Local Environments of Dilute Activator Ions in the Solid-State Lighting Phosphor Y<sub>3–<i>x</i></sub>Ce<sub><i>x</i></sub>Al<sub>5</sub>O<sub>12</sub>

Abstract

The oxide garnet Y<sub>3</sub>Al<sub>5</sub>O<sub>12</sub> (YAG), when substituted with a few percent of the activator ion Ce<sup>3+</sup> to replace Y<sup>3+</sup>, is a luminescent material that is nearly ideal for phosphor-converted solid-state white lighting. The local environments of the small number of substituted Ce<sup>3+</sup> ions are known to critically influence the optical properties of the phosphor. Using a combination of powerful experimental methods, the nature of these local environments is determined and is correlated with the macroscopic luminescent properties of Ce-substituted YAG. The rigidity of the garnet structure is established and is shown to play a key role in the high quantum yield and in the resistance toward thermal quenching of luminescence. Local structural probes reveal compression of the Ce<sup>3+</sup> local environments by the rigid YAG structure, which gives rise to the unusually large crystal-field splitting, and hence yellow emission. Effective design rules for finding new phosphor materials inferred from the results establish that efficient phosphors require rigid, highly three-dimensionally connected host structures with simple compositions that manifest a low number of phonon modes, and low activator ion concentrations to avoid quenching

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