Ligand-field helical luminescence in a 2D ferromagnetic insulator

Abstract

Bulk chromium triiodide (CrI${}_3$) has long been known as a layered van der Waals ferromagnet. However, its monolayer form was only recently isolated and confirmed to be a truly two-dimensional (2D) ferromagnet, providing a new platform for investigating light-matter interactions and magneto-optical phenomena in the atomically thin limit. Here, we report spontaneous circularly polarized photoluminescence in monolayer CrI${}_3$ under linearly polarized excitation, with helicity determined by the monolayer magnetization direction. In contrast, the bilayer CrI${}_3$ photoluminescence exhibits vanishing circular polarization, supporting the recently uncovered anomalous antiferromagnetic interlayer coupling in CrI${}_3$ bilayers. Distinct from the Wannier-Mott excitons that dominate the optical response in well-known 2D van der Waals semiconductors, our absorption and layer-dependent photoluminescence measurements reveal the importance of ligand-field and charge-transfer transitions to the optoelectronic response of atomically thin CrI${}_3$. We attribute the photoluminescence to a parity-forbidden d-d transition characteristic of Cr${}^{3+}$ complexes, which displays broad linewidth due to strong vibronic coupling and thickness-independent peak energy due to its localized molecular orbital nature.

12 pages of main text, 4 figures, 6 pages of supplementary materials

References in corpus (2)

• Ising-Type Magnetic Ordering in Atomically Thin FePS3
• Optical Properties of III-Mn-V Ferromagnetic Semiconductors

Cited by in corpus (121)

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