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Journal of Advanced Ceramics 2023, 12(4): 734-746 https://doi.org/10.26599/JAC.2023.9220716
Research Article | Open Access | Issue | Published: 24 March 2023

Broadband orange-emitting Sr3Si8O4N10:Eu2+ phosphor discovered by a modified single-particle-diagnosis approach

Show Author's Information Le Wanga,  Guozhen Dingb,  Shuxing Lib,  Shiro Funahashic,  Takashi Takedac,  Lu Yina,  Pei Lianga,  Naoto Hirosakic,  Rong-Jun Xieb,d( )
College of Optical and Electronic Technology, China Jiliang University, Hangzhou 310018, China
Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials, College of Materials, Xiamen University, Xiamen 361005, China
Phosphors Group, National Institute for Materials Science, Tsukuba 305-0035, Japan
State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University, Xiamen 361005, China
Keywords:
photoluminescence (PL), phosphor, solid-state lighting, imaging spectroscopy, oxonitridosilicate
Cite this article:
Wang L, Ding G, Li S, et al. Broadband orange-emitting Sr3Si8O4N10:Eu2+ phosphor discovered by a modified single-particle-diagnosis approach. Journal of Advanced Ceramics, 2023, 12(4): 734-746. https://doi.org/10.26599/JAC.2023.9220716
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Abstract Full text About this article

Discovery of new phosphors with desired properties is of great significance for developing high optical quality solid-state lighting. The single-particle-diagnosis approach is an effective way to search novel phosphors by analyzing tiny single crystals screened from the fired powder mixtures. In this work, a broadband orange-emitting phosphor of Sr3Si8O4N10:Eu2+ for solid state lighting was discovered by this method. The new oxonitridosilicate crystallizes in the monoclinic space group of P21/n (No. 14) with cell parameters of a = 4.8185 Å, b = 24.2303 Å, c = 10.5611 Å, β = 90.616°, and Z = 4. The crystal structure of Sr3Si8O4N10 was determined from the single-crystal X-ray diffraction (XRD) data of a single crystal, which is made up of a three-dimensional framework consisting of vertex-sharing SiN4 and SiN3O tetrahedra. Sr2+ ions occupy five crystallographic sites and have coordination numbers between 6 and 8 with one ordered Sr and other four disordered Sr atoms. The multiple Sr sites lead to a broadband emission centered at 565–600 nm and a bandwidth of 128–138 nm. The internal and external quantum efficiencies (IQE/EQE) of the title phosphor are 48.6% and 29.1% under 450 nm excitation, respectively. To improve the accuracy and speed of distinguishing phosphor particles in fired powder mixtures, a microscopic imaging spectroscopy is developed and demonstrated to modify the single-particle-diagnosis method.


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About this article

Broadband orange-emitting Sr3Si8O4N10:Eu2+ phosphor discovered by a modified single-particle-diagnosis approach

Show Author's information Le Wanga, Guozhen Dingb, Shuxing Lib, Shiro Funahashic, Takashi Takedac, Lu Yina, Pei Lianga, Naoto Hirosakic, Rong-Jun Xieb,d( )
College of Optical and Electronic Technology, China Jiliang University, Hangzhou 310018, China
Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials, College of Materials, Xiamen University, Xiamen 361005, China
Phosphors Group, National Institute for Materials Science, Tsukuba 305-0035, Japan
State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University, Xiamen 361005, China

Abstract

Discovery of new phosphors with desired properties is of great significance for developing high optical quality solid-state lighting. The single-particle-diagnosis approach is an effective way to search novel phosphors by analyzing tiny single crystals screened from the fired powder mixtures. In this work, a broadband orange-emitting phosphor of Sr3Si8O4N10:Eu2+ for solid state lighting was discovered by this method. The new oxonitridosilicate crystallizes in the monoclinic space group of P21/n (No. 14) with cell parameters of a = 4.8185 Å, b = 24.2303 Å, c = 10.5611 Å, β = 90.616°, and Z = 4. The crystal structure of Sr3Si8O4N10 was determined from the single-crystal X-ray diffraction (XRD) data of a single crystal, which is made up of a three-dimensional framework consisting of vertex-sharing SiN4 and SiN3O tetrahedra. Sr2+ ions occupy five crystallographic sites and have coordination numbers between 6 and 8 with one ordered Sr and other four disordered Sr atoms. The multiple Sr sites lead to a broadband emission centered at 565–600 nm and a bandwidth of 128–138 nm. The internal and external quantum efficiencies (IQE/EQE) of the title phosphor are 48.6% and 29.1% under 450 nm excitation, respectively. To improve the accuracy and speed of distinguishing phosphor particles in fired powder mixtures, a microscopic imaging spectroscopy is developed and demonstrated to modify the single-particle-diagnosis method.

Keywords: photoluminescence (PL), phosphor, solid-state lighting, imaging spectroscopy, oxonitridosilicate

References(46)

[1]
Wang L, Xie RJ, Suehiro T, et al. Down-conversion nitride materials for solid state lighting: Recent advances and perspectives. Chem Rev 2018, 118: 1951–2009.
DOI Google Scholar
[2]
Zeuner M, Pagano S, Schnick W. Nitridosilicates and oxonitridosilicates: From ceramic materials to structural and functional diversity. Angew Chem Int Ed 2011, 50: 7754–7775.
DOI Google Scholar
[3]
Hirosaki N, Xie RJ, Kimoto K, et al. Characterization and properties of green-emitting β-SiAlON:Eu2+ powder phosphors for white light-emitting diodes. Appl Phys Lett 2005, 86: 211905.
DOI Google Scholar
[4]
Li YQ, Delsing ACA, de With G, et al. Luminescence properties of Eu2+-activated alkaline-earth silicon-oxynitride MSi2O2−δN2+2/3δ (M = Ca, Sr, Ba):   A promising class of novel LED conversion phosphors. Chem Mater 2005, 17: 3242–3248.
DOI Google Scholar
[5]
Xie RJ, Hirosaki N, Mitomo M, et al. Photoluminescence of rare-earth-doped Ca-α-SiAlON phosphors: Composition and concentration dependence. J Am Ceram Soc 2005, 88: 2883–2888.
DOI Google Scholar
[6]
Duan CJ, Wang XJ, Otten WM, et al. Preparation, electronic structure, and photoluminescence properties of Eu2+- and Ce3+/Li+-activated alkaline earth silicon nitride MSiN2 (M = Sr, Ba). Chem Mater 2008, 20: 1597–1605.
DOI Google Scholar
[7]
Li JW, Watanabe T, Sakamoto N, et al. Synthesis of a multinary nitride, Eu-doped CaAlSiN3, from alloy at low temperatures. Chem Mater 2008, 20: 2095–2105.
DOI Google Scholar
[8]
Li YQ, Hirosaki N, Xie RJ, et al. Yellow–orange-emitting CaAlSiN3:Ce3+ phosphor: Structure, photoluminescence, and application in white LEDs. Chem Mater 2008, 20: 6704–6714.
DOI Google Scholar
[9]
Li HL, Xie RJ, Hirosaki N, et al. Synthesis and luminescence properties of orange–red-emitting M2Si5N8:Eu2+ (M = Ca, Sr, Ba) light-emitting diode conversion phosphors by a simple nitridation of MSi2. Int J Appl Ceram Tec 2009, 6: 459–464.
DOI Google Scholar
[10]
Liu LH, Xie RJ, Hirosaki N, et al. Temperature dependent luminescence of yellow-emitting α-SiAlON:Eu2+ oxynitride phosphors for white light-emitting diodes. J Am Ceram Soc 2009, 92: 2668–2673.
DOI Google Scholar
[11]
Braun C, Seibald M, Börger SL, et al. Material properties and structural characterization of M3Si6O12N2:Eu2+ (M = Ba, Sr)—A comprehensive study on a promising green phosphor for pc-LEDs. Chem-Eur J 2010, 16: 9646–9657.
DOI Google Scholar
[12]
Ryu JH, Won HS, Park YG, et al. Photoluminescence of Ce3+-activated β-SiAlON blue phosphor for UV-LED. Electrochem Solid St 2010, 13: H30–H32.
DOI Google Scholar
[13]
Wang XM, Wang CH, Kuang XJ, et al. Promising oxonitridosilicate phosphor host Sr3Si2O4N2: Synthesis, structure, and luminescence properties activated by Eu2+ and Ce3+/Li+ for pc-LEDs. Inorg Chem 2012, 51: 3540–3547.
DOI Google Scholar
[14]
Park WB, Shin N, Hong KP, et al. A new paradigm for materials discovery: Heuristics-assisted combinatorial chemistry involving parameterization of material novelty. Adv Funct Mater 2012, 22: 2258–2266.
DOI Google Scholar
[15]
Miao SH, Xia ZG, Molokeev MS, et al. Crystal structure refinement and luminescence properties of blue–green-emitting CaSrAl2SiO7:Ce3+,Li+,Eu2+ phosphors. J Mater Chem C 2015, 3: 8322–8328.
DOI Google Scholar
[16]
Wang ZB, Chu IH, Zhou F, et al. Electronic structure descriptor for the discovery of narrow-band red-emitting phosphors. Chem Mater 2016, 28: 4024–4031.
DOI Google Scholar
[17]
Zhuo Y, Mansouri Tehrani A, Oliynyk AO, et al. Identifying an efficient, thermally robust inorganic phosphor host via machine learning. Nat Commun 2018, 9: 4377.
DOI Google Scholar
[18]
Park WB, Singh SP, Yoon C, et al. Eu2+ luminescence from 5 different crystallographic sites in a novel red phosphor, Ca15Si20O10N30:Eu2+. J Mater Chem 2012, 22: 14068–14075.
DOI Google Scholar
[19]
Park WB, Jeong YS, Singh SP, et al. A yellow-emitting oxynitride phosphor: Ce4−xCaxSi12O3+xN18−x:Eu2+. ECS J Solid State Sci Technol 2013, 2: R3100–R3106.
DOI Google Scholar
[20]
Park WB, Singh SP, Yoon C, et al. Combinatorial chemistry of oxynitride phosphors and discovery of a novel phosphor for use in light emitting diodes, Ca1.5Ba0.5Si5N6O3: Eu2+. J Mater Chem C 2013, 1: 1832–1839.
DOI Google Scholar
[21]
Park WB, Singh SP, Sohn KS. Discovery of a phosphor for light emitting diode applications and its structural determination, Ba(Si,Al)5(O,N)8:Eu2+. J Am Chem Soc 2014, 136: 2363–2373.
DOI Google Scholar
[22]
Liao HX, Zhao M, Molokeev MS, et al. Learning from a mineral structure toward an ultra-narrow-band blue-emitting silicate phosphor RbNa3(Li3SiO4)4:Eu2+. Angew Chem Int Ed 2018, 130: 11902–11905.
DOI Google Scholar
[23]
Zhao M, Liao HX, Ning LX, et al. Next-generation narrow-band green-emitting RbLi(Li3SiO4)2:Eu2+ phosphor for backlight display application. Adv Mater 2018, 30: 1802489.
DOI Google Scholar
[24]
Liao HX, Zhao M, Zhou YY, et al. Polyhedron transformation toward stable narrow-band green phosphors for wide-color-gamut liquid crystal display. Adv Funct Mater 2019, 29: 1901988.
DOI Google Scholar
[25]
Zhao M, Zhou YY, Molokeev MS, et al. Discovery of new narrow-band phosphors with the UCr4C4-related type structure by alkali cation effect. Adv Opt Mater 2019, 7: 1801631.
DOI Google Scholar
[26]
Pust P, Hintze F, Hecht C, et al. Group (III) nitrides M[Mg2Al2N4] (M = Ca, Sr, Ba, Eu) and Ba[Mg2Ga2N4]— Structural relation and nontypical luminescence properties of Eu2+ doped samples. Chem Mater 2014, 26: 6113–6119.
DOI Google Scholar
[27]
Pust P, Weiler V, Hecht C, et al. Narrow-band red-emitting Sr[LiAl3N4]:Eu2+ as a next-generation LED-phosphor material. Nat Mater 2014, 13: 891–896.
DOI Google Scholar
[28]
Pust P, Wochnik AS, Baumann E, et al. Ca[LiAl3N4]:Eu2+—A narrow-band red-emitting nitridolithoaluminate. Chem Mater 2014, 26: 3544–3549.
DOI Google Scholar
[29]
Wagatha P, Weiler V, Schmidt PJ, et al. Tailoring emission characteristics: Narrow-band red luminescence from SLA to CaBa[Li2Al6N8]:Eu2+. Chem Mater 2018, 30: 7885–7891.
DOI Google Scholar
[30]
Ha J, Kim YH, Novitskaya E, et al. Color tunable single-phase Eu2+ and Ce3+ co-activated Sr2LiAlO4 phosphors. J Mater Chem C 2019, 7: 7734–7744.
DOI Google Scholar
[31]
Li SX, Xia YH, Amachraa M, et al. Data-driven discovery of full-visible-spectrum phosphor. Chem Mater 2019, 31: 6286–6294.
DOI Google Scholar
[32]
Hirosaki N, Takeda T, Funahashi S, et al. Discovery of new nitridosilicate phosphors for solid state lighting by the single-particle-diagnosis approach. Chem Mater 2014, 26: 4280–4288.
DOI Google Scholar
[33]
Wang XJ, Wang L, Takeda T, et al. Blue-emitting Sr3Si8−xAlxO7+xN8−x:Eu2+ discovered by a single-particle-diagnosis approach: Crystal structure, luminescence, scale-up synthesis, and its abnormal thermal quenching behavior. Chem Mater 2015, 27: 7689–7697.
DOI Google Scholar
[34]
Ten Kate OM, Xie RJ, Wang CY, et al. Eu2+-doped Sr2B2−2xSi2+3xAl2−xN8+x: A boron-containing orange-emitting nitridosilicate with interesting composition-dependent photoluminescence properties. Inorg Chem 2016, 55: 11331–11336.
DOI Google Scholar
[35]
Wang CY, Takeda T, ten Kate OM, et al. New deep-blue-emitting Ce-doped A4−mBnC19+2mX29+m (A = Sr, La; B = Li; C = Si, Al; X = O, N; 0 ≤ m ≤ 1; 0 ≤ n ≤ 1) phosphors for high-color-rendering warm white light-emitting diodes. ACS Appl Mater Interfaces 2019, 11: 29047–29055.
DOI Google Scholar
[36]
Zhang YX, Li SX, Takeda T, et al. Realizing red/orange emission of Eu2+/Ce3+ in La26−xSrxSi41Ox+1N80−x (x = 12.72–12.90) phosphors for high color rendition white LEDs. J Mater Chem C 2020, 8: 13458–13466.
DOI Google Scholar
[37]
Yao FF, Wang L, Lv Y, et al. Composition-dependent thermal degradation of red-emitting (Ca1−xSrx)AlSiN3:Eu2+ phosphors for high color rendering white LEDs. J Mater Chem C 2018, 6: 890–898.
DOI Google Scholar
[38]
Kim Y, Kim J, Kang S. First-principles thermodynamic calculations and experimental investigation of Sr–Si–N–O system—Synthesis of Sr2Si5N8:Eu phosphor. J Mater Chem C 2013, 1: 69–78.
DOI Google Scholar
[39]
Wu YP, Lu H, Wang SS, et al. Asymmetric boron-complexes containing keto-isoindolinyl and pyridyl groups: Solvatochromic fluorescence, efficient solid-state emission and DFT calculations. J Mater Chem C 2015, 3: 12281–12289.
DOI Google Scholar
[40]
Strobel P, de Boer T, Weiler V, et al. Luminescence of an oxonitridoberyllate: A study of narrow-band cyan-emitting Sr[Be6ON4]:Eu2+. Chem Mater 2018, 30: 3122–3130.
DOI Google Scholar
[41]
Li SX, Amachraa M, Chen C, et al. Efficient near-infrared phosphors discovered by parametrizing the Eu(II) 5d-to-4f energy gap. Matter 2022, 5: 1924–1936.
DOI Google Scholar
[42]
Xie RJ, Hirosaki N, Sakuma K, et al. Eu2+-doped Ca-α-SiAlON: A yellow phosphor for white light-emitting diodes. Appl Phys Lett 2004, 84: 5404–5406.
DOI Google Scholar
[43]
Qin X, Liu XW, Huang W, et al. Lanthanide-activated phosphors based on 4f–5d optical transitions: Theoretical and experimental aspects. Chem Rev 2017, 117: 4488–4527.
DOI Google Scholar
[44]
Ueda J, Dorenbos P, Bos AJJ, et al. Insight into the thermal quenching mechanism for Y3Al5O12:Ce3+ through thermoluminescence excitation spectroscopy. J Phys Chem C 2015, 119: 25003–25008.
DOI Google Scholar
[45]
Li SX, Wang L, Tang DM, et al. Achieving high quantum efficiency narrow-band β-SiAlON:Eu2+ phosphors for high-brightness LCD backlights by reducing the Eu3+ luminescence killer. Chem Mater 2018, 30: 494–505.
DOI Google Scholar
[46]
Liu XJ, Li HL, Xie RJ, et al. Cerium-doped lutetium aluminum garnet optically transparent ceramics fabricated by a sol–gel combustion process. J Mater Res 2006, 21: 1519–1525.
DOI Google Scholar
Publication history
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Publication history

Received: 16 November 2022
Revised: 31 December 2022
Accepted: 03 January 2023
Published: 24 March 2023
Issue date: April 2023

Copyright

© The Author(s) 2023.

Acknowledgements

This work was supported by the National Key R&D Program of China (No. 2022YFE0108800), the National Natural Science Foundation of China (Nos. 51832005, 51802274, 62075203, and U2005213), and Foreign Coorperation Project of Fujian Provincial Science and Technology Plan (No. 2020I0002).

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