Neighboring-Cation Substitution Tuning of Photoluminescence by Remote-Controlled Activator in Phosphor Lattice
Highly efficient red phosphors with superior intrinsic properties that are excited by ultraviolet or blue light-emitting diodes are important white light sources for our daily life. Nitride-based phosphors, such as Sr2Si5N8:Eu2+ and CaAlSiN3:Eu2+, are commonly more red-shifted in photoluminescence a...
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Published in | Journal of the American Chemical Society Vol. 135; no. 34; pp. 12504 - 12507 |
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Main Authors | , , , , , |
Format | Journal Article |
Language | English |
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United States
American Chemical Society
28.08.2013
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Abstract | Highly efficient red phosphors with superior intrinsic properties that are excited by ultraviolet or blue light-emitting diodes are important white light sources for our daily life. Nitride-based phosphors, such as Sr2Si5N8:Eu2+ and CaAlSiN3:Eu2+, are commonly more red-shifted in photoluminescence and have better thermal/chemical stability than oxides. Cation substitutions are usually performed to optimize photoluminescence and thermal quenching behavior. However, the underlying mechanisms are unclear in most cases. Here we show that neighboring-cation substitution systematically controls temperature-dependent photoluminescence behavior in CaAlSiN3:Eu2+ lattice. Trivalent cation substitution at the Ca2+ site degrades the photoluminescence in high-temperature environments but achieves better thermal stability when the substituted cation turns monovalent. The neighboring-cation control of lifetime decay is also observed. A remote control effect that guides Eu2+ activators in selective Ca2+ sites is proposed for neighboring-cation substitution while the compositional Si4+/Al3+ ratio adjusts to the valence of M n+ (n = 1–3) cation. In the remote control effect, the Eu2+ activators are surrounded with nitride anions which neighbor with M3+-dominant and Si4+/Al3+-equivalent coordination when M is trivalent, but shift to the site where surrounded nitride anions neighbor with M+-dominant and Si-rich coordination when M is monovalent. This mechanism can efficiently tune optical properties, especially thermal stability, and could be general to luminescent materials, which are sensitive to valence variation in local environments. |
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AbstractList | Highly efficient red phosphors with superior intrinsic properties that are excited by ultraviolet or blue light-emitting diodes are important white light sources for our daily life. Nitride-based phosphors, such as Sr2Si5N8:Eu(2+) and CaAlSiN3:Eu(2+), are commonly more red-shifted in photoluminescence and have better thermal/chemical stability than oxides. Cation substitutions are usually performed to optimize photoluminescence and thermal quenching behavior. However, the underlying mechanisms are unclear in most cases. Here we show that neighboring-cation substitution systematically controls temperature-dependent photoluminescence behavior in CaAlSiN3:Eu(2+) lattice. Trivalent cation substitution at the Ca(2+) site degrades the photoluminescence in high-temperature environments but achieves better thermal stability when the substituted cation turns monovalent. The neighboring-cation control of lifetime decay is also observed. A remote control effect that guides Eu(2+) activators in selective Ca(2+) sites is proposed for neighboring-cation substitution while the compositional Si(4+)/Al(3+) ratio adjusts to the valence of M(n+) (n = 1-3) cation. In the remote control effect, the Eu(2+) activators are surrounded with nitride anions which neighbor with M(3+)-dominant and Si(4+)/Al(3+)-equivalent coordination when M is trivalent, but shift to the site where surrounded nitride anions neighbor with M(+)-dominant and Si-rich coordination when M is monovalent. This mechanism can efficiently tune optical properties, especially thermal stability, and could be general to luminescent materials, which are sensitive to valence variation in local environments. Highly efficient red phosphors with superior intrinsic properties that are excited by ultraviolet or blue light-emitting diodes are important white light sources for our daily life. Nitride-based phosphors, such as Sr2Si5N8:Eu2+ and CaAlSiN3:Eu2+, are commonly more red-shifted in photoluminescence and have better thermal/chemical stability than oxides. Cation substitutions are usually performed to optimize photoluminescence and thermal quenching behavior. However, the underlying mechanisms are unclear in most cases. Here we show that neighboring-cation substitution systematically controls temperature-dependent photoluminescence behavior in CaAlSiN3:Eu2+ lattice. Trivalent cation substitution at the Ca2+ site degrades the photoluminescence in high-temperature environments but achieves better thermal stability when the substituted cation turns monovalent. The neighboring-cation control of lifetime decay is also observed. A remote control effect that guides Eu2+ activators in selective Ca2+ sites is proposed for neighboring-cation substitution while the compositional Si4+/Al3+ ratio adjusts to the valence of M n+ (n = 1–3) cation. In the remote control effect, the Eu2+ activators are surrounded with nitride anions which neighbor with M3+-dominant and Si4+/Al3+-equivalent coordination when M is trivalent, but shift to the site where surrounded nitride anions neighbor with M+-dominant and Si-rich coordination when M is monovalent. This mechanism can efficiently tune optical properties, especially thermal stability, and could be general to luminescent materials, which are sensitive to valence variation in local environments. |
Author | Li, Ye Chen, Wei-Ting Wang, Siao-Shan Liu, Ru-Shi Wang, Jing Sheu, Hwo-Shuenn |
AuthorAffiliation | National Synchrotron Radiation Research Center Sun Yat-sen University National Taiwan University |
AuthorAffiliation_xml | – name: National Taiwan University – name: National Synchrotron Radiation Research Center – name: Sun Yat-sen University |
Author_xml | – sequence: 1 givenname: Siao-Shan surname: Wang fullname: Wang, Siao-Shan – sequence: 2 givenname: Wei-Ting surname: Chen fullname: Chen, Wei-Ting – sequence: 3 givenname: Ye surname: Li fullname: Li, Ye – sequence: 4 givenname: Jing surname: Wang fullname: Wang, Jing – sequence: 5 givenname: Hwo-Shuenn surname: Sheu fullname: Sheu, Hwo-Shuenn – sequence: 6 givenname: Ru-Shi surname: Liu fullname: Liu, Ru-Shi email: rsliu@ntu.edu.tw |
BackLink | https://www.ncbi.nlm.nih.gov/pubmed/23941075$$D View this record in MEDLINE/PubMed |
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Title | Neighboring-Cation Substitution Tuning of Photoluminescence by Remote-Controlled Activator in Phosphor Lattice |
URI | http://dx.doi.org/10.1021/ja404510v https://www.ncbi.nlm.nih.gov/pubmed/23941075 https://search.proquest.com/docview/1428772265 |
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