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.

Influence of Orbital Character on the Ground State Electronic Properties in the van Der Waals Transition Metal Iodides VI3 and CrI3 / A. DE VITA, T. Thi Phuong Nguyen, R. Sant, G. Marco Pierantozzi, D. Amoroso, C. Bigi, V. Polewczyk, G. Vinai, L.T. Nguyen, T. Kong, J. Fujii, I. Vobornik, N.B. Brookes, G. Rossi, R.J. Cava, F. Mazzola, K. Yamauchi, S. Picozzi, A. Giancarlo Panaccione. - In: NANO LETTERS. - ISSN 1530-6984. - (2022). [Epub ahead of print] [10.1021/acs.nanolett.2c01922]

Influence of Orbital Character on the Ground State Electronic Properties in the van Der Waals Transition Metal Iodides VI3 and CrI3

A. DE VITA
Primo
;
C. Bigi;G. Rossi;
2022

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.
Electronic structure; van der Waals systems; ARPES; DFT
Settore FIS/01 - Fisica Sperimentale
Settore FIS/03 - Fisica della Materia
30-ago-2022
Article (author)
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Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/2434/936877
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