Composition Screening in Blue-Emitting Li4Sr1+xCa0.97–x(SiO4)2:Ce3+ Phosphors for High Quantum Efficiency and Thermally Stable Photoluminescence

Photoluminescence quantum efficiency (QE) and thermal stability are important for phosphors used in phosphor-converted light-emitting diodes (pc-LEDs). Li4Sr1+xCa0.97-x(SiO4)2:0.03Ce3+ (-0.7 ≤ x ≤ 1.0) phosphors were designed from the initial model of Li4SrCa(SiO4)2:Ce3+, and their single-phased crystal structures were found to be located in the composition range of -0.4 ≤ x ≤ 0.7. Depending on the substitution of Sr2+ for Ca2+ ions, the absolute QE value of blue-emitting composition-optimized Li4Sr1.4Ca0.57(SiO4)2:0.03Ce3+ reaches ∼94%, and the emission intensity at 200 °C remains 95% of that at room temperature. Rietveld refinements and Raman spectral analyses suggest the increase of crystal rigidity, increase of force constant in CeO6, and decrease of vibrational frequency by increasing Sr2+ content, which are responsible for the enhanced quantum efficiency and thermal stability. The present study points to a new strategy for future development of the pc-LEDs phosphors based on local structures correlation via composition screening.