Anisotropic hybridization probed by polarization dependent x-ray absorption spectroscopy in VI3 van der Waals Mott ferromagnet

Polarization dependent x-ray absorption spectroscopy was used to study the magnetic ground state and the orbital occupation in bulk-phase VI3 van der Waals crystals below and above the ferromagnetic and structural transitions. X-ray natural linear dichroism and x-ray magnetic circular dichroism spectra acquired at the V L2,3 edges are compared against multiplet cluster calculations within the frame of the ligand field theory to quantify the intra-atomic electronic interactions at play and evaluate the effects of symmetry reduction occurring in a trigonally distorted VI6 unit. We observed a non zero linear dichroism proving the presence of an anisotropic charge density distribution around the V3+ ion due to the unbalanced hybridization between the vanadium and the ligand states. Such hybridization acts as an effective trigonal crystal field, slightly lifting the degeneracy of the t2g2 ground state. However, the energy splitting associated to the distortion underestimates the experimental band gap, suggesting that the insulating ground state is stabilized by Mott correlation effects rather than via a Jahn–Teller mechanism. Our results clarify the role of the distortion in VI3 and establish a benchmark for the study of the spectroscopic properties of other van der Waals halides, including emerging 2D materials with mono and few-layers thickness, whose fundamental properties might be altered by reduced dimensions and interface proximity.

• Publication year

  2023

• Venue

  Journal of Physics: Condensed Matter

• Publication date

  2023-05-09

• Fields of study

  Medicine, Physics

• Identifiers
  DOI 10.1088/1361-648X/ace1bfarXiv 2305.05360PMID 37364587
• External record

  Open on Semantic Scholar

• Source metadata

  Semantic Scholar, PubMed

• No claims are published for this paper.

• No concepts are published for this paper.

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