Electron correlation effects on exchange interactions and spin excitations in 2D van der Waals materials

Abstract

Despite serious effort, the nature of the magnetic interactions and the role of electron-correlation effects in magnetic two-dimensional (2D) van der Waals materials remain elusive. Using CrI${}_3$ as a model system, we show that the calculated electronic structure including nonlocal electron correlations yields spin excitations consistent with inelastic neutron scattering measurements. Remarkably, this approach identifies an unreported correlation-enhanced interlayer super-superexchange, which rotates the magnon Dirac lines off, and introduces a gap along, the high-symmetry $\Gamma$-$K$-$M$ path. This discovery provides a different perspective on the gap opening mechanism observed in CrI${}_3$, which was previously associated with spin-orbit coupling through the Dzyaloshinskii-Moriya interaction or Kitaev interaction. Our observation elucidates the critical role of electron correlations on the spin ordering and spin dynamics in magnetic van der Waals materials and demonstrates the necessity of explicit treatment of electron correlations in the broad family of 2D magnetic materials.

arXiv comment16 pages, 8 figures

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• Self-consistently renormailzed spin-wave theory of layered ferromagnets on honeycomb lattice
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• A Self-Adaptive First-Principles Approach for Magnetic Excited States
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• Delving into the anisotropic interlayer exchange in bilayer CrI${}_3$
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