Sliding multiferrocity in van der Waals layered CrI$_2$

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Main Authors: Yu, Hui-Shi, Ni, Xiao-Sheng, Cao, Kun
Format: Preprint
Published: 2025
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author Yu, Hui-Shi
Ni, Xiao-Sheng
Cao, Kun
author_facet Yu, Hui-Shi
Ni, Xiao-Sheng
Cao, Kun
contents Understanding magnetoelectric coupling in emerging van der Waals multiferroics is crucial for developing atomically thin spintronic devices. Here, we present a comprehensive first-principles investigation of magnetoelectric coupling in orthorhombic CrI$_2$. Monte Carlo simulations based on DFT-calculated magnetic exchange interactions suggest a proper-screw helimagnetic ground state with a Néel temperature consistent with experimental observations. A ferroelectric switching pathway driven by interlayer sliding is predicted, featuring a low switching energy barrier and out-of-plane ferroelectric polarization. To quantitatively characterize the magnetoelectric effect in orthorhombic CrI$_2$ and its microscopic origin, we evaluate the spin-driven polarization using the paramagnetic phase as a reference alongside the magnetoelectric tensor method. The extracted spin-driven polarization aligns along the $z$-axis, with its origin dominated by the exchange-striction mechanism. Although in-plane components of the total polarization in the bulk vanish due to global symmetry constraints, each CrI$_2$ single layer exhibits local electric polarization along the $x$ direction, arising from the generalized spin-current mechanism, which couples spin chirality to the electric polarization. As a result, we further predict that a proper-screw helimagnetic state may persist in monolayer CrI$_2$, with its charity reversable by switching the in-plane electric polarization through applying external electric field, providing another promising candidate for electrical control of two-dimensional multiferroics.
format Preprint
id arxiv_https___arxiv_org_abs_2507_17562
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Sliding multiferrocity in van der Waals layered CrI$_2$
Yu, Hui-Shi
Ni, Xiao-Sheng
Cao, Kun
Materials Science
Strongly Correlated Electrons
Understanding magnetoelectric coupling in emerging van der Waals multiferroics is crucial for developing atomically thin spintronic devices. Here, we present a comprehensive first-principles investigation of magnetoelectric coupling in orthorhombic CrI$_2$. Monte Carlo simulations based on DFT-calculated magnetic exchange interactions suggest a proper-screw helimagnetic ground state with a Néel temperature consistent with experimental observations. A ferroelectric switching pathway driven by interlayer sliding is predicted, featuring a low switching energy barrier and out-of-plane ferroelectric polarization. To quantitatively characterize the magnetoelectric effect in orthorhombic CrI$_2$ and its microscopic origin, we evaluate the spin-driven polarization using the paramagnetic phase as a reference alongside the magnetoelectric tensor method. The extracted spin-driven polarization aligns along the $z$-axis, with its origin dominated by the exchange-striction mechanism. Although in-plane components of the total polarization in the bulk vanish due to global symmetry constraints, each CrI$_2$ single layer exhibits local electric polarization along the $x$ direction, arising from the generalized spin-current mechanism, which couples spin chirality to the electric polarization. As a result, we further predict that a proper-screw helimagnetic state may persist in monolayer CrI$_2$, with its charity reversable by switching the in-plane electric polarization through applying external electric field, providing another promising candidate for electrical control of two-dimensional multiferroics.
title Sliding multiferrocity in van der Waals layered CrI$_2$
topic Materials Science
Strongly Correlated Electrons
url https://arxiv.org/abs/2507.17562