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单离子掺杂体系单一基质白光荧光粉可以有效克服紫外芯片+三基色荧光粉获得白光方案中颗粒分散性和沉降性不均的问题, 克服荧光粉彼此间发光再吸收及三基色配比调控等问题. 本文采用熔融盐法制备了Sm3+离子单掺NaLa(WO4)2:x Sm3+白光荧光粉. 在紫外光激发下,
${\rm{WO}}_{4}^{2-}$ 自激活发出的蓝绿光, 与Sm3+发射的绿光、黄光、橙光和红光混合得到了白光. 在250 nm激发下, 荧光粉会发出冷白光; 在403 nm激发下会发出暖白光. 随着Sm3+掺杂浓度增加, 相对色温逐渐降低. 所制备的样品均为纯的四方相结构, 晶粒形貌为不规则菱形薄片. 通过分析实验数据确定Sm3+离子间的能量猝灭类型为电偶极-电偶极作用. 得到的NaLa(WO4)2: x Sm3+荧光粉具有较高的稳定性, 能被近紫外LED芯片有效地激发, 可作为单离子掺杂单一基质白光荧光粉潜在候选.-
关键词:
- NaLa(WO4)2: Sm3+ /
- 光致发光 /
- 白光荧光粉
Single ion doped single phase white emitting phosphors have some special advantages and great potential applications in the field of high quality LED lighting. This type of phosphors can effectively solve the problem of uneven particle dispersion and sedimentation in the white light scheme obtained by UV chip plus trichromatic phosphor, and solve the problems of the luminescence and reabsorption between phosphors and the regulation of trichromatic ratio. A comparison of the single-ion doping luminescent material with the multi-ion doping system shows that the single-ion doping luminescent material is simpler in both preparation process and luminescence color adjustment, which can achieve higher color rendering index, more easily controlled color temperature and closer to the color coordinates of white light. According to the principle of colorimetry and luminescence, light of two or more wavelengths may be combined to obtain white light emission. Under the UV excitation, the Sm3+ ions emit relatively strong green, yellow, orange and red light at 580–670 nm. Under UV excitation, the broadband spectrum of ${\rm{WO}}_{4}^{2-} $ self-activated emission covers almost the whole visible region, but the blue-green light is strong in the short wavelength region and the yellow-orange-red light is weak in the long wavelength region. When Sm3+ ions are doped into tungstate, Sm3+ ions’ luminescence can effectively supplement the weak luminescence intensity of tungstate in the long-wave region, and white light can be obtained. Under the excitation of 250 nm, the phosphor emits cold white light, and warm white light under the excitation of 403 nm. The experimental results show that Sm3+ ions have a significant effect on the correlated color temperature adjustment of self-activated luminescence of NLW phosphors. All the prepared samples are crystallized into the tetragonal crystal phase structures and that their morphologies present rhombic sheet. By analyzing the experimental data, the type of energy transfer between Sm3+ ions is determined to be electrical dipole–electrical dipole interaction. The NLW: xSm3+ phosphor has high stability and can be effectively excited by ultraviolet/near-ultraviolet light, which can be used as a potential candidate of single matrix single-ion doped white phosphors.-
Keywords:
- NaLa(WO4)2: Sm3+ /
- photoluminescence /
- white light phosphors
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图 1 晶体结构信息 (a) NLW:x Sm3+荧光粉的XRD谱; (b) (112)峰位置随Sm3+浓度变化偏移; (c) NLW:2%Sm3+ XRD谱的Rietveld精修; (d) NLW:x Sm3+晶体结构图
Fig. 1. Crystal structure information: (a) XRD patterns of NLW:x Sm3+ phosphors; (b) offset of the (112) peak position with the Sm3+ concentration; (c) rietveld refinement of XRD pattern of NLW:2%Sm3+; (d) the crystal structure of NLW:x Sm3+.
图 2 NLW:2%Sm3+样品的表征 (a) SEM; (b) EDS; (c)−(g) 元素Mapping
Fig. 2. Characterization of NLW:2%Sm3+ sample: (a) SEM; (b) EDS; (c)−(g) element mapping.
图 4 样品在403 nm激发下发射谱 (a) NLW:x Sm3+(x = 1%−5%); (b) NLW:2%Sm3+
Fig. 4. Emission spectra excited at 403 nm: (a) NLW:x Sm3+ (x = 1%−5%); (b) NLW:2%Sm3+.
图 5 样品在250 nm激发下发射谱 (a) NLW:x Sm3+(x = 1%−5%); (b) NLW:2%Sm3+发射谱的宽带峰拟合; (c) NLW:2%Sm3+渲染图
Fig. 5. Emission spectra excited at 250 nm: (a) NLW:x Sm3+ (x = 1%−5%); (b) fitting broad band peak of emission spectrum of NLW:2%Sm3+; (c) rendering picture of NLW:2%Sm3+.
图 6 样品NLW:x Sm3+的色度图与色坐标 (a) 250 nm激发下; (b) 403 nm激发下
Fig. 6. Chromaticity diagrams and color coordinates of NLW:x Sm3+: (a) Excited at 250 nm; (b) excited at 403 nm.
图 7
${\rm{WO}}_{4}^{2-} $ 向Sm3+能量转移过程Fig. 7. Energy transfer process from
${\rm{WO}}_{4}^{2-} $ to Sm3+.
图 8 系列样品NLW:x Sm3+中Sm3+的衰减曲线与荧光寿命
Fig. 8. Decay curves and fluorescence lifetimes of Sm3+ in series NLW:x Sm3+ sample.
图 9 NLW:x Sm3+的lg(I/x)与lg(x)关系曲线
Fig. 9. Curve of lg(I/x) versus lg(x) for NLW:x Sm3+.
表 1 NLW:x Sm3+晶格参数
Table 1. Lattice constants of NLW:x Sm3+.
NLW:xSm3+
concentrationsa/Å c/Å unit cell
volume/Å31% 5.542 11.692 359.1 2% 5.539 11.699 358.9 3% 5.531 11.692 357.7 4% 5.530 11.691 357.5 5% 5.528 11.690 357.2 
下载: 导出CSV
表 2 在403 nm激发下NLW:x Sm3+的I644/I604比值
Table 2. Ratios of I644 to I604 of NLW:x Sm3+ excited at 403 nm.
Sm3+ concentrations/% 1 2 3 4 5 I644/I604 0.93 1.07 1.05 1.04 1.02
下载: 导出CSV
表 3 NLW:x Sm3+色坐标和相对色温
Table 3. Color coordinates and relative color temperatures of NLW:x Sm3+ samples.
Sm3+ concentrations/% 1 2 3 4 5 λex = 250 nm (0.270, 0.249)
16618 K(0.287, 0.248)
12435 K(0.288, 0.258)
11032 K(0.283, 0.255)
12346 K(0.313, 0.280)
6971 Kλex = 403 nm (0.298, 0.251)
9963 K(0.374, 0.286)
3057 K(0.377, 0.282)
2911 K(0.376, 0.286)
3004 K(0.357, 0.279)
3798 K
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[1] 郭伟玲, 邓杰, 王嘉露, 王乐, 邰建鹏 2019 物理学报 68 247303
Google Scholar
Guo W L, Deng J, Wang J L, Wang L, Tai J P 2019 Acta Phys. Sin. 68 247303
Google Scholar
[2] Xia H, Lei L, Hong W Q, Xu S Q 2018 J. Alloy Compd. 757 239
Google Scholar
[3] 苏小娜, 万英, 周芷萱, 胡莲莲 2017 物理学报 66 230701
Google Scholar
Su X N, Wan Y, Zhou Z X, Hu L L 2017 Acta Phys. Sin. 66 230701
Google Scholar
[4] Jiang G C, Wei X T, Chen Y H, Duan C K, Yin M, Yang B, Cao W W 2015 Mater. Lett. 143 98
Google Scholar
[5] Du P, Wu Y F, Yu J S 2018 RSC Adv. 12 6419
Google Scholar
[6] Du P, Yu J S 2016 Mater. Res. Bull. 84 303
Google Scholar
[7] Du P, Huang X Y, Yu J S 2018 Chem. Eng. J. 337 91
Google Scholar
[8] 梁思思, 尚蒙蒙, 林君 2018 物理化学学报 34 237
Google Scholar
Liang S S, Shang M M, Lin J 2018 Acta Phys-Chem. Sin. 34 237
Google Scholar
[9] 曹逊, 曹翠翠, 孙光耀, 金平实 2019 无机材料学报 34 1145
Google Scholar
Cao X, Cao C C, Sun G Y, Jin P S 2019 J. Inorg. Mater. 34 1145
Google Scholar
[10] Tian L, Wang L X, Zhang L, Zhang Q T, Ding W H, Yu M X 2015 J. Mater. Sci-Mater El. 26 8507
Google Scholar
[11] Hsu C H, Das S, Lu C H 2012 J. Electro. Chem. Soc. 159 193
Google Scholar
[12] Meng J X, Yang C T, Chen Q Q 2010 J. Lumin. 130 1320
Google Scholar
[13] Wu Z C, Liu J, Hou W G 2010 J. Alloy Compd. 498 139
Google Scholar
[14] Du P, Yu J S 2017 Dyes. Pigments. 147 16
Google Scholar
[15] Luwang M N, Ningthoujam R S, Srivastava S K 2011 J. Mater. Chem. 21 5326
Google Scholar
[16] 任艳东, 吕树臣 2011 物理学报 60 087804
Google Scholar
Ren Y D, Lü S C 2011 Acta Phys. Sin. 60 087804
Google Scholar
[17] 孟庆裕, 李明, 刘林峰, 曲秀荣, 万维龙, 孙江亭 2012 物理学报 61 107804
Google Scholar
Meng Q Y, Li M, Liu L F, Qu X R, Wan W L, Sun J T 2012 Acta Phys. Sin. 61 107804
Google Scholar
[18] 刘艳, 姜莹莹, 刘桂霞, 王进贤 2013 无机化学学报 29 277
Google Scholar
Liu Y, Jiang Y Y, Liu G X, Wang J X 2013 Inorg. Chem. 29 277
Google Scholar
[19] Du P, Wu S Q, Yu J S 2016 J. Lumin. 173 192
Google Scholar
[20] Jiang H X, Lü S C 2021 Mater. Res. Bull. 135 111123
Google Scholar
[21] Li L L, Yang X Y, Li J Q, et al. 2020 J. Lumin. 173 117377
Google Scholar
[22] 毕长虹, 孟庆裕 2013 物理学报 19 197804
Google Scholar
Bi C H, Meng Q Y 2013 Acta Phys. Sin. 19 197804
Google Scholar
[23] Chanu T T T, Singh N R 2016 J. Mater. Sci-Mater. El. 28 3909
Google Scholar
[24] Liu Y, Liu G X, Dong X T, Wang J X, Yu W S 2014 RSC Adv. 4 58708
Google Scholar
[25] Cao R P, Xu H D, Peng D D, Jiang S H 2015 Supperlattice Microst. 88 5
Google Scholar
[26] Zhai Y Q, Wang M, Zhao Q, Yang H L, Ding H H 2016 J. Mater. Sci-Mater. El. 27 279
Google Scholar
[27] Durirajan A, Balaji D, Kavi Rasu K, et al. 2016 J. Lumin. 170 743
Google Scholar
[28] 陈炳炎, 刘粤惠, 陈东丹, 姜中宏 2005 物理学报 54 3418
Google Scholar
Chen B Y, Liu Y H, Chen D D, Jiang Z H 2005 Acta Phys. Sin. 54 3418
Google Scholar
[29] 孟庆裕, 刘志鑫, 孙文军 2013 物理学报 62 097801
Google Scholar
Meng Q Y, Liu Z X, Sun W J 2013 Acta Phys. Sin. 62 097801
Google Scholar
[30] Dexter D L, Schulman J H 1954 J. Chem. Phys. 22 1063
Google Scholar
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