Abstract
Mn4+-activated oxide-fluoride phosphors are attractive for application in a wide range of solid-state lighting devices because of their distinct red emission at about 630 nm and the abundant storage of Mn ions. However, the zero-phonon line (ZPL) of Mn4+ ions is too weak to be detected in most host materials due to the magnetic dipole nature. In this article, we introduce a co-precipitation method for synthesizing a Mn4+-doped oxyfluoride perovskite KNaMoO2F4 phosphor containing [MoO2F4]2- building units. The electron paramagnetic resonance (EPR) spectra are consistent with the presence of a MnF62- species at g = 1.991. The KNaMoO2F4:0.01Mn4+ phosphor exhibits strong absorption under blue light and an internal quantum yield (IQE) of 65.8%. Attributed to the distorted octahedral environment of the Mn4+ ions, visible ZPL emission was detected at 625 nm. Based on theoretical calculations, the Mn4+ ions in the KNaMoO2F4 host exist in a strong crystal field with a high Dq/B value of ∼3.86. A series of photoluminescence-dependent low-temperature spectra indicates that the Mn4+ emissive state experiences weak electron-phonon interactions upon calculating the Huang-Rhys factor. Benefiting from the ZPL, a warm white-light-emitting diode is achieved using YAG:Ce3+ and KNaMoO2F4:Mn4+ as color converters, in which the color rendering index was Ra = 83.5 and CCT = 4490 K.
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