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An HBr‐assisted slow cooling method is developed for the growth of centimeter‐sized Cs4PbBr6 crystals. The obtained crystals show strong green photoluminescence with absolute photoluminescence quantum yields up to 97%. More importantly, the evolution process and structural characterizations support that the nonstoichiometry of initial Cs4PbBr6 crystals induce the formation of nanosized CsPbBr3 nanocrystals...
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