Ab Initio -Aided Sensitizer Design for Mn 4+ -Activated Mg 2 TiO 4 as an Ultrabright Fluoride-Free Red-Emitting Phosphor

Chieh Szu Huang, Cheng-Liang Huang, Yu Chen Liu, Shih-kang Lin, Ting Shan Chan, Hao Wei Tu

Research output: Contribution to journalArticle

10 Citations (Scopus)

Abstract

Red-light phosphor materials are crucial components in solid-state lighting (SSL) for simulating natural sunlight. Mn-doped Mg 2 TiO 4 is a promising fluoride-free red-emitting phosphor; however, a sensitizer is necessary to enhance its brightness. In this work, we perform ab initio calculations based on the density functional theory (DFT) to systematically examine the electronic-band coupling between the luminescent center, Mn, and several possible sensitizers, Zn, Nb, Mo, In, Sn, and Ta. Nb was identified as the optimal sensitizer. Well-crystallized 0.1 at. % Mn and 0.0-0.7 at. % Nb-codoped Mg 2 TiO 4 were synthesized at 1450 °C. Synchrotron-radiation-based X-ray absorption spectroscopy (XAS) experimentally validated the proposed atomistic structure, indicating that the Nb 5+ dopant substitutes Ti 4+ at the 16d sites, leading to the formation of Ti vacancies and of a parasitic MgTiO 3 phase. Effective sensitization, resulting in a 243% enhancement of the photoluminescence intensity, was achieved. The 0.1 at. % Mn and 0.5 at. % Nb-codoped Mg 2 TiO 4 were obtained as an ultrabright "rare-earth-free" (RE-free) and "fluoride-free" red-light phosphor.

Original languageEnglish
Pages (from-to)1769-1775
Number of pages7
JournalChemistry of Materials
Volume30
Issue number5
DOIs
Publication statusPublished - 2018 Mar 13

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Fluorides
Phosphors
X ray absorption spectroscopy
Synchrotron radiation
Rare earths
Vacancies
Density functional theory
Luminance
Photoluminescence
Lighting
Doping (additives)

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Chemical Engineering(all)
  • Materials Chemistry

Cite this

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title = "Ab Initio -Aided Sensitizer Design for Mn 4+ -Activated Mg 2 TiO 4 as an Ultrabright Fluoride-Free Red-Emitting Phosphor",
abstract = "Red-light phosphor materials are crucial components in solid-state lighting (SSL) for simulating natural sunlight. Mn-doped Mg 2 TiO 4 is a promising fluoride-free red-emitting phosphor; however, a sensitizer is necessary to enhance its brightness. In this work, we perform ab initio calculations based on the density functional theory (DFT) to systematically examine the electronic-band coupling between the luminescent center, Mn, and several possible sensitizers, Zn, Nb, Mo, In, Sn, and Ta. Nb was identified as the optimal sensitizer. Well-crystallized 0.1 at. {\%} Mn and 0.0-0.7 at. {\%} Nb-codoped Mg 2 TiO 4 were synthesized at 1450 °C. Synchrotron-radiation-based X-ray absorption spectroscopy (XAS) experimentally validated the proposed atomistic structure, indicating that the Nb 5+ dopant substitutes Ti 4+ at the 16d sites, leading to the formation of Ti vacancies and of a parasitic MgTiO 3 phase. Effective sensitization, resulting in a 243{\%} enhancement of the photoluminescence intensity, was achieved. The 0.1 at. {\%} Mn and 0.5 at. {\%} Nb-codoped Mg 2 TiO 4 were obtained as an ultrabright {"}rare-earth-free{"} (RE-free) and {"}fluoride-free{"} red-light phosphor.",
author = "Huang, {Chieh Szu} and Cheng-Liang Huang and Liu, {Yu Chen} and Shih-kang Lin and Chan, {Ting Shan} and Tu, {Hao Wei}",
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Ab Initio -Aided Sensitizer Design for Mn 4+ -Activated Mg 2 TiO 4 as an Ultrabright Fluoride-Free Red-Emitting Phosphor . / Huang, Chieh Szu; Huang, Cheng-Liang; Liu, Yu Chen; Lin, Shih-kang; Chan, Ting Shan; Tu, Hao Wei.

In: Chemistry of Materials, Vol. 30, No. 5, 13.03.2018, p. 1769-1775.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Ab Initio -Aided Sensitizer Design for Mn 4+ -Activated Mg 2 TiO 4 as an Ultrabright Fluoride-Free Red-Emitting Phosphor

AU - Huang, Chieh Szu

AU - Huang, Cheng-Liang

AU - Liu, Yu Chen

AU - Lin, Shih-kang

AU - Chan, Ting Shan

AU - Tu, Hao Wei

PY - 2018/3/13

Y1 - 2018/3/13

N2 - Red-light phosphor materials are crucial components in solid-state lighting (SSL) for simulating natural sunlight. Mn-doped Mg 2 TiO 4 is a promising fluoride-free red-emitting phosphor; however, a sensitizer is necessary to enhance its brightness. In this work, we perform ab initio calculations based on the density functional theory (DFT) to systematically examine the electronic-band coupling between the luminescent center, Mn, and several possible sensitizers, Zn, Nb, Mo, In, Sn, and Ta. Nb was identified as the optimal sensitizer. Well-crystallized 0.1 at. % Mn and 0.0-0.7 at. % Nb-codoped Mg 2 TiO 4 were synthesized at 1450 °C. Synchrotron-radiation-based X-ray absorption spectroscopy (XAS) experimentally validated the proposed atomistic structure, indicating that the Nb 5+ dopant substitutes Ti 4+ at the 16d sites, leading to the formation of Ti vacancies and of a parasitic MgTiO 3 phase. Effective sensitization, resulting in a 243% enhancement of the photoluminescence intensity, was achieved. The 0.1 at. % Mn and 0.5 at. % Nb-codoped Mg 2 TiO 4 were obtained as an ultrabright "rare-earth-free" (RE-free) and "fluoride-free" red-light phosphor.

AB - Red-light phosphor materials are crucial components in solid-state lighting (SSL) for simulating natural sunlight. Mn-doped Mg 2 TiO 4 is a promising fluoride-free red-emitting phosphor; however, a sensitizer is necessary to enhance its brightness. In this work, we perform ab initio calculations based on the density functional theory (DFT) to systematically examine the electronic-band coupling between the luminescent center, Mn, and several possible sensitizers, Zn, Nb, Mo, In, Sn, and Ta. Nb was identified as the optimal sensitizer. Well-crystallized 0.1 at. % Mn and 0.0-0.7 at. % Nb-codoped Mg 2 TiO 4 were synthesized at 1450 °C. Synchrotron-radiation-based X-ray absorption spectroscopy (XAS) experimentally validated the proposed atomistic structure, indicating that the Nb 5+ dopant substitutes Ti 4+ at the 16d sites, leading to the formation of Ti vacancies and of a parasitic MgTiO 3 phase. Effective sensitization, resulting in a 243% enhancement of the photoluminescence intensity, was achieved. The 0.1 at. % Mn and 0.5 at. % Nb-codoped Mg 2 TiO 4 were obtained as an ultrabright "rare-earth-free" (RE-free) and "fluoride-free" red-light phosphor.

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