Cation-Size-Mismatch Tuning of Photoluminescence in Oxynitride Phosphors
Red or yellow phosphors excited by a blue light-emitting diode are an efficient source of white light for everyday applications. Many solid oxides and nitrides, particularly silicon nitride-based materials such as M2Si5N8 and MSi2O2N2 (M = Ca, Sr, Ba), CaAlSiN3, and SiAlON, are useful phosphor hosts...
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| Published in | Journal of the American Chemical Society Vol. 134; no. 19; pp. 8022 - 8025 |
|---|---|
| Main Authors | , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
16.05.2012
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| Subjects | |
| Online Access | Get full text |
| ISSN | 0002-7863 1520-5126 1520-5126 |
| DOI | 10.1021/ja301593z |
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| Abstract | Red or yellow phosphors excited by a blue light-emitting diode are an efficient source of white light for everyday applications. Many solid oxides and nitrides, particularly silicon nitride-based materials such as M2Si5N8 and MSi2O2N2 (M = Ca, Sr, Ba), CaAlSiN3, and SiAlON, are useful phosphor hosts with good thermal stabilities. Both oxide/nitride and various cation substitutions are commonly used to shift the emission spectrum and optimize luminescent properties, but the underlying mechanisms are not always clear. Here we show that size-mismatch between host and dopant cations tunes photoluminescence shifts systematically in M1.95Eu0.05Si5–x Al x N8–x O x lattices, leading to a red shift when the M = Ba and Sr host cations are larger than the Eu2+ dopant, but a blue shift when the M = Ca host is smaller. Size-mismatch tuning of thermal quenching is also observed. A local anion clustering mechanism in which Eu2+ gains excess nitride coordination in the M = Ba and Sr structures, but excess oxide in the Ca analogues, is proposed for these mismatch effects. This mechanism is predicted to be general to oxynitride materials and will be useful in tuning optical and other properties that are sensitive to local coordination environments. |
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| AbstractList | Red or yellow phosphors excited by a blue light-emitting diode are an efficient source of white light for everyday applications. Many solid oxides and nitrides, particularly silicon nitride-based materials such as M₂Si₅N₈ and MSi₂O₂N₂ (M = Ca, Sr, Ba), CaAlSiN₃, and SiAlON, are useful phosphor hosts with good thermal stabilities. Both oxide/nitride and various cation substitutions are commonly used to shift the emission spectrum and optimize luminescent properties, but the underlying mechanisms are not always clear. Here we show that size-mismatch between host and dopant cations tunes photoluminescence shifts systematically in M₁.₉₅Eu₀.₀₅Si₅–ₓAlₓN₈–ₓOₓ lattices, leading to a red shift when the M = Ba and Sr host cations are larger than the Eu²⁺ dopant, but a blue shift when the M = Ca host is smaller. Size-mismatch tuning of thermal quenching is also observed. A local anion clustering mechanism in which Eu²⁺ gains excess nitride coordination in the M = Ba and Sr structures, but excess oxide in the Ca analogues, is proposed for these mismatch effects. This mechanism is predicted to be general to oxynitride materials and will be useful in tuning optical and other properties that are sensitive to local coordination environments. Red or yellow phosphors excited by a blue light-emitting diode are an efficient source of white light for everyday applications. Many solid oxides and nitrides, particularly silicon nitride-based materials such as M(2)Si(5)N(8) and MSi(2)O(2)N(2) (M = Ca, Sr, Ba), CaAlSiN(3), and SiAlON, are useful phosphor hosts with good thermal stabilities. Both oxide/nitride and various cation substitutions are commonly used to shift the emission spectrum and optimize luminescent properties, but the underlying mechanisms are not always clear. Here we show that size-mismatch between host and dopant cations tunes photoluminescence shifts systematically in M(1.95)Eu(0.05)Si(5-x)Al(x)N(8-x)O(x) lattices, leading to a red shift when the M = Ba and Sr host cations are larger than the Eu(2+) dopant, but a blue shift when the M = Ca host is smaller. Size-mismatch tuning of thermal quenching is also observed. A local anion clustering mechanism in which Eu(2+) gains excess nitride coordination in the M = Ba and Sr structures, but excess oxide in the Ca analogues, is proposed for these mismatch effects. This mechanism is predicted to be general to oxynitride materials and will be useful in tuning optical and other properties that are sensitive to local coordination environments.Red or yellow phosphors excited by a blue light-emitting diode are an efficient source of white light for everyday applications. Many solid oxides and nitrides, particularly silicon nitride-based materials such as M(2)Si(5)N(8) and MSi(2)O(2)N(2) (M = Ca, Sr, Ba), CaAlSiN(3), and SiAlON, are useful phosphor hosts with good thermal stabilities. Both oxide/nitride and various cation substitutions are commonly used to shift the emission spectrum and optimize luminescent properties, but the underlying mechanisms are not always clear. Here we show that size-mismatch between host and dopant cations tunes photoluminescence shifts systematically in M(1.95)Eu(0.05)Si(5-x)Al(x)N(8-x)O(x) lattices, leading to a red shift when the M = Ba and Sr host cations are larger than the Eu(2+) dopant, but a blue shift when the M = Ca host is smaller. Size-mismatch tuning of thermal quenching is also observed. A local anion clustering mechanism in which Eu(2+) gains excess nitride coordination in the M = Ba and Sr structures, but excess oxide in the Ca analogues, is proposed for these mismatch effects. This mechanism is predicted to be general to oxynitride materials and will be useful in tuning optical and other properties that are sensitive to local coordination environments. Red or yellow phosphors excited by a blue light-emitting diode are an efficient source of white light for everyday applications. Many solid oxides and nitrides, particularly silicon nitride-based materials such as M(2)Si(5)N(8) and MSi(2)O(2)N(2) (M = Ca, Sr, Ba), CaAlSiN(3), and SiAlON, are useful phosphor hosts with good thermal stabilities. Both oxide/nitride and various cation substitutions are commonly used to shift the emission spectrum and optimize luminescent properties, but the underlying mechanisms are not always clear. Here we show that size-mismatch between host and dopant cations tunes photoluminescence shifts systematically in M(1.95)Eu(0.05)Si(5-x)Al(x)N(8-x)O(x) lattices, leading to a red shift when the M = Ba and Sr host cations are larger than the Eu(2+) dopant, but a blue shift when the M = Ca host is smaller. Size-mismatch tuning of thermal quenching is also observed. A local anion clustering mechanism in which Eu(2+) gains excess nitride coordination in the M = Ba and Sr structures, but excess oxide in the Ca analogues, is proposed for these mismatch effects. This mechanism is predicted to be general to oxynitride materials and will be useful in tuning optical and other properties that are sensitive to local coordination environments. Red or yellow phosphors excited by a blue light-emitting diode are an efficient source of white light for everyday applications. Many solid oxides and nitrides, particularly silicon nitride-based materials such as M2Si5N8 and MSi2O2N2 (M = Ca, Sr, Ba), CaAlSiN3, and SiAlON, are useful phosphor hosts with good thermal stabilities. Both oxide/nitride and various cation substitutions are commonly used to shift the emission spectrum and optimize luminescent properties, but the underlying mechanisms are not always clear. Here we show that size-mismatch between host and dopant cations tunes photoluminescence shifts systematically in M1.95Eu0.05Si5–x Al x N8–x O x lattices, leading to a red shift when the M = Ba and Sr host cations are larger than the Eu2+ dopant, but a blue shift when the M = Ca host is smaller. Size-mismatch tuning of thermal quenching is also observed. A local anion clustering mechanism in which Eu2+ gains excess nitride coordination in the M = Ba and Sr structures, but excess oxide in the Ca analogues, is proposed for these mismatch effects. This mechanism is predicted to be general to oxynitride materials and will be useful in tuning optical and other properties that are sensitive to local coordination environments. |
| Author | Chen, Wei-Ting Liu, Ru-Shi Attfield, J. Paul Sheu, Hwo-Shuenn |
| AuthorAffiliation | University of Edinburgh National Synchrotron Radiation Research Center National Taiwan University |
| AuthorAffiliation_xml | – name: National Taiwan University – name: National Synchrotron Radiation Research Center – name: University of Edinburgh |
| Author_xml | – sequence: 1 givenname: Wei-Ting surname: Chen fullname: Chen, Wei-Ting – sequence: 2 givenname: Hwo-Shuenn surname: Sheu fullname: Sheu, Hwo-Shuenn – sequence: 3 givenname: Ru-Shi surname: Liu fullname: Liu, Ru-Shi email: j.p.attfield@ed.ac.uk, rsliu@ntu.edu.tw – sequence: 4 givenname: J. Paul surname: Attfield fullname: Attfield, J. Paul email: j.p.attfield@ed.ac.uk, rsliu@ntu.edu.tw |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/22534019$$D View this record in MEDLINE/PubMed |
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| Snippet | Red or yellow phosphors excited by a blue light-emitting diode are an efficient source of white light for everyday applications. Many solid oxides and... |
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| SubjectTerms | barium calcium cations europium nitrides oxides photoluminescence silicon strontium white light |
| Title | Cation-Size-Mismatch Tuning of Photoluminescence in Oxynitride Phosphors |
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