Structure and luminescence properties of Li2Gd4(MoO4)7:Sm3+ orange-red phosphor for solid-state lighting

Lu Jing-Wen; Zhao Jin; Zhang Yong-Chun; Tu Ru-Ting; Liu Fu-Ni; Leng Zhi-Hua

doi:10.7498/aps.73.20241017

Abstract

White LEDs have the broad application prospect and market demand, while the red phosphor can greatly affect the color temperature and color rendering index of the modulated white light. In this work, a series of Li₂Gd_4–x Sm_x(MoO₄)₇ (x = 0.01–0.13) phosphors is prepared by the high-temperature solid phase method. The successful doping of Sm³⁺ into Li₂Gd₄(MoO₄)₇ is confirmed by X-ray diffractometry (XRD) and does not lead to any change in crystal structure. The samples are detected by scanning electron microscope (SEM) to have irregular blocky structures with particle size less than 20 μm. The existence of Li, Gd, Mo, O and Sm elements in the phosphor is confirmed by energy dispersive X-ray spectroscopy (EDS). The observation of X-ray photoelectron spectroscopy (XPS) shows that the activators are successfully doped into materials. Under 406 nm excitation, the emission peaks of the samples are located at 563, 598, 645 and 706 nm respectively, which are caused by the 4f-4f transition of Sm³⁺, and the strongest emission peak comes from ⁴G_5/2→⁶H_9/2 transition. It is found that optimal concentration of Sm³⁺ is 0.07. With the increase of Sm³⁺ concentration, the fluorescence lifetime decreases gradually. The temperature-dependent emission of phosphor is also studied. The emission intensity at 473 K is still 79% of that at 298 K, indicating that the sample has excellent heat resistance. The CIE chromaticity diagram shows the luminescence of the prepared phosphor is located in the orange-red region and the color purity is high (99%). Moreover, a white LED is fabricated using the optical doped phosphor, which has CIE coordinates of (0.3788, 0.3134) that are located in the circle of white light. Research shows that the Li₂Gd₄(MoO₄)₇:Sm³⁺ phosphor is a promising orange-red phosphor for white LEDs.

Keywords:

Authors and contacts

1.
College of Science, Xi’an University of Architecture and Technology, Xi’an 710055, China
2.
School of Chemistry and Chemical Engineering, Xi’an University of Architecture and Technology, Xi’an 710055, China

Corresponding author: Zhao Jin, zhaojin@xauat.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 11804265), the Key Science and Technology Innovation Team of Shaanxi Province, China (Grant No. 2022TD-30), and the Natural Science Basic Research Program of Shaanxi Province, China (Grant No. 2024JC-YBMS-384).

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References

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Cited By

图 1 样品的物相分析与结构　(a) Li₂Gd₄(MoO₄)₇:x Sm³⁺ (x = 0.01, 0.07, 0.13)的XRD图谱; (b) Li₂Gd₄(MoO₄)₇的晶体结构

Figure 1. Phase analysis and structrue of samples: (a) XRD patterns of Li₂Gd₄(MoO₄)₇:x Sm³⁺ (x = 0.01, 0.07, 0.13); (b) crystal structure of Li₂Gd₄(MoO₄)₇.

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图 2 Li₂Gd₄(MoO₄)₇:0.07Sm³⁺荧光粉的形貌分析　(a) SEM图; (b)—(g)各元素分布图和EDS能谱图

Figure 2. Morphology analysis of Li₂Gd₄(MoO₄)₇:0.07Sm³⁺: (a) SEM image; (b)–(g) distribution of elements and EDS energy spectrum.

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图 3 (a) Li₂Gd₄(MoO₄)₇:0.07Sm³⁺荧光粉XPS全谱; (b)—(f) Li 1s, Gd 4d, Mo 3d, O 1s和Sm 3d核心级频谱

Figure 3. (a) Full XPS spectrum of Li₂Gd₄(MoO₄)₇:0.07Sm³⁺ phosphor; (b)–(f) Li 1s, Gd 4d, Mo 3d, O 1s and Sm 3d core-level spectra.

DownLoad: Full-Size Img PowerPoint

图 4 Li₂Gd₄(MoO₄)₇:x Sm³⁺ (x = 0.01—0.13)样品的荧光光谱　(a) 激发光谱; (b) 发射光谱

Figure 4. Fluorescence spectra of Li₂Gd₄(MoO₄)₇:x Sm³⁺ (x = 0.01–0.13) samples: (a) Excitation spectra; (b) emission spectra.

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图 5 (a) Li₂Gd₄(MoO₄)₇:x Sm³⁺ (x = 0.01—0.13)的发射光谱; (b) 发射强度与Sm³⁺掺杂浓度的关系图; (c) lg(I/x)与lg(x)的关系曲线; (d) Sm³⁺的掺杂浓度与598, 645 nm处发射峰积分面积关系图

Figure 5. (a) Emission spectra of Li₂Gd₄(MoO₄)₇:x Sm³⁺ (x = 0.01–0.13); (b) the relationship between emission intensity and Sm³⁺ doping concentration; (c) lg(I/x)-lg(x); (d) the relationship between the concentration of Sm³⁺ and the emission integral intensity at 598 nm and 645 nm.

DownLoad: Full-Size Img PowerPoint

图 6 荧光衰减曲线和发光机理　(a) Li₂Gd₄(MoO₄)₇:x Sm³⁺ (x = 0.01—0.13)系列样品在645 nm处的寿命衰减曲线(λ_ex = 406 nm); (b) Sm³⁺的能级跃迁图

Figure 6. Fluorescence attenuation curves and luminescence mechanism: (a) Lifetime decay curves of Li₂Gd₄(MoO₄)₇:x Sm³⁺ (x = 0.01–0.13) at 645 nm (λ_ex = 406 nm); (b) energy level transition diagram of Sm³⁺.

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图 7 (a) Li₂Gd₄(MoO₄)₇:0.07Sm³⁺荧光粉在不同温度下的发光光谱; (b) 样品在298—448 K范围内的热行为映射图; (c) 归一化发光强度随温度的变化; (d) $\ln[(I_0/I) - 1]$与10000/T关系

Figure 7. (a) Luminescence spectra of Li₂Gd₄(MoO₄)₇:0.07Sm³⁺ phosphor at different temperatures; (b) the thermal behavior mapping diagram of sample in the range of 298–448 K; (c) the normalized luminescence intensity varies with temperature; (d) the relationship between $\ln[(I_0/I) -1] $ of phosphor and 10000/T.

DownLoad: Full-Size Img PowerPoint

图 8 (a) Li₂Gd₄(MoO₄)₇:x Sm³⁺ (x = 0.01—0.13)荧光粉在406 nm激发下的色坐标图; (b) Li₂Gd₄(MoO₄)₇:x Sm³⁺ (x = 0.01—0.13)的色度坐标x, y点线图

Figure 8. (a) Color coordinates of Li₂Gd₄(MoO₄)₇:x Sm³⁺ (x = 0.01–0.13) excited at 406 nm; (b) the chromaticity coordinates x, y point plot of Li₂Gd₄(MoO₄)₇:x Sm³⁺ (x = 0.01–0.13).

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图 9 (a) Li₂Gd₄(MoO₄)₇:0.07Sm³⁺的内量子效率和放大图; (b)白光LED装置的色坐标、电致发光光谱及照片

Figure 9. (a) Internal quantum efficiency of Li₂Gd₄(MoO₄)₇:0.07Sm³⁺ and enlarged profile; (b) the color coordinates, electroluminescence spectrum and LED image of the fabricated w-LED.

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表 1 Li₂Gd₄(MoO₄)₇:x Sm³⁺ (x = 0.01—0.13)的CIE色度坐标及色纯度

Table 1. The CIE coordinates and color purity of Li₂Gd₄(MoO₄)₇:x Sm³⁺ (x = 0.01—0.13).

Concentration of Sm³⁺	CIE coordinates (x, y)	Color purity/%
x = 0.01	(0.6311, 0.3682)	99.77
x = 0.03	(0.6314, 0.3679)	99.86
x = 0.05	(0.6315, 0.3678)	99.89
x = 0.07	(0.6315, 0.3679)	99.89
x = 0.09	(0.6318, 0.3676)	99.98
x = 0.11	(0.6313, 0.3680)	99.83
x = 0.01	(0.6312, 0.3681)	99.80

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[11]	Wang C W, Peng L X, Qin F, Kou M, Wang Y D, Xu L L, Zhang Z G 2024 Opt. Mater. 154 115741
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[21]	骆志杨 2020 硕士学位论文(大连: 大连工业大学) Luo Z Y 2020 M. S. Thesis (Dalian: Dalian Polytechnic University
[22]	Chen J Q, Chen J Y, Zhang W N, Xu S J, Chen L P, Guo H 2023 Ceram. Int. 49 16252 Google Scholar
[23]	Jiang K Z, Zhou C, Li W H, Su H R, He D M, Chen X Y, Zhang D, Xie S A, Yu R J 2024 J. Alloys Compds. 980 173518 Google Scholar
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[30]	Zhao C C, Yin X, Huang F Q, Hang Y 2011 J. Solid State Chem. 184 3190 Google Scholar
[31]	Li H, Li L, Zhao W, Zhou X, Hua Y 2023 Mater. Today Chem. 32 101661 Google Scholar
[32]	Ji C Y, Huang Z, Tian X Y 2020 J. Alloys Compds. 825 154176 Google Scholar
[33]	Liu H K, Nie K, Zhang Y Y, Mei L F, Deyneko D V, Ma X X 2023 J. Rare Earth 41 1288 Google Scholar
[34]	阿依努热木·吐尔逊, 王磊, 苏比伊努尔·吉力力, 艾尔肯·斯地克 2022 激光与光电子学进展 59 329 Ayinuremu T, Wang L, Subiyinuer J, Aierken S 2022 Prog. Laser Optoelectron. 59 329
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[47]	Cui R R, Guo X, Deng C Y 2020 J. Lumin. 224 117233 Google Scholar
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Vol. 73, Issue 21 - 2024-11-05

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Structure and luminescence properties of Li₂Gd₄(MoO₄)₇:Sm³⁺ orange-red phosphor for solid-state lighting

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Corresponding author: Zhao Jin, zhaojin@xauat.edu.cn

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