Mechanochemistry-driven engineering of 0D/3D heterostructure for designing highly luminescent Cs-Pb-Br perovskites

Embedding metal-halide perovskite particles within an insulating host matrix has proven to be an effective strategy for revealing the outstanding luminescence properties of perovskites as an emerging class of light emitters. Particularly, unexpected bright green emission observed in a nominally pure zero-dimensional cesium-lead-bromide perovskite (Cs₄PbBr₆) has triggered intensive research in better understanding the serendipitous incorporation of emissive guest species within the Cs₄PbBr₆ host. However, a limited controllability over such heterostructural configurations in conventional solution-based synthesis methods has limited the degree of freedom in designing synthesis routes for accessing different structural and compositional configurations of these host-guest species. In this study, we provide means of enhancing the luminescence properties in the nominal Cs₄PbBr₆ powder through a guided heterostructural configuration engineering enabled by solid-state mechanochemical synthesis. Realized by an in-depth study on time-dependent evaluation of optical and structural properties during the synthesis of Cs₄PbBr₆, our target-designed synthesis protocol to promote the endotaxial formation of Cs₄PbBr₆/CsPbBr₃ heterostructures provides key insights for understanding and designing kinetics-guided syntheses of highly luminescent perovskite emitters for light-emitting applications.