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    Revealing the electronic structure of van der Waals antiferromagnetic NiPS3 through synchrotron-based μ-ARPES and alkali metal dosing

    Yifeng Cao1,2,*, Qishuo Tan3,*, Yucheng Guo2,4,*, Clóvis Guerim Vieira5, Mário S. C. Mazzoni6, Jude Laverock7, Nicholas Russo1,2, Hongze Gao3, Chris Jozwiak2 et al.

    Aaron Bostwick2, Eli Rotenberg2, Jinghua Guo2, Ming Yi4, Matheus J. S. Matos5,†, Xi Ling3,8,9,‡, and Kevin E. Smith1,3,8,§

    • *These authors contributed equally to this work.
    • †Contact author: matheusmatos@ufop.edu.br
    • ‡Contact author: xiling@bu.edu
    • §Contact author: ksmith@bu.edu

    Phys. Rev. Materials 9, 104001 – Published 8 October, 2025

    DOI: https://doi.org/10.1103/tdbk-3mv8

    Abstract

    Antiferromagnetic NiPS3 has recently emerged as a quantum material of considerable interest, thanks to the discovery of multiple new couplings involving electrons, spins, orbitals, phonons, and magnons. However, controversies and open questions persist concerning the fundamental origins of these couplings. A critical piece of information required to advance the understanding is the precise electronic band structure of NiPS3. Angle-resolved photoemission spectroscopy (ARPES), combined with alkali metal dosing (AMD), can enable us to directly observe the subtle electronic states that appear around the Fermi surface, offering valuable insights into the intriguing quantum properties and interplays of the examined material. Here, we present a comprehensive characterization and analysis of the band structure of van der Waals layered antiferromagnet NiPS3, leveraging state-of-the-art μ-ARPES measurements supported by density functional theory (DFT) calculations. Theoretical DFT results identify the orbital contributions to the observed bands, providing a precise understanding of the experimental ARPES data. Crucially, AMD enables the observation of conduction band and defect-related states above the valence band maximum in NiPS3. Furthermore, temperature dependent ARPES results across the Néel transition temperature of NiPS3 reveal that the paramagnetic and antiferromagnetic phases have nearly identical band structures, underlining the highly localized character of Ni d states. These findings substantially deepen our understanding of the electronic properties of NiPS3 and lay a vital foundation for exploring the intriguing quantum phenomena it exhibits.

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