing of long-range order in the 2D limit. This study explicitly demonstrates the influence of $inter$layer electronic interactions on $intra$layer ones in insulating magnets. As a consequence, the magnetic Hamiltonian in few-layer insulating magnets can be significantly different from that in the bulk.

5 pages, 4 figures; additional 9 pages and 13 figures of supplementary information

References in corpus (8)

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• Correlations in the Electronic Structure of van der Waals NiPS${}_3$ Crystals: An X-Ray Absorption and Resonant Photoelectron Spectroscopy Study

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• Exploring Quantum Materials with Resonant Inelastic X-Ray Scattering
• Dimensionality crossover to 2D vestigial nematicity from 3D zigzag antiferromagnetism in an XY-type honeycomb van der Waals magnet
• Dispersive dark excitons in van der Waals ferromagnet CrI3