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PreprintCC BY-NC-ND 4.0arXiv

Emergent gold-induced interfacial magnetism in monolayer FePS3

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Abstract

Owing to their atomically clean interfaces and extreme thinness, two-dimensional (2D) materials are ideal hosts for strong proximity effects, whereby contact with an adjacent material reshapes their ground state. Here, we demonstrate such an effect within a hybrid heterostructure, between the 2D antiferromagnet FePS3 and an ultrathin gold film. Rather than a passive support, the latter profoundly changes the nature of the magnetism in the 2D magnet, inducing a sizeable interfacial moment. Large-area flakes from Au-assisted exfoliation, combined with element-selective X-ray absorption mapping, enable a layer-by-layer study from monolayer to bulk, benchmarked against an inert SiO2 substrate reference. At 9 T and 5 K, the monolayer on gold shows a three-fold enhanced X-ray magnetic circular dichroism relative to SiO2, with a ∼40% reduction of the orbital-to-spin moment ratio. Resonant inelastic X-ray scattering reveals a collapse of the crystal-field (d-d) excitations and a massive spectral-weight transfer to the charge-transfer region, unveiling the microscopic mechanism behind this change. Supported by atomic multiplet calculations, we identify interfacial charge transfer and Fe 3d-Au hybridization as the origin of these effects, which decay over the first three layers and vanish at the pentalayer, establishing layer number combined with substrate engineering as an atomically precise handle.

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BibTeX
@misc{buccoliero2026emergent,
  title = {{Emergent gold-induced interfacial magnetism in monolayer FePS$_3$}},
  author = {Giuseppe Buccoliero and Anita Polli and Marli dos Reis Cantarino and Rachel Nickel and Aloïs Arrighi and Roberto Sant and Tristan Riccardi and Valérie Reita and Nedjma Bendiab and Laëtitia Marty and Kurt Kummer and Johann Coraux and Nicholas B. Brookes},
  howpublished = {arXiv},
  year = {2026},
  month = oct,
  doi = {10.48550/arxiv.2610.12041},
  eprint = {2610.12041},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2610.12041},
  note = {CC BY-NC-ND 4.0},
}
RIS
TY  - UNPB
TI  - Emergent gold-induced interfacial magnetism in monolayer FePS_3
AU  - Giuseppe Buccoliero
AU  - Anita Polli
AU  - Marli dos Reis Cantarino
AU  - Rachel Nickel
AU  - Aloïs Arrighi
AU  - Roberto Sant
AU  - Tristan Riccardi
AU  - Valérie Reita
AU  - Nedjma Bendiab
AU  - Laëtitia Marty
AU  - Kurt Kummer
AU  - Johann Coraux
AU  - Nicholas B. Brookes
PY  - 2026
DA  - 2026/10/08
PB  - arXiv
DO  - 10.48550/arxiv.2610.12041
UR  - https://arxiv.org/abs/2610.12041
AB  - Owing to their atomically clean interfaces and extreme thinness, two-dimensional (2D) materials are ideal hosts for strong proximity effects, whereby contact with an adjacent material reshapes their ground state. Here, we demonstrate such an effect within a hybrid heterostructure, between the 2D antiferromagnet FePS_3 and an ultrathin gold film. Rather than a passive support, the latter profoundly changes the nature of the magnetism in the 2D magnet, inducing a sizeable interfacial moment. Large-area flakes from Au-assisted exfoliation, combined with element-selective X-ray absorption mapping, enable a layer-by-layer study from monolayer to bulk, benchmarked against an inert SiO_2 substrate reference. At 9 T and 5 K, the monolayer on gold shows a three-fold enhanced X-ray magnetic circular dichroism relative to SiO_2, with a ∼40% reduction of the orbital-to-spin moment ratio. Resonant inelastic X-ray scattering reveals a collapse of the crystal-field (d-d) excitations and a massive spectral-weight transfer to the charge-transfer region, unveiling the microscopic mechanism behind this change. Supported by atomic multiplet calculations, we identify interfacial charge transfer and Fe 3d-Au hybridization as the origin of these effects, which decay over the first three layers and vanish at the pentalayer, establishing layer number combined with substrate engineering as an atomically precise handle.
ER  -