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Title: Consequences of Optimal Bond Valence on Structural Rigidity and Improved Luminescence Properties in SrxBa2-xSiO4:Eu2+ Orthosilicate Phosphors

The orthosilicate phosphors SrxBa2–xSiO4:Eu2+ have now been known for over four decades and have found extensive recent use in solid-state white lighting. It is well-recognized in the literature and in practice that intermediate compositions in the solid-solutions between the orthosilicates Sr2SiO4 and Ba2SiO4 yield the best phosphor hosts when the thermal stability of luminescence is considered. We employ a combination of synchrotron X-ray diffraction, total scattering measurements, density functional theory calculations, and low-temperature heat capacity measurements, in conjunction with detailed temperature- and time-resolved studies of luminescence properties to understand the origins of the improved luminescence properties. We observe that in the intermediate compositions, the two cation sites in the crystal structure are optimally bonded as determined from bond valence sum calculations. Optimal bonding results in a more rigid lattice, as established by the intermediate compositions possessing the highest Debye temperature, which are determined experimentally from low-temperature heat capacity measurements. Greater rigidity in turn results in the highest luminescence efficiency for intermediate compositions at elevated temperatures.
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Publication Date:
OSTI Identifier:
Resource Type:
Journal Article
Resource Relation:
Journal Name: Chem. Mater.; Journal Volume: 26; Journal Issue: (7) ; 04, 2014
Research Org:
Advanced Photon Source (APS), Argonne National Laboratory (ANL), Argonne, IL (US)
Sponsoring Org:
Country of Publication:
United States