Phase-Transition-Driven Regional Distribution of Rare-Earth Ions for Multiplexed Upconversion Emissions
JACS AU(2023)
摘要
Phase transition of the polymorphs is critical for controlled synthesis and property modulation of functional materials. Upconversion emissions from an efficient hexagonal sodium rare-earth (RE) fluoride compound, beta-NaREF4, which is generally obtained from the phase transition of the cubic (alpha-) phase counterpart, are attractive for photonic applications. However, the investigation of the alpha -> beta phase transition of NaREF4 and its effect on the composition and architecture is still preliminary. Herein, we investigated the phase transition with two kinds of alpha-NaREF4 particles. Instead of a uniform composition, the beta-NaREF4 microcrystals exhibited regionally distributed RE3+ ions, in which the RE3+ with a smaller ionic radius (smaller RE3+) sandwiched the RE3+ with a larger ionic radius (larger RE3+). We unravel that the alpha-NaREF4 particles transformed to beta-NaREF4 nuclei with no controversial dissolution, and the alpha -> beta phase transition toward NaREF4 microcrystals included nucleation and growth steps. The component-dependent phase transition is corroborated with RE3+ ions from Ho3+ to Lu3+ and multiple sandwiched microcrystals were obtained, in which up to five kinds of RE components were distributed regionally. Moreover, with rational integration of luminescent RE3+ ions, a single particle with multiplexed upconversion emissions in wavelength and lifetime domains is demonstrated, which provides a unique platform for optical multiplexing applications.
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关键词
phase transition,upconversion,beta-NaREF4,optical multiplexing,core/shell microcrystal
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