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A series of Eu-doped LaSr 2 AlO 5 phosphors were synthesized by high-temperature solid state reactions under oxidative and reductive atmospheres, respectively. The photoluminescence properties, fluorescence quenching mechanism and valence-change behavior of europium ions in the phosphor have been studied. For the samples prepared in oxidative atmosphere, the Eu 3+ ions occupy the La 3+ sites and exhibit characteristic sharp lines(500–750 nm) originating from the 5 D 1 and 5 D 0 levels to 7F transitions. With the increase of Eu 3+ concentration, the chromaticity coordinates of La 1− x Sr 2 AlO 5 : x Eu 3+ phosphors are turned from (0.479, 0.453) for x =0.005 to (0.621, 0.358) for x =1.0. The quenching process of 5 D 1 → 7 F 1 (533 nm) emission is attributed to cross-relaxation as the Eu 3+ concentration reaches 5 mol%. The dominant line emission 5 D 0 → 7 F 2 (619 nm) is quenched due to the exchange interaction as the Eu 3+ concentration reaches 75 mol%. For the sample prepared in reductive atmosphere, it shows the presence of both Eu 3+ and Eu 2+ . The Eu 2+ in LaSr 2 AlO 5 host lattice can be excited by a blue light with an intense broad red emission band centered at 610 nm (a full width at half maximum of 110 nm) with color coordinates of (0.611, 0.368). The internal quantum efficiency was measured to be ~42%, indicating that this phosphor has a great potential in blue-chip pumped white light emitting diodes (WLEDs). The conditions for the reduction process of Eu 3+ to Eu 2+ in solid state compounds were discussed. From the X-ray diffraction and Gaussian fitting of the emission spectra, we propose that Eu 3+ ions occupy the La 3+ sites while Eu 2+ ions occupy the two different Sr 2+ sites. [ABSTRACT FROM AUTHOR]