MulticomponentMagneto-Orbital Order and Magneto-Orbitonsin Monolayer VCl<sub>3</sub>

Van der Waals monolayers featuring magnetic states provide fundamental building blocks for artificial quantum matter. Here, we establish the emergence of a multicomponent ground state featuring magneto-orbital excitations of the 3<i>d</i><sup>2</sup>-transition metal trihalide VCl<sub>3</sub> monolayer. We show that monolayer VCl<sub>3</sub> realizes a ground state with simultaneous magnetic and orbital ordering by using density functional theory. Using first-principles methods we derive an effective Hamiltonian with intertwined spin and orbital degrees of freedom, which we demonstrate can be tuned by strain. We show that magneto-orbitons appear as the collective modes of this complex order and arise from coupled orbiton magnon excitations due to the magneto-orbital coupling in the system. Our results establish VCl<sub>3</sub> is a promising 2D material to observe emergent magneto-orbital excitations and provides a platform for multicomponent symmetry breaking.

Publication Details

Journal
Figshare
Published
2025-02-17
DOI
https://doi.org/10.1021/acs.nanolett.4c06400.s001
Primary Topic
2D Materials and Applications
Type
article
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article

MulticomponentMagneto-Orbital Order and Magneto-Orbitonsin Monolayer VCl3

Figshare
2D Materials and Applications
article

MulticomponentMagneto-Orbital Order and Magneto-Orbitonsin Monolayer VCl3

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Abstract

Van der Waals monolayers featuring magnetic states provide fundamental building blocks for artificial quantum matter. Here, we establish the emergence of a multicomponent ground state featuring magneto-orbital excitations of the 3<i>d</i><sup>2</sup>-transition metal trihalide VCl<sub>3</sub> monolayer. We show that monolayer VCl<sub>3</sub> realizes a ground state with simultaneous magnetic and orbital ordering by using density functional theory. Using first-principles methods we derive an effective Hamiltonian with intertwined spin and orbital degrees of freedom, which we demonstrate can be tuned by strain. We show that magneto-orbitons appear as the collective modes of this complex order and arise from coupled orbiton magnon excitations due to the magneto-orbital coupling in the system. Our results establish VCl<sub>3</sub> is a promising 2D material to observe emergent magneto-orbital excitations and provides a platform for multicomponent symmetry breaking.

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