Luminescence spectra and energy transfer of Tm3+ and Tb3+ doped in LiMgPO4 phosphors

Xu Zhuo; Guo Jing-Yuan; Xiong Zheng-Ye; Tang Qiang; Gao Mu

doi:10.7498/aps.70.20210357

Abstract

LiMgPO₄ (LMP) phosphor doped with rare earth is a promising radiation dosimeter material. Thermoluminescence (TL) spectroscopy is an effective method to study the carrier traps and luminescence centers in materials. To study the luminescent mechanism of rare-earth-doped LMP phosphors, LMP phosphors doped with Tm and Tb (LMP:Tm, LMP:Tb and LMP:Tm, Tb) are prepared by high temperature solid state reaction. The TL glow curve and TL spectrum of the phosphors are measured by the linear heating method, and compared with the photoluminescence (PL) spectrum. The shape of the TL glow curve of LMP phosphor varies with the doping active impurities, but the TL glow curves can be fitted by seven TL peaks. Double-doping Tm³⁺ and Tb³⁺ in LMP phosphor can enhance the TL intensity of the fifth peak (E ~ 1.39 eV) and weaken the seventh TL peak (E ~ 1.70 eV). By comparing the PL spectra with TL spectra of the phosphors, it can be seen that the TL spectra are more complex than the PL spectra excited by ultraviolet light (λ = 352 nm). In the TL process, the electrons which are excited to the conduction band release the energy to recombination centers, and the released energy can more effectively excite the rare earth ions from the ground state to excited states, resulting in the more TL emitting peaks than in the the PL process. Although Tm³⁺ and Tb³⁺ can be the luminescent centers in LMP phosphors when Tm³⁺ and Tb³⁺ are doped in LMP simultaneously, Tb³⁺ ions are likely to act as sensitizers in LMP:Tm and LMP:Tb phosphor, and Tb³⁺ ions transfer energy to the low-energy Tm³⁺ ions, which makes the luminescent centers, Tm³⁺ ions, excited to the high-energy state and then de-excited with emitting light. This result is also proved by the fact that the luminescence decay of Tb³⁺ in phosphors increases with Tm³⁺ concentration increasing. The energy transfer through non-radiative transition is more significant at higher temperature.

Keywords:

Authors and contacts

1.
School of Electronics and Information Engineering, Guangdong Ocean University, Zhanjiang 524088, China
2.
School of Physics, Sun Yat-Sen University, Guangzhou 510275, China
3.
Institute of intelligent manufacturing, Zhanjiang University of Science and Technology, Zhanjiang 524094, China

Corresponding author: Xiong Zheng-Ye, xiongzhengye@139.com

Funds: Project supported by Science and Technology Planning Project of Guangdong Province, China (Grant No. 2015A020216020), the National Natural Science Foundation of China (Grant No. 11375278) and Guangdong Ocean University, China(Grant No. CXXL2019260)

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References

[1]	Daniels F, Boyd C A, Saunders D F 1953 Science 117 343 Google Scholar
[2]	Xiong Z Y, Xu J Y, Zhao F L, Zhang Y, Liu J, Tang Q 2017 J. Lumin. 192 85 Google Scholar
[3]	ZhangS, HuangY, Shi L, Seo H J 2010 J. Phys. Condens. Matter 22 235402 Google Scholar
[4]	Gai M Q, Chen C Y, Fan Y W, Wang J H 2013 J. Rare Earths 31 551 Google Scholar
[5]	Dhabekar B, Menon S N, Raja E A, Bakshi A K, Singh A K, Chougaonkar M P, Mayya Y S 2011 Nucl. Instrum. Meth. Phys. A 269 1844 Google Scholar
[6]	Singh A K, Menon S N, Dhabekar B, Kadam S, Chougaonkar M P, Mayya Y S 2012 Nucl. Instrum. Meth. Phys. A 274 177 Google Scholar
[7]	Bajaj N S, Palan C B, Koparkar K A, Kulkarni M S, Omanwar S K 2016 J. Lumin. 175 915
[8]	郭竞渊, 唐强, 唐桦明, 张纯祥, 罗达铃, 刘小伟 2017 66 107802 Google Scholar GuoJ Y, Tang Q, Tang H M, Zhang C X, Luo D L, Liu X W 2017 Acta Phys. Sin. 66 107802 Google Scholar
[9]	Baran A, Mahlik S, Grinberg M, Cai P, Kim S I, Seo H J 2014 J. Phys. Condens. Matter 26 85401 Google Scholar
[10]	Kumar M, Dhabekar B, Menon S N, Bakshi A K 2013 Radiat. Prot. Dosim. 155 410 Google Scholar
[11]	Kumar M, Dhabekar B, Menon S N, Chougaonkar M P, Mayya Y S 2011 Nucl. Instrum. Methods Phys. Res. B 269 1849 Google Scholar
[12]	Gieszczyk W, Bilski P, Osowski M K, Nowak T, Malinowski L 2018 Radiat. Meas. 113 1419
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[14]	Tang H M, Lin L T, Zhang C X, Tang Q 2019 Inorg. Chem. 58 9698 Google Scholar
[15]	郭竞渊, 唐强, 兰婷婷, 张纯祥, 罗达玲 2015 中国稀土学报 33 404 Guo J Y, Tang Q, Lan T T, Zhang C X, Luo D L 2015 J. Chin. Rare Earths Soc. 33 404
[16]	Gieszczyk W, Marczewska B, Kosowski M, Mrozik A, Stoch P 2019 Materials 12 2861 Google Scholar
[17]	Hanic F, Handlovic M, Burdova K, Majling J 1982 J. Cryst. Spectrosc. 12 99 Google Scholar
[18]	詹明亮, 陈瑶窈, 续卓, 熊正烨 2020 核技术 43 050501 Google Scholar Zhan M L, Chen Y Y, Xu Z, Xiong Z Y 2020 Nucl. Tech. 43 050501 Google Scholar
[19]	McKeever S W S 1988 Thermoluminescence of Solids (London: Cambridge University Press) p75
[20]	Liu X, Teng Y, Zhuang Y, Xie J, Qiao Y, Dong G, Chen D, Qiu J 2009 Opt. Lett. 22 3565

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图 1 LMP磷光体的XRD与标准卡片对比图

Figure 1. XRD of LMP phosphors doped with rare earth.

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图 2 LMP:Tb0.5at%磷光体的热释光发光曲线及其拟合

Figure 2. TL glow curve and the fitting of LMP:Tb0.5at% phosphor.

DownLoad: Full-Size Img PowerPoint

图 3 LMP:Tm0.5at%磷光体的热释光发光曲线及其拟合

Figure 3. TL glow curve and the fitting of LMP:Tm0.5at% phosphor.

DownLoad: Full-Size Img PowerPoint

图 4 LMP:Tb0.5at%, Tm0.5at%磷光体的热释光发光曲线及其拟合　(a) 线性纵坐标; (b)对数纵坐标

Figure 4. TL glow curve and the fitting of LMP:Tb0.5at%, Tm0.5at% phosphor: (a) The ordinate is in linear scale; (b) the ordinate is in logarithmic scale.

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图 5 LMP:Tb0.5at%, Tmxat%磷光体在352 nm的近紫外光激发时的发光谱

Figure 5. Luminescence spectra of phosphors LMP:Tb0.5at%, Tm x at% excited by ultraviolet light (λ = 352 nm).

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图 6 LMP:Tb0.5at%, Tm x at%磷光体荧光(λ_Em = 450 nm)衰减曲线

Figure 6. Luminescence Decay Curves (λ_Em = 450 nm) of phosphors LMP:Tb0.5at%, Tm x at%.

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图 7 (a) LMP:Tb0.5at%磷光体的热释光谱 (b) LMP:Tm0.5at%磷光体的热释光谱 (c) LMP:Tb0.5at%, Tm0.5at%磷光体的热释光谱

Figure 7. (a). TL contour spectra of phosphors LMP:Tb0.5at%. (b). TL contour spectra of phosphors LMP:Tm0.5at%. (c). TL contour spectra of phosphors LMP:Tb0.5at%, Tm0.5at%.

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图 8 (a) LMP:Tb0.5at%磷光体不同温区的热释光谱 (b) LMP:Tm0.5at%磷光体不同温区的热释光谱 (c) LMP:Tm0.5at%, Tb0.5at%磷光体不同温区的热释光谱

Figure 8. (a). TL spectra of phosphors LMP:Tb0.5at% in different temperature ranges. (b). TL spectra of phosphors LMP:Tm0.5at% in different temperature ranges. (c). TL spectra of phosphors LMP:Tm0.5at%, Tb0.5at% in different temperature ranges.

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图 9 Tm离子和Tb离子的能级跃迁示意图

Figure 9. Diagrammatic sketch of energy transition of Tm and Tb ions.

DownLoad: Full-Size Img PowerPoint

表 1 LMP:Tb0.5at%磷光体的热释光陷阱参数

Table 1. TL trap’s parameters of LMP:Tb0.5at% phosphor.

峰序号	E/eV	s/Hz	n₀	b
峰1	0.87	4.18 × 10¹¹	1.68 × 10⁵	1.5
峰2	0.99	2.28 × 10¹²	1.11 × 10⁵	1.3
峰3	1.02	4.39 × 10¹¹	2.76 × 10⁵	2.0
峰4	1.17	4.88 × 10¹⁰	2.84 × 10⁵	2.0
峰5	1.39	1.23 × 10¹¹	1.64 × 10⁵	2.0
峰6	1.64	1.32 × 10¹²	1.32 × 10⁵	2.0
峰7	1.70	3.67 × 10¹¹	4.84 × 10⁵	1.6

DownLoad: CSV

表 2 LMP:Tm0.5at%磷光体的热释光陷阱参数

Table 2. TL trap’s parameters of LMP:Tm0.5at% phosphor.

峰序号	E/eV	s/Hz	n₀	b
峰1	0.89	7.92 × 10¹¹	8.83 × 10⁴	1.2
峰2	1.01	3.31 × 10¹²	2.34 × 10⁵	2.0
峰3	1.08	8.00 × 10¹⁰	1.04 × 10⁵	1.5
峰4	1.20	4.27 × 10¹⁰	1.85 × 10⁵	1.2
峰5	1.38	8.32 × 10¹⁰	2.83 × 10⁵	1.3
峰6	1.63	1.17 × 10¹²	4.50 × 10⁴	1.3
峰7	1.69	4.26 × 10¹¹	3.67 × 10⁴	1.0

DownLoad: CSV

表 3 LMP:Tb0.5at, Tm0.5at%磷光体的热释光陷阱参数

Table 3. TL trap’s parameters of LMP:Tb0.5at%, Tm0.5at% phosphor.

峰序号	E/eV	s/Hz	n₀	b
峰1	0.85	9.30 × 10¹¹	1.48 × 10⁵	1.9
峰2	0.95	1.89 × 10¹²	9.83 × 10⁴	2.0
峰3	1.09	2.74 × 10¹²	4.02 × 10⁴	2.0
峰4	1.16	4.99 × 10¹¹	2.48 × 10⁵	1.4
峰5	1.40	6.26 × 10¹¹	3.80 × 10⁶	1.2
峰6	1.58	8.31 × 10¹²	2.13 × 10⁵	1.5
峰7	1.70	2.18 × 10¹²	3.09 × 10³	1.1

DownLoad: CSV

表 4 LMP:Tb0.5at%, Tm0.5at%磷光体中Tb³⁺向Tm³⁺的能量转移效率

Table 4. The efficiency of energy transfer from Tb³⁺ to Tm³⁺ in LMP:Tb0.5at%, Tm0.5at% phosphor.

x	τ/μs	σ_τ/μs	η_ET	σ_η_ET
0	66.5	1.1	—	—
0.05	33.3	0.3	49.9%	1.0%
0.10	26.6	0.2	60.0%	1.1%
0.20	20.3	0.2	69.5%	1.4%
1.00	13.4	0.3	79.8%	2.3%

DownLoad: CSV

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[1]	Daniels F, Boyd C A, Saunders D F 1953 Science 117 343 Google Scholar
[2]	Xiong Z Y, Xu J Y, Zhao F L, Zhang Y, Liu J, Tang Q 2017 J. Lumin. 192 85 Google Scholar
[3]	ZhangS, HuangY, Shi L, Seo H J 2010 J. Phys. Condens. Matter 22 235402 Google Scholar
[4]	Gai M Q, Chen C Y, Fan Y W, Wang J H 2013 J. Rare Earths 31 551 Google Scholar
[5]	Dhabekar B, Menon S N, Raja E A, Bakshi A K, Singh A K, Chougaonkar M P, Mayya Y S 2011 Nucl. Instrum. Meth. Phys. A 269 1844 Google Scholar
[6]	Singh A K, Menon S N, Dhabekar B, Kadam S, Chougaonkar M P, Mayya Y S 2012 Nucl. Instrum. Meth. Phys. A 274 177 Google Scholar
[7]	Bajaj N S, Palan C B, Koparkar K A, Kulkarni M S, Omanwar S K 2016 J. Lumin. 175 915
[8]	郭竞渊, 唐强, 唐桦明, 张纯祥, 罗达铃, 刘小伟 2017 66 107802 Google Scholar GuoJ Y, Tang Q, Tang H M, Zhang C X, Luo D L, Liu X W 2017 Acta Phys. Sin. 66 107802 Google Scholar
[9]	Baran A, Mahlik S, Grinberg M, Cai P, Kim S I, Seo H J 2014 J. Phys. Condens. Matter 26 85401 Google Scholar
[10]	Kumar M, Dhabekar B, Menon S N, Bakshi A K 2013 Radiat. Prot. Dosim. 155 410 Google Scholar
[11]	Kumar M, Dhabekar B, Menon S N, Chougaonkar M P, Mayya Y S 2011 Nucl. Instrum. Methods Phys. Res. B 269 1849 Google Scholar
[12]	Gieszczyk W, Bilski P, Osowski M K, Nowak T, Malinowski L 2018 Radiat. Meas. 113 1419
[13]	Keskin I C, Türemis M, Kat M I, Gültekin S, Arslanlar Y T, Cetin A, Kibar R 2020 J. Lumin. 225 117276 Google Scholar
[14]	Tang H M, Lin L T, Zhang C X, Tang Q 2019 Inorg. Chem. 58 9698 Google Scholar
[15]	郭竞渊, 唐强, 兰婷婷, 张纯祥, 罗达玲 2015 中国稀土学报 33 404 Guo J Y, Tang Q, Lan T T, Zhang C X, Luo D L 2015 J. Chin. Rare Earths Soc. 33 404
[16]	Gieszczyk W, Marczewska B, Kosowski M, Mrozik A, Stoch P 2019 Materials 12 2861 Google Scholar
[17]	Hanic F, Handlovic M, Burdova K, Majling J 1982 J. Cryst. Spectrosc. 12 99 Google Scholar
[18]	詹明亮, 陈瑶窈, 续卓, 熊正烨 2020 核技术 43 050501 Google Scholar Zhan M L, Chen Y Y, Xu Z, Xiong Z Y 2020 Nucl. Tech. 43 050501 Google Scholar
[19]	McKeever S W S 1988 Thermoluminescence of Solids (London: Cambridge University Press) p75
[20]	Liu X, Teng Y, Zhuang Y, Xie J, Qiao Y, Dong G, Chen D, Qiu J 2009 Opt. Lett. 22 3565

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Luminescence spectra and energy transfer of Tm³⁺ and Tb³⁺ doped in LiMgPO₄ phosphors

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Corresponding author: Xiong Zheng-Ye, xiongzhengye@139.com

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