Intrinsic localized excitons in MoSe₂/CrSBr heterostructures

We present a comprehensive investigation of optical properties in MoSe₂/CrSBr heterostructures, unveiling the presence of localized excitons represented by a new emission feature, X^*. We demonstrate through temperature- and power-dependent photoluminescence spectroscopy that X^* originates from excitons confined by intrinsic defects within the CrSBr layer. The valley polarization of X^* and trion peaks displays opposite polarity under a magnetic field, which closely correlates with the magnetic order of CrSBr. This is attributed to spin-dependent charge transfer mechanisms across the heterointerface, supported by density functional theory calculations revealing a type-II band alignment and spin-polarized band structures. Furthermore, the strong in-plane anisotropy of CrSBr induces unique polarization-dependent responses in MoSe₂ emissions. Our study highlights the crucial role of defects in shaping excitonic properties. It offers valuable insights into spectral-resolved proximity effects in van der Waals heterostructures between semiconductor and magnet, contributing to advancing spintronic and valleytronic devices.