Influence of orbital character on the ground state electronic properties in the van Der Waals transition metal iodides VI3 and CrI3

Alessandro De Vita, Thao Thi Phuong Nguyen, Roberto Sant, Gian Marco Pierantozzi, Danila Amoroso, Chiara Bigi, Vincent Polewczyk, Giovanni Vinai, Loi T. Nguyen, Tai Kong, Jun Fujii, Ivana Vobornik, Nicholas B. Brookes, Giorgio Rossi, Robert J. Cava, Federico Mazzola, Kunihiko Yamauchi, Silvia Picozzi, Giancarlo Panaccione*

*Corresponding author for this work

Research output: Contribution to journalLetterpeer-review

13 Citations (Scopus)
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Abstract

Two-dimensional van der Waals magnetic semiconductors display emergent chemical and physical properties and hold promise for novel optical, electronic and magnetic “few-layers” functionalities. Transition-metal iodides such as CrI3 and VI3 are relevant for future electronic and spintronic applications; however, detailed experimental information on their ground state electronic properties is lacking often due to their challenging chemical environment. By combining X-ray electron spectroscopies and first-principles calculations, we report a complete determination of CrI3 and VI3 electronic ground states. We show that the transition metal-induced orbital filling drives the stabilization of distinct electronic phases: a wide bandgap in CrI3 and a Mott insulating state in VI3. Comparison of surface-sensitive (angular-resolved photoemission spectroscopy) and bulk-sensitive (X-ray absorption spectroscopy) measurements in VI3 reveals a surface-only V2+ oxidation state, suggesting that ground state electronic properties are strongly influenced by dimensionality effects. Our results have direct implications in band engineering and layer-dependent properties of two-dimensional systems.
Original languageEnglish
Pages (from-to)7034-7041
Number of pages8
JournalNano Letters
Volume22
Issue number17
Early online date30 Aug 2022
DOIs
Publication statusPublished - 14 Sept 2022

Keywords

  • Electronic structure
  • van der Waals systems
  • ARPES
  • DFT

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