Competing multiferroic phases in monolayer and few-layer NiI${}_2$

Abstract

A recent experiment reported type-II multiferroicity in monolayer (ML) NiI${}_2$ based on a presumed spiral magnetic configuration (Spiral-B), which is, as we found here, under debate in the ML limit. Freestanding ML NiI${}_2$ breaks its C${}_3$ symmetry, as it prefers a striped antiferromagnetic order (AABB-AFM) along with an intralayer antiferroelectric (AFE) order. However, substrate confinement may preserve the C${}_3$ symmetry and/or apply tensile strain to the ML. This leads to another spiral magnetic order (Spiral-$I{V}^X$), while 2L shows a different order (Spiral-$V^Y$) and Spiral-B dominates in thicker layers. Thus, three multiferroic phases, namely, Spiral-B+FE, Spiral-$I{V}^X$ +FE, Spiral-$V^Y$+FE, and an anti-multiferroic AABB-AFM+AFE one, show layer-thickness-dependent and geometry-dependent dominance, ascribed to competitions among thickness-dependent Kitaev, biquadratic, and Heisenberg spin-exchange interactions and single-ion magnetic anisotropy. Our theoretical results clarify the debate on the multiferroicity of ML NiI${}_2$ and shed light on the role of layer-stacking-induced changes in noncollinear spin-exchange interactions and magnetic anisotropy in thickness-dependent magnetism.

48 pages, 21 figures

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• Bimeron Crystals by a Linearly Polarized AC Electric Field in Frustrated Magnets
• Magnetodielectric Properties in Two Dimensional Magnetic Insulators
• Sizable Ligand-Mediated Bond-Dependent Interactions in a Spin-1 Triangular Antiferromagnet NiI${}_2$
• Dimensional crossover and local strain induced deflection of the spin spiral state in multiferroic NiI2