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Controlled colloidal synthesis and structure–property–stability relationships in lead-free CsMBr3 (M = Mn; Fe; Ni) perovskite nanocrystals
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DOI：10.1039/D6RA02065H.png)
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Abstract
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Transition-metal halide perovskites of the form CsMBr3 (M = Mn; Fe; Ni) are emerging as attractive lead-free alternatives for optoelectronic applications; offering composition-tunable electronic structures; strong light–matter interactions; and enhanced environmental stability compared with hybrid lead halide perovskites. Despite this promise; the reliable synthesis of phase-pure; highly crystalline CsMBr3 nanocrystals (NCs) remains challenging due to their pronounced sensitivity to reaction temperature; precursor reactivity; and surface-ligand chemistry. Here; we report a reproducible and optimized colloidal hot-injection strategy for the synthesis of CsMnBr3; CsFeBr3; and CsNiBr3 NCs; and systematically elucidate the influence of reaction temperature and growth time on their structural; morphological; and optical properties. X-ray diffraction confirms the formation of phase-pure hexagonal CsMBr3 (P63/mmc) across all compositions under optimized conditions. Transmission electron microscopy reveals uniform nanocrystal morphologies with narrow size distributions and well-resolved lattice fringes; indicative of high crystallinity. Optical studies; including UV-vis absorption; steady-state photoluminescence; and time-resolved photoluminescence; demonstrate composition-dependent absorption characteristics and exciton recombination dynamics; reflecting the role of the transition metal cation in tuning optoelectronic behaviour. Time-dependent UV-vis and XRD analyses further reveal notable ambient stability over one month; with structural and optical degradation becoming evident only after prolonged exposure beyond 46 days; demonstrating stability far superior to that of equivalent untreated or unencapsulated CsPbBr3 perovskite NCs. X-ray photoelectron spectroscopy confirms correct metal incorporation and stable metal-halide bonding environments; while thermogravimetric analysis uncovers distinct; composition-dependent thermal decomposition pathways. Collectively; this work establishes a clear structure–property–stability relationship for CsMBr3 nanocrystals and provides a robust synthetic framework for advancing next-generation; lead-free perovskite nanomaterials for optoelectronic applications.
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