Unconventional and Fragile Magnetic Exciton in a van der Waals Quantum Magnet
arXiv:2607.27695
The study investigates a magnetic exciton in the van der Waals antiferromagnet NiPS3, showing that its sharp, optically bright emission is quickly quenched by modest hydrostatic pressure, revealing that its brightness arises from a higher‑order correlated mechanism rather than disorder or simple magnetic weakening.
Abstract
The recently discovered magnetic exciton in the van der Waals (vdW) antiferromagnet NiPS3 exemplifies these phenomena, exhibiting several distinctive characteristics. Despite extensive investigation, much of its physics remains unresolved, with key questions about why the NiPS3 magnetic exciton is so sharp and optically bright despite the nominally spin-forbidden transition, posing significant challenges to a proper understanding and practical manipulation of the exciton. An urgent question is to what extent it is due to chemical disorder, magnetic weakening, lattice modification, or intrinsic instability of the bright exciton itself: answers to which will put stringent constraints on possible theoretical models. Here we address these questions using hydrostatic pressure as a clean, continuous, reversible, and in-situ tuning parameter. We find that the sharp photoluminescence peak is drastically suppressed by as little as 0.4 GPa and completely quenched by 1.5 GPa, with demonstrating its reversibility. Crucially, this bright-to-dark conversion occurs without magnetic, crystallographic, or electronic reconstruction despite an increase in the Neel temperature, as established by Raman, X-ray absorption, nuclear magnetic resonance spectroscopy, and first-principles many-body calculations. Our results demonstrate that the optical brightness of the magnetic exciton is independent of chemical disorder, lattice expansion, and weakening of magnetic order, indicating that a higher-order correlated mechanism governs the bright exciton. We further propose experimentally constrained microscopic scenarios involving exciton pairing, crystal-field-controlled spin-orbit mixing, and symmetry breaking, providing a framework for future tests of entangled magnetic exciton in correlated quantum magnets.
Our findings indicate that the sharp coherence of the entangled magnetic exciton benefits from its delicate quantum nature, and its optical brightness can be activated by exciton pairing or spin-orbit coupling, while its fragility under external control is achievable through a high-order perturbation rather than a first-order transition