Multicomponent Magneto-Orbital Order and Magneto-Orbitons in 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 3d2-transition metal trihalide VCl3 monolayer. We show that monolayer VCl3 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 VCl3 is a promising 2D material to observe emergent magneto-orbital excitations and provides a platform for multicomponent symmetry breaking.
Funding Information
  • Aalto Science Institute, Aalto University (331342, 349696, 358088)
  • Jane ja Aatos Erkon S??ti?
  • Ministero dell'Universit? e della Ricerca (ECS00000041 VITALITY-CUP E13C220010600)
  • Finnish Quantum Flagship

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