Atomic-level defects in van der Waals (vdW) materials are essential building blocks for quantum technologies and quantum sensing applications. The layered magnetic semiconductor CrSBr is an outstanding candidate for exploring optically active defects because of a direct gap, in addition to a rich magnetic phase diagram, including a recently hypothesized defect-induced magnetic order at low temperature. Here, we show optically active defects in CrSBr that are probes of the local magnetic environment. We observe a spectrally narrow (1 meV) defect emission in CrSBr that is correlated with both the bulk magnetic order and an additional low-temperature, defect-induced magnetic order. We elucidate the origin of this magnetic order in the context of local and nonlocal exchange coupling effects. Our work establishes vdW magnets like CrSBr as an exceptional platform to optically study defects that are correlated with the magnetic lattice. We anticipate that controlled defect creation allows for tailor-made complex magnetic textures and phases with direct optical access.

College of Letters and Science UCLA Los Angeles California90095 United States

Department of Electrical and Computer Engineering The University of Texas at Austin Austin Texas78712 United States

Department of Electrical Engineering City College of the City University of New York New York New York10031 United States

Department of Inorganic Chemistry University of Chemistry and Technology Prague Technická 5 166 28Prague 6 Czech Republic

Department of Materials Science and Engineering Massachusetts Institute of Technology Cambridge Massachusetts02139 United States

Department of Physics City College of New York New York New York10031 United States

Department of Physics Massachusetts Institute of Technology Cambridge Massachusetts02139 United States

Department of Physics The Graduate Center City University of New York New York New York10016 United States

Francis Bitter Magnet Laboratory Plasma Science and Fusion Center Massachusetts Institute of Technology Cambridge Massachusetts02139 United States

John A Paulson School of Engineering and Applied Sciences Harvard University Cambridge Massachusetts02138 United States

Photonics Initiative CUNY Advanced Science Research Center New York New York10031 United States

Physics Program Graduate Center City University of New York New York New York10026 United States

QuTech Delft University of Technology 2600 GADelft The Netherlands

U S Army CCDC Army Research Laboratory Adelphi Maryland20783 United States

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