Magnetically confined surface and bulk excitons in a layered antiferromagnet

The discovery of two-dimensional van der Waals magnets has greatly expanded our ability to create and control nanoscale quantum phases. A unique capability emerges when a two-dimensional magnet is also a semiconductor that features tightly bound excitons with large oscillator strengths that fundamentally determine the optical response and are tunable with magnetic fields. Here we report a previously unidentified type of optical excitation—a magnetic surface exciton—enabled by the antiferromagnetic spin correlations that confine excitons to the surface of CrSBr. Magnetic surface excitons exhibit stronger Coulomb attraction, leading to a higher binding energy than excitons confined in bulk layers, and profoundly alter the optical response of few-layer crystals. Distinct magnetic confinement of surface and bulk excitons is established by layer- and temperature-dependent exciton reflection spectroscopy and corroborated by ab initio many-body perturbation theory calculations. By quenching interlayer excitonic interactions, the antiferromagnetic order of CrSBr strictly confines the bound electron–hole pairs within the same layer, regardless of the total number of layers. Our work unveils unique confined excitons in a layered antiferromagnet, highlighting magnetic interactions as a vital approach for nanoscale quantum confinement, from few layers to the bulk limit. The emergence of magnetically confined surface excitons enabled by antiferromagnetic spin correlations is reported, which leads to the confinement of excitons to the surface of layered antiferromagnet CrSBr.