Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 8, Issue 13, Pages 3095-3100Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.7b01158
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- Ministerio de Economia y Competitividad, Spain (Direccion General de Investigacion y Gestion del Plan Nacional de I+D+i) [MAT2014-54395-P]
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Controlling luminescence in phosphors able to produce several emissions from different stable excited states determines their use in optical devices. We investigate the color control mechanism that quenches the greenish-blue emission in favor of the red one in the archetype phosphor CaTiO3:Pr3+. State-of-the-art ab initio calculations indicate that direct host-to-dopant energy transfer (released by electron-hole recombination following the interband excitation and structural reorganization) selectively populates the D-1(2) red luminescent state of Pr3+ and bypasses the P-3(0) greenish-blue emitter. Local defects can modulate the electron-hole recombination energy and therefore increase the red emission efficiency, as experimentally observed. The selection of red emission does not happen in CaZrO3:Pr3+ because the electron-hole recombination energy is much higher. The calculations could not support the widely accepted color control mechanism based on metal-to-metal charge transfer states. The conclusion sets new points of view for the color control of lanthanide activated inorganic phosphors.
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