Structural Ordering and Charge Variation Induced by Cation Substitution in (Sr,Ca)AlSiN3:Eu Phosphor
Nitride phosphors are suitable for white light-emitting diode applications. In this study, the structure of phosphor has been modified through cation substitution to induce charge variation and a rearrangement of neighboring nitride clusters, and consequently enhance its luminescent behavior. Substi...
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| Published in: | Journal of the American Chemical Society Vol. 137; no. 28; pp. 8936 - 8939 |
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| Main Authors: | , , , , , |
| Format: | Journal Article |
| Language: | English |
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United States
22.07.2015
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| ISSN: | 1520-5126 |
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| Abstract | Nitride phosphors are suitable for white light-emitting diode applications. In this study, the structure of phosphor has been modified through cation substitution to induce charge variation and a rearrangement of neighboring nitride clusters, and consequently enhance its luminescent behavior. Substitution of Ca(2+) by Sr(2+) cations expanded the lattice volume and the bc plane, but shortened the distance between the layers along the a axis. Lattice distortion of the framework introduced high-coordination sites in the Sr/Eu centers and adequate space, thereby facilitating charge variation of activators under reduced atmosphere, as detected through X-ray absorption near-edge structure spectroscopy. As such, the photoluminescent intensity of the phosphors increased by more than 10% and a blue shift occurred. The microstructures of the samples were also analyzed using high-resolution transmission electron microscopy. Cation substitution induced a special change in the anion environment, as indicated in the solid-state Raman spectra. Moreover, typical ordering variations in the SiN4 and AlN4 clusters are generated in the lattice. Meanwhile, neighbor sequence of (Si/Al)N4 around the divalent centers were observed through solid-state nuclear magnetic resonance spectroscopy. The modified ordering distribution resulted in a rigid structure and improved the thermal quenching behavior. Thermal stability has been enhanced by 10% at 473 K when x = 0.9 in SrxCa0.993-xAlSiN3:Eu(2+)0.007 compared with that at x = 0. This study promotes the research of neighbor sequence for selective tetrahedral sites such as Li, Mg, Al, and Si coordinated by N atoms in contact with cation sites. |
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| AbstractList | Nitride phosphors are suitable for white light-emitting diode applications. In this study, the structure of phosphor has been modified through cation substitution to induce charge variation and a rearrangement of neighboring nitride clusters, and consequently enhance its luminescent behavior. Substitution of Ca(2+) by Sr(2+) cations expanded the lattice volume and the bc plane, but shortened the distance between the layers along the a axis. Lattice distortion of the framework introduced high-coordination sites in the Sr/Eu centers and adequate space, thereby facilitating charge variation of activators under reduced atmosphere, as detected through X-ray absorption near-edge structure spectroscopy. As such, the photoluminescent intensity of the phosphors increased by more than 10% and a blue shift occurred. The microstructures of the samples were also analyzed using high-resolution transmission electron microscopy. Cation substitution induced a special change in the anion environment, as indicated in the solid-state Raman spectra. Moreover, typical ordering variations in the SiN4 and AlN4 clusters are generated in the lattice. Meanwhile, neighbor sequence of (Si/Al)N4 around the divalent centers were observed through solid-state nuclear magnetic resonance spectroscopy. The modified ordering distribution resulted in a rigid structure and improved the thermal quenching behavior. Thermal stability has been enhanced by 10% at 473 K when x = 0.9 in SrxCa0.993-xAlSiN3:Eu(2+)0.007 compared with that at x = 0. This study promotes the research of neighbor sequence for selective tetrahedral sites such as Li, Mg, Al, and Si coordinated by N atoms in contact with cation sites. |
| Author | Zhou, Wuzong Lee, Jyh-Fu Tsai, Yi-Ting Chiang, Chang-Yang Liu, Ru-Shi Sheu, Hwo-Shuenn |
| Author_xml | – sequence: 1 givenname: Yi-Ting surname: Tsai fullname: Tsai, Yi-Ting organization: †Department of Chemistry, National Taiwan University, Taipei 106, Taiwan – sequence: 2 givenname: Chang-Yang surname: Chiang fullname: Chiang, Chang-Yang organization: ‡EaStCHEM, School of Chemistry, University of St Andrews, St Andrews, KY16 9ST, United Kingdom – sequence: 3 givenname: Wuzong surname: Zhou fullname: Zhou, Wuzong organization: ‡EaStCHEM, School of Chemistry, University of St Andrews, St Andrews, KY16 9ST, United Kingdom – sequence: 4 givenname: Jyh-Fu surname: Lee fullname: Lee, Jyh-Fu organization: §National Synchrotron Radiation Research Center, Hsinchu 300, Taiwan – sequence: 5 givenname: Hwo-Shuenn surname: Sheu fullname: Sheu, Hwo-Shuenn organization: §National Synchrotron Radiation Research Center, Hsinchu 300, Taiwan – sequence: 6 givenname: Ru-Shi surname: Liu fullname: Liu, Ru-Shi organization: ∥Department of Mechanical Engineering and Graduate Institute of Manufacturing Technology, National Taipei University of Technology, Taipei 106, Taiwan |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/26161898$$D View this record in MEDLINE/PubMed |
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| Snippet | Nitride phosphors are suitable for white light-emitting diode applications. In this study, the structure of phosphor has been modified through cation... |
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| Title | Structural Ordering and Charge Variation Induced by Cation Substitution in (Sr,Ca)AlSiN3:Eu Phosphor |
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