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 inJournal of the American Chemical Society Vol. 135; no. 34; pp. 12504 - 12507
Main Authors Wang, Siao-Shan, Chen, Wei-Ting, Li, Ye, Wang, Jing, Sheu, Hwo-Shuenn, Liu, Ru-Shi
Format Journal Article
LanguageEnglish
Published 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.
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
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– name: Sun Yat-sen University
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  givenname: Siao-Shan
  surname: Wang
  fullname: Wang, Siao-Shan
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  surname: Li
  fullname: Li, Ye
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  givenname: Jing
  surname: Wang
  fullname: Wang, Jing
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  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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Snippet Highly efficient red phosphors with superior intrinsic properties that are excited by ultraviolet or blue light-emitting diodes are important white light...
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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
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