In this work, highly luminescent quaternary CuNiInS nanocrystals (NCs) are put forward as a good prototype for investigating defect-induced room temperature ferromagnetism. A ferromagnetic Ni cation can preserve the strong luminescence of NCs without introducing intermediate energy levels in the center of the forbidden band. The strong luminescence of NCs is used as an indicator for monitoring the concentration of vacancy defects inside them, facilitating the investigation of the origin of room temperature ferromagnetism in CuNiInS NCs. Our results reveal that the patching of Cu vacancies [Formula: see text] with Ni will result in bound magnetic polarons composed of both [Formula: see text] and a substitution of Cu by Ni [Formula: see text] giving rise to the room temperature ferromagnetism of CuNiInS NCs. Either the ferromagnetic Ni or the non-ferromagnetic Cu cation can tune the magnetism of CuNiInS NCs because of the change of bound magnetic polaron concentration at the altered concentration ratio of [Formula: see text] and [Formula: see text].
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