Institute of Multidisciplinary Research for Advanced Materials, Tohoku University , Sendai 980-8577, Japan.
Faculty of Science, Okayama University of Science , Okayama 700-0005, Japan.
ACS Appl Mater Interfaces. 2016 May 11;8(18):11615-20. doi: 10.1021/acsami.6b02237. Epub 2016 Apr 28.
Phosphors with sufficient red emission component are necessary for warm white light-emitting diodes. In this work on (Sr,Ba)2(1-x)Eu2xSiO4 phosphors, (Sr,Ba)1.5Eu0.5SiO4 achieved 75% of an internal quantum efficiency under excitation by blue light. Surprisingly, the (Sr,Ba)1.5Eu0.5SiO4 exhibited orange emission, against the well-known traditional green-yellow emission of (Sr,Ba)2SiO4:Eu(2+). Moreover, the concentration quenching of Eu(2+) in (Sr,Ba)2SiO4 was abnormally unobvious. With the help of calculations based on the density functional theory, it was discovered that the distinct local environment of luminescence centers rather than usual explanation such as self-absorption or intensified crystal field splitting, is responsible to the interesting red shifts in excitation and emission spectra. The refinement analysis based on X-ray diffraction revealed that the unequal distribution of Eu(2+) to two crystallographic sites caused low concentration of Eu(2+) at the 9-coordination site, inhibiting the concentration quenching. The (Sr,Ba)1.5Eu0.5SiO4 phosphor has warmer emission than the commercial Y3Al5O12:Ce(3+). This study also promotes research on the effect of site occupancy and the local environment of luminescence centers.
对于暖白光发光二极管而言,需要足够的红光发射成分的荧光粉。在本研究中,(Sr,Ba)2(1-x)Eu2xSiO4 荧光粉在蓝光激发下实现了 75%的内量子效率。令人惊讶的是,(Sr,Ba)1.5Eu0.5SiO4 表现出橙色发射,而不是(Sr,Ba)2SiO4:Eu(2+)熟知的传统黄绿发射。此外,Eu(2+)在(Sr,Ba)2SiO4 中的浓度猝灭异常不明显。借助基于密度泛函理论的计算,发现发光中心的明显局部环境而不是自吸收或增强的晶体场分裂等常见解释,是导致激发和发射光谱中有趣的红移的原因。基于 X 射线衍射的精修分析表明,Eu(2+)在两个晶位上的不均匀分布导致 9 配位位上的 Eu(2+)浓度较低,抑制了浓度猝灭。(Sr,Ba)1.5Eu0.5SiO4 荧光粉的发射比商用 Y3Al5O12:Ce(3+)更暖。本研究还促进了对占据位置和发光中心局部环境的研究。