Mechanisms of Energy Transfer and Enhanced Stability of Carbidonitride Phosphors for Solid-State Lighting

Christopher Grieco, Kurt F. Hirsekorn, Andrew T. Heitsch, Alan C. Thomas, Mark H. McAdon, Britt A. Vanchura, Michael M. Romanelli, Lora L. Brehm, Anne Leugers, Anatoliy N. Sokolov, John B. Asbury

Research output: Contribution to journalArticle

4 Citations (Scopus)

Abstract

Phosphor-converted light emitting diodes (pcLEDs) produce white light through the use of phosphors that convert blue light emitted from the LED chip into green and red wavelengths. Understanding the mechanisms of degradation of the emission spectra and quantum yields of the phosphors used in pcLEDs is of critical importance to fully realize the potential of solid-state lighting as an energy efficient technology. Toward this end, time-resolved photoluminescence spectroscopy was used to identify the mechanistic origins of enhanced stability and luminescence efficiency that can be obtained from a series of carbidonitride red phosphors with varying degrees of substitutional carbon. The increasing substitution of carbon and oxygen in nitrogen positions of the carbidonitride phosphor (Sr2Si5N8-[(4x/3)+z]CxO3z/2:Eu2+) systematically changed the dimensions of the crystalline lattice. These structural changes caused a red shift and broadening of the emission spectra of the phosphors due to faster energy transfer from higher to lower energy emission sites. Surprisingly, in spite of broadening of the emission spectra, the quantum yield was maintained or increased with carbon substitution. Aging phosphors with lowered carbon content under conditions that accurately reflected thermal and optical stresses found in functioning pcLED packages led to spectral changes that were dependent on substitutional carbon content. Importantly, phosphors that contained optimal amounts of carbon and oxygen possessed luminescence spectra and quantum yields that did not undergo changes associated with aging and therefore provided a more stable color point for superior control of the emission properties of pcLED packages. These findings provide insights to guide continued development of phosphors for efficient and stable solid-state lighting materials and devices.

Original languageEnglish (US)
Pages (from-to)12547-12555
Number of pages9
JournalACS Applied Materials and Interfaces
Volume9
Issue number14
DOIs
StatePublished - Apr 12 2017

Fingerprint

Phosphors
Energy transfer
Lighting
Carbon
Quantum yield
Light emitting diodes
Luminescence
Substitution reactions
Aging of materials
Oxygen
Photoluminescence spectroscopy
Crystal lattices
Nitrogen
Crystalline materials
Color
Degradation
Wavelength

All Science Journal Classification (ASJC) codes

  • Materials Science(all)

Cite this

Grieco, Christopher ; Hirsekorn, Kurt F. ; Heitsch, Andrew T. ; Thomas, Alan C. ; McAdon, Mark H. ; Vanchura, Britt A. ; Romanelli, Michael M. ; Brehm, Lora L. ; Leugers, Anne ; Sokolov, Anatoliy N. ; Asbury, John B. / Mechanisms of Energy Transfer and Enhanced Stability of Carbidonitride Phosphors for Solid-State Lighting. In: ACS Applied Materials and Interfaces. 2017 ; Vol. 9, No. 14. pp. 12547-12555.
@article{7ed883942c07480ba464d6f878c149c8,
title = "Mechanisms of Energy Transfer and Enhanced Stability of Carbidonitride Phosphors for Solid-State Lighting",
abstract = "Phosphor-converted light emitting diodes (pcLEDs) produce white light through the use of phosphors that convert blue light emitted from the LED chip into green and red wavelengths. Understanding the mechanisms of degradation of the emission spectra and quantum yields of the phosphors used in pcLEDs is of critical importance to fully realize the potential of solid-state lighting as an energy efficient technology. Toward this end, time-resolved photoluminescence spectroscopy was used to identify the mechanistic origins of enhanced stability and luminescence efficiency that can be obtained from a series of carbidonitride red phosphors with varying degrees of substitutional carbon. The increasing substitution of carbon and oxygen in nitrogen positions of the carbidonitride phosphor (Sr2Si5N8-[(4x/3)+z]CxO3z/2:Eu2+) systematically changed the dimensions of the crystalline lattice. These structural changes caused a red shift and broadening of the emission spectra of the phosphors due to faster energy transfer from higher to lower energy emission sites. Surprisingly, in spite of broadening of the emission spectra, the quantum yield was maintained or increased with carbon substitution. Aging phosphors with lowered carbon content under conditions that accurately reflected thermal and optical stresses found in functioning pcLED packages led to spectral changes that were dependent on substitutional carbon content. Importantly, phosphors that contained optimal amounts of carbon and oxygen possessed luminescence spectra and quantum yields that did not undergo changes associated with aging and therefore provided a more stable color point for superior control of the emission properties of pcLED packages. These findings provide insights to guide continued development of phosphors for efficient and stable solid-state lighting materials and devices.",
author = "Christopher Grieco and Hirsekorn, {Kurt F.} and Heitsch, {Andrew T.} and Thomas, {Alan C.} and McAdon, {Mark H.} and Vanchura, {Britt A.} and Romanelli, {Michael M.} and Brehm, {Lora L.} and Anne Leugers and Sokolov, {Anatoliy N.} and Asbury, {John B.}",
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doi = "10.1021/acsami.6b15323",
language = "English (US)",
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Grieco, C, Hirsekorn, KF, Heitsch, AT, Thomas, AC, McAdon, MH, Vanchura, BA, Romanelli, MM, Brehm, LL, Leugers, A, Sokolov, AN & Asbury, JB 2017, 'Mechanisms of Energy Transfer and Enhanced Stability of Carbidonitride Phosphors for Solid-State Lighting', ACS Applied Materials and Interfaces, vol. 9, no. 14, pp. 12547-12555. https://doi.org/10.1021/acsami.6b15323

Mechanisms of Energy Transfer and Enhanced Stability of Carbidonitride Phosphors for Solid-State Lighting. / Grieco, Christopher; Hirsekorn, Kurt F.; Heitsch, Andrew T.; Thomas, Alan C.; McAdon, Mark H.; Vanchura, Britt A.; Romanelli, Michael M.; Brehm, Lora L.; Leugers, Anne; Sokolov, Anatoliy N.; Asbury, John B.

In: ACS Applied Materials and Interfaces, Vol. 9, No. 14, 12.04.2017, p. 12547-12555.

Research output: Contribution to journalArticle

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T1 - Mechanisms of Energy Transfer and Enhanced Stability of Carbidonitride Phosphors for Solid-State Lighting

AU - Grieco, Christopher

AU - Hirsekorn, Kurt F.

AU - Heitsch, Andrew T.

AU - Thomas, Alan C.

AU - McAdon, Mark H.

AU - Vanchura, Britt A.

AU - Romanelli, Michael M.

AU - Brehm, Lora L.

AU - Leugers, Anne

AU - Sokolov, Anatoliy N.

AU - Asbury, John B.

PY - 2017/4/12

Y1 - 2017/4/12

N2 - Phosphor-converted light emitting diodes (pcLEDs) produce white light through the use of phosphors that convert blue light emitted from the LED chip into green and red wavelengths. Understanding the mechanisms of degradation of the emission spectra and quantum yields of the phosphors used in pcLEDs is of critical importance to fully realize the potential of solid-state lighting as an energy efficient technology. Toward this end, time-resolved photoluminescence spectroscopy was used to identify the mechanistic origins of enhanced stability and luminescence efficiency that can be obtained from a series of carbidonitride red phosphors with varying degrees of substitutional carbon. The increasing substitution of carbon and oxygen in nitrogen positions of the carbidonitride phosphor (Sr2Si5N8-[(4x/3)+z]CxO3z/2:Eu2+) systematically changed the dimensions of the crystalline lattice. These structural changes caused a red shift and broadening of the emission spectra of the phosphors due to faster energy transfer from higher to lower energy emission sites. Surprisingly, in spite of broadening of the emission spectra, the quantum yield was maintained or increased with carbon substitution. Aging phosphors with lowered carbon content under conditions that accurately reflected thermal and optical stresses found in functioning pcLED packages led to spectral changes that were dependent on substitutional carbon content. Importantly, phosphors that contained optimal amounts of carbon and oxygen possessed luminescence spectra and quantum yields that did not undergo changes associated with aging and therefore provided a more stable color point for superior control of the emission properties of pcLED packages. These findings provide insights to guide continued development of phosphors for efficient and stable solid-state lighting materials and devices.

AB - Phosphor-converted light emitting diodes (pcLEDs) produce white light through the use of phosphors that convert blue light emitted from the LED chip into green and red wavelengths. Understanding the mechanisms of degradation of the emission spectra and quantum yields of the phosphors used in pcLEDs is of critical importance to fully realize the potential of solid-state lighting as an energy efficient technology. Toward this end, time-resolved photoluminescence spectroscopy was used to identify the mechanistic origins of enhanced stability and luminescence efficiency that can be obtained from a series of carbidonitride red phosphors with varying degrees of substitutional carbon. The increasing substitution of carbon and oxygen in nitrogen positions of the carbidonitride phosphor (Sr2Si5N8-[(4x/3)+z]CxO3z/2:Eu2+) systematically changed the dimensions of the crystalline lattice. These structural changes caused a red shift and broadening of the emission spectra of the phosphors due to faster energy transfer from higher to lower energy emission sites. Surprisingly, in spite of broadening of the emission spectra, the quantum yield was maintained or increased with carbon substitution. Aging phosphors with lowered carbon content under conditions that accurately reflected thermal and optical stresses found in functioning pcLED packages led to spectral changes that were dependent on substitutional carbon content. Importantly, phosphors that contained optimal amounts of carbon and oxygen possessed luminescence spectra and quantum yields that did not undergo changes associated with aging and therefore provided a more stable color point for superior control of the emission properties of pcLED packages. These findings provide insights to guide continued development of phosphors for efficient and stable solid-state lighting materials and devices.

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