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Two dimensional (2D) semiconductors present unique opportunities tointertwine optical and magnetic functionalities and to tune these performancesthrough defects and dopants. In 2D semiconductors, the properties of excitonsoften vary due to the underlying magnetic order, but the modification of theirmagnetic properties by excitonic processes remains difficult to achieve. Here,we integrate exciton pumping into a quantum sensing protocol onnitrogen-vacancy centers in diamond to image the optically-induced transientstray fields in few-layer, antiferromagnetic CrCl$_3$. We discover that excitonrecombination enhances the in-plane magnetization of the CrCl$_3$ layers, withan outsized effect in the surface monolayers and when the surface isunencapsulated. Concomitantly, time-resolved photoluminescence measurementsreveal that a defect-assisted Auger recombination dominates for atomically thinCrCl$_3$ with tightly localized, nearly forbidden excitons and amplifiedsurface-to-volume ratio. These experimental signatures establish themagnetically enhanced state to result from an exciton-activated electrontransfer between surface impurities and the spin-polarized conduction band.Density functional theory calculations identify that the mediating impuritystate could originate from oxygen adsorbates with spins antiparallel to themagnetization of their host layer. Our work unambiguously demonstrates thetunability of single intrinsic magnetic layers via defect engineering and opensa pathway to dynamically reconfigure these effects in devices through opticalcontrol.

Enhanced Magnetization by Defect-Assisted Exciton Recombination in Atomically Thin CrCl$_3$