Hydrothermal Synthesis and Solid-State Laser Refrigeration of Ytterbium-Doped Potassium Lutetium Fluoride (KLF) Microcrystals

Xia, Xiaojing; Pant, Anupum; Zhou, Xuezhe; Dobretsova, Elena; Bard, Alex; Lim, Matthew B.; Roh, Joo Yeon; Gamelin, Daniel R.; Pauzauskie, Peter J.

doi:10.26434/chemrxiv.12330737.v1

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“…While KYF can form in multiple stoichiometries, the KY 3 F 10 stoichiometry forms in this case because it is stable in the cubic crystal phase and has the lowest potassium / yttrium ion ratio. 34 By varying the amount of time spent incubating in the native solution before filtering and transfering to the KF solution (t inc ), we can observe how much sodium has incorporated into the gel in that time and how much YF 3 remains, which we can observe after converting to KYF. As t inc increases from 15 minutes to two hours, we observe the proportion of the sodium phase to increase linearly with a corresponding linear decrease in the relative amount of material that incorporates potassium (Figure 3C).…”

Section: Resultsmentioning

confidence: 99%

Multi-Step Crystallization and Chemical Evolution of Sodium Yttrium Fluoride

Pauzauskie

Bard

Felsted

et al. 2021

Preprint

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Two-step crystallization mechanisms based on spinodal decomposition followed by nucleation are commonly observed both in the laboratory and in nature. While this pathway may require chemical reactions, subsequent nucleation and growth are often considered as separate, discrete events from the reaction itself. Recent work has also shown a distinct intermediate step involving the formation of an amorphous aggregate. Here we report a novel four-step mechanism in the aqueous synthesis of sodium yttrium fluoride involving 1) the segregation of aqueous ions into a dense liquid phase, 2) the formation of an amorphous aggregate, 3) nucleation of a cubic YF3 phase, and 4) subsequent solid-state diffusion of sodium and fluoride ions to form a final NaYF4 phase. The final step involves a continuous, gradual change of the solid phase’s chemical stoichiometry from YF3 toward NaYF4. Unlike previously studied nucleation and growth mechanisms, the stoichiometry of the final solid phase evolves throughout the crystallization process rather than being determined at nucleation. This novel four-step mechanism provides a new perspective into the nucleation and growth of many other crystalline materials given the ubiquity of nonstoichiometric compounds in nature.

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Section: Resultsmentioning

confidence: 99%