Interacting donor-acceptor pairs as the origin of coupled spin-optical signals in hexagonal boron nitride

Abstract

Optically addressable spin defects in hexagonal boron nitride hold promise for room-temperature quantum technologies, but their microscopic identities remain largely unknown. Using first principles calculations, we show that coupled spin optical signals arise from interacting donor acceptor pairs, not the commonly believed isolated defects. Intra and inter pair separations control charge transfer, electronic structure, and spin coupling, thereby greatly modulating zero phonon lines, phonon sidebands, lifetimes, and the sign of optically detected magnetic resonance contrast. Importantly, we identify two distinct charge-state-dependent coupling regimes and extend this picture to correlated defect ensembles, explaining the wide diversity of experimental observations. Our results establish a microscopic framework for coupled defect behavior and provide design principles for spin-active quantum emitters in wide bandgap semiconductors.