Multiferroic-Enabled Magnetic-Excitons in 2D Quantum-Entangled Van der Waals Antiferromagnet NiI₂

Matter–light interaction is at the center of diverse research fields from quantum optics to condensed matter physics, opening new fields like laser physics. A magnetic exciton is one such rare example found in magnetic insulators. However, it is relatively rare to observe that external variables control matter-light interaction. Here, it is reported that the broken inversion symmetry of multiferroicity can act as an external knob enabling magnetic excitons in the van der Waals antiferromagnet NiI₂. It is further discovered that this magnetic exciton arises from a transition between Zhang–Rice-triplet and Zhang–Rice-singlet fundamentally quantum-entangled states. This quantum entanglement produces an ultrasharp optical exciton peak at 1.384 eV with a 5 meV linewidth. The work demonstrates that NiI₂ is 2D magnetically ordered with an intrinsically quantum-entangled ground state.