Faculty Publications
Effect of Ni Deposition on CrI3 Monolayer: First-Principles Study
Document Type
Article
Keywords
2D magnetism, CrI3, Electronic structure, First-principles calculations
Journal/Book/Conference Title
Journal of Magnetism and Magnetic Materials
Volume
628
Abstract
In our recent experimental work, we demonstrated that Ni thin film deposition can be used to tune the surface magnetic states in bulk CrI3. Here, we present the results of a computational study of Ni deposition on a CrI3 monolayer. In particular, we compare structural, electronic, and magnetic properties of three different systems: a pristine CrI3 monolayer, a CrI3 monolayer with partial Ni coverage, and a CrI3 monolayer with full Ni coverage. The corresponding cells used in our calculations are Cr2I6, Cr2I6Ni1, and Cr2I6Ni3. In Cr2I6Ni1, the Ni atom is positioned over the hollow site, which corresponds to the lowest energy configuration. In Cr2I6Ni3, the three Ni atoms are positioned over the single hollow site, and over the two Cr sites. Our calculations indicate that the partial coverage of CrI3 monolayer with Ni retains the semiconducting nature of the parent compound, but results in a strong reduction of the energy band gap. At the same time, the full coverage of CrI3 monolayer with Ni results in a metallic transition, with a highly spin-polarized (possibly half-metallic) electronic structure. The magnetic alignment of the CrI3 monolayer with the deposited Ni is ferrimagnetic, due to the anti-aligned magnetic moments of Cr and Ni atoms. While the partial coverage of the CrI3 monolayer with Ni has a moderate impact on the lattice parameter of the parent compound, full coverage by Ni results in a significant increase of the lattice constant. For both partial and full coverages, the lowest energy configuration corresponds to the Ni atoms being approximately aligned with the out-of-plane coordinate of the surface iodine layer. In addition, in the full coverage mode, the Cr layer exhibits a significant shift away from the Ni atoms, effectively “detaching” the Ni / I atomic layer from the rest of the cell.
Department
Department of Physics
Original Publication Date
9-15-2025
DOI of published version
10.1016/j.jmmm.2025.173176
Recommended Citation
Sadler, Caden; Nguyen, Nhat Phat; Yan, Jia An; Stollenwerk, Andrew J.; Shand, Paul M.; He, Rui; and Lukashev, Pavel V., "Effect of Ni Deposition on CrI3 Monolayer: First-Principles Study" (2025). Faculty Publications. 6777.
https://scholarworks.uni.edu/facpub/6777
