Spin-forbidden ( ) multiplet excitations and their coupling to magnetic properties are of increasing importance for magneto-optical studies of correlated materials. Nonetheless, the mechanisms for optically brightening these transitions and their generality remain poorly understood. Here, we report magnetic circular dichroism (MCD) spectroscopy on the van der Waals ferromagnet (FM) . Previously unreported spin-forbidden ( ) excitations are observed near the ligand-to-metal charge-transfer excitation threshold. The assignment of these excitations and their multiplet character is established through complementary Cr -edge resonant inelastic x-ray scattering measurements along with charge-transfer multiplet calculations and chemical trends in the chromium trihalide series ( , Cl, Br, I). We utilize the high sensitivity of MCD spectroscopy to study the thickness-dependent optical response. The spin-forbidden excitations remain robust down to the monolayer limit, and we observe a significant magnetic-field dependence of the MCD spectrum across the antiferromagnetic-to-FM transition in few-layer samples. We preliminarily attribute this behavior to changes in the metal-ligand covalency with magnetic state. Our results clarify the magneto-optical response of and identify covalency as a central mechanism for the brightening and field tunability of spin-forbidden multiplet excitations.
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This content will become publicly available on January 1, 2027
Spin-orbit coupling controlled two-dimensional magnetism in chromium trihalides
( = Cl, Br, I) have the same crystal structure and Hamiltonian but different ligand spin-orbit coupling (SOC) constant , providing an excellent material platform exploring for exotic two-dimensional (2D) spin orders. Their microscopic mechanism underlying 2D spin physics remain unestablished, along with experimental corroboration of Kitaev exchange interaction, central to realizing topological quantum spin liquids. Finding direct evidence for Kitaev interaction and determining its value has been an essential but formidable challenge in Kitaev physics. Here we report the direct Kitaev interaction signature in magnetic anisotropy measured by ferromagnetic resonance (FMR) spectroscopy. We present measured values of Heisenberg , Kitaev , and off-diagonal symmetric exchange interactions in determined using FMR and exact diagonalization. and exhibit dominant dependencies on , indicating its central role in 2D magnetism. Our study provides a foundation for designing 2D magnetic materials exhibiting novel behaviors by tuning intrinsic material parameters such as SOC.
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- Award ID(s):
- 2011876
- PAR ID:
- 10682998
- Publisher / Repository:
- APS
- Date Published:
- Journal Name:
- Physical Review B
- Volume:
- 113
- Issue:
- 1
- ISSN:
- 2469-9950
- Page Range / eLocation ID:
- 014401
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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