Pr3+共掺杂调控的Li0.9K0.1NbO3:Er3+荧光粉上/下转换双模式光学测温研究

贾朝阳; 杨雪; 王志刚; 柴瑞鹏; 庞庆; 张翔宇; 高当丽

doi:10.7498/aps.72.20231170

摘要

光热传感对于智能穿戴设备的开发至关重要. 然而, 设计合成具有合适多波长发射的发光材料, 并在单一材料体系中利用多组探针构建宽温度范围的高灵敏温度传感器是一个巨大挑战. 本研究采用高温固相法成功制备了Li_0.9K_0.1NbO₃:Pr³⁺/Er³⁺单掺及双掺荧光粉. 通过X射线衍射仪、扫描电子显微镜、荧光光谱仪以及自制的加热装置对其结构、形貌及激发波长和温度依赖的荧光特性进行了表征. 详细研究了Er³⁺单掺与Pr³⁺, Er³⁺共掺样品的上/下转换荧光及Er³⁺的双模荧光温度传感特性. 结果表明: Pr³⁺掺杂优化了Li_0.9K_0.1NbO₃:Er³⁺荧光粉中源自于Er³⁺离子热耦合能级的双模光学测温性能. 本研究为温度探测提供了材料基础和光学测温技术.

关键词:

Abstract

Photothermal sensing is crucial in developing smart wearable devices. However, designing and synthesizing luminescent materials with suitable multi-wavelength emission and constructing multiple sets of probes in a single material system is a huge challenge for constructing sensitive temperature sensors with a wide temperature range. In this paper, Pr³⁺, Er³⁺ single-doped and double-doped Li_0.9K_0.1NbO₃ phosphors are successfully prepared by high temperature solid phase method, and their structures, morphologies, excitation wavelengths and temperature-dependent fluorescence properties are characterized by XRD, SEM, fluorescence spectrometer and self-made heating device. Firstly, the photoluminescences of the synthesized series of samples are investigated. The results show that comparing with the single-doped Li_0.9K_0.1NbO₃: Er³⁺ sample, the up/down-conversion spectra of Pr³⁺, Er³⁺ co-doped phosphors under 808 nm/380 nm excitation show that the green fluorescence emission of Er³⁺ is enhanced. In addition, under 980 nm excitation, Pr³⁺ can effectively regulate the fluorescence energy level population pathway, so that the electrons are more effectively arranged in the ²H_11/2 and ⁴S_3/2 energy levels in the excitation process. The red emission is weakened and the green emission is enhanced, which improves the signal resolution of the fluorescent material and has a significant influence on the optical temperature measurement. Secondly, the up-conversion fluorescence property of Er³⁺ under 808 nm/980 nm laser excitation in Li_0.9K_0.1NbO₃:Er³⁺ and Li_0.9K_0.1NbO₃:Pr³⁺,Er³⁺ phosphors are investigated. The results show that the red and green fluorescence emissions of Er³⁺ are two-photon processes. Finally, the up/down-conversion dual-mode temperature sensing properties of Er³⁺ in Li_0.9K_0.1NbO₃:Er³⁺ and Li_0.9K_0.1NbO₃:Pr³⁺, Er³⁺ phosphors are investigated. It is found that both materials have good optical temperature measurement performances. The Pr³⁺ doping optimizes the dual-mode optical temperature measurement performances of Li_0.9K_0.1NbO₃:Er³⁺ phosphors derived from the thermal coupling energy level of Er³⁺ ions. In addition, the up/down-conversion fluorescence mechanism of Li_0.9K_0.1NbO₃:Er³⁺ and Li_0.9K_0.1NbO₃:Er³⁺, Pr³⁺ phosphors are proposed, and the enhanced green fluorescence by Pr³⁺ co-doping is attributed to the energy transfer from Pr³⁺ ions to Er³⁺ ions, leading to the increase of green fluorescence level population and the decrease of red fluorescence level population of the Er³⁺ ions. This new dual-mode optical temperature measurement material provides a material basis and optical temperature measurement technology for exploring other temperature measurement materials.

Keywords:

作者及机构信息

1.
西安建筑科技大学理学院, 西安　710055

2.
长安大学理学院, 西安　710064

通信作者: 高当丽, gaodangli@163.com

基金项目: 国家自然科学基金(批准号: 11604253, 51672208)、陕西省重点科技创新团队项目(批准号: 2022TD-34)和中央高校基本科研业务费专项资金(批准号: 300102120101)资助的课题.

Authors and contacts

1.
College of Science, Xi’an University of Architecture and Technology, Xi’an 710055, China

2.
College of Science, Chang’an University, Xi’an 710064, China

Corresponding author: Gao Dang-Li, gaodangli@163.com

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 11604253, 51672208), the Key Science and Technology Innovation Team of Shaanxi Province, China (Grant No. 2022TD-34), and the Fundamental Research Funds for the Central Universities, China (Grant No. 300102120101).

文章全文

参考文献

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施引文献

图 1 (a) Li_0.9K_0.1NbO₃:Ln³⁺系列样品的XRD图; (b) Li_0.9K_0.1NbO₃的晶体结构图

Fig. 1. (a) XRD patterns of a series of Li_0.9K_0.1NbO₃:Ln³⁺ samples; (b) crystal structure of Li_0.9K_0.1NbO₃.

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图 2 Li_0.9K_0.1NbO₃:Ln³⁺样品的SEM图片及EDX元素谱　(a) Li_0.9K_0.1NbO₃:Er³⁺的SEM图片; (b) Li_0.9K_0.1NbO₃:Pr³⁺, Er³⁺的SEM图片; (c) Li_0.9K_0.1NbO₃:Er³⁺荧光粉的EDX元素分布图谱

Fig. 2. SEM images and element mappings of Li_0.9K_0.1NbO₃:Ln³⁺ phosphors: (a) SEM image of Li_0.9K_0.1NbO₃:Er³⁺; (b) SEM image of Li_0.9K_0.1NbO₃:Pr³⁺, Er³⁺; (c) EDX elemental distribution spectra of Li_0.9K_0.1NbO₃:Er³⁺ phosphors.

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图 3 不同波长激发下, Li_0.9K_0.1NbO₃:Ln³⁺的上/下转换发射谱比较　(a) Pr³⁺和Er³⁺单掺样品及Pr³⁺, Er³⁺共掺样品的发射谱 (λ_ex = 280 nm/380 nm); (b) Pr³⁺, Er³⁺共掺样品的激发谱(λ_moni = 554 nm/620 nm); Er³⁺单掺及Pr³⁺, Er³⁺共掺样品在(c) λ_ex= 808 nm, (d) 980 nm激光激发下的上转换发射谱

Fig. 3. Comparison of up-conversion and down-conversion emission spectra of rare earth doped Li_0.9K_0.1NbO₃:Ln³⁺ under different excitation wavelengths: (a) Emission spectra of Pr³⁺ and Er³⁺ single-doped samples and Pr³⁺, Er³⁺ co-doped samples (λ_ex = 280 nm/380 nm); (b) excitation spectra of Pr³⁺, Er³⁺ co-doped samples (λ_moni = 554 nm/620 nm); (c), (d) up-conversion emission spectra of Er³⁺ single doped and Pr³⁺, Er³⁺ co-doped samples under 808 and 980 nm excitations.

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图 4 激发功率依赖的Li_0.9K_0.1NbO₃:Er³⁺和Li_0.9K_0.1NbO₃:Pr³⁺, Er³⁺荧光粉的发射谱, 其中内插图为对应发光强度与入射激光的功率关系　(a), (b) Li_0.9K_0.1NbO₃:Er³⁺荧光粉的发射谱(λ_ex = 808 nm和λ_ex = 980 nm); (c), (d) Li_0.9K_0.1NbO₃:Pr³⁺, Er³⁺荧光粉的发射谱(λ_ex = 808 nm和λ_ex = 980 nm)

Fig. 4. Excitation power-dependent emission spectra of Li_0.9K_0.1NbO₃:Er³⁺ and Li_0.9K_0.1NbO₃:Pr³⁺, Er³⁺ phosphors, where the insets are the relationships between luminescence intensity and incident laser power: (a), (b) Emission spectra of Li_0.9K_0.1NbO₃:Er³⁺ phosphors (λ_ex = 808 nm and λ_ex = 980 nm); (c), (d) emission spectra of Li_0.9K_0.1NbO₃:Pr³⁺, Er³⁺ phosphors (λ_ex = 808 nm and λ_ex = 980 nm).

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图 5 Li_0.9K_0.1NbO₃:Er³⁺荧光粉的上、下转换测温性能　(a)—(c) 分别在380, 808, 980 nm激发下的发射谱; (d)—(f) 相应于图(a)—(c)中的上/下转换发射谱的双峰绿色FIR与温度的关系; (g)—(i) 相应于图(d)—(f)中双峰荧光强度比率测温的灵敏度曲线

Fig. 5. Up/down-conversion temperature measurement performance of Li_0.9K_0.1NbO₃:Er³⁺ phosphor: (a)–(c) The emission spectra excited at 380, 808 and 980 nm, respectively; (d)–(f) the relationship between the bimodal green FIR and temperature corresponding to the up/down-conversion emission spectra in panel (a)–(c); (g)–(i) the sensitivity curves of temperature measurement of bimodal FIR corresponding to panel (d)–(f).

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图 6 Li_0.9K_0.1NbO₃:Pr³⁺, Er³⁺荧光粉的上/下转换双模式光学测温性能　(a)—(c) 分别在380, 808, 980 nm激发下的发射谱; (d)—(f) 相应于图(a)—(c)中的上/下转换发射谱的双峰绿色FIR与温度的关系; (g)—(i) 相应于图(d)—(f)中双峰FIR测温的灵敏度曲线

Fig. 6. Up/down-conversion temperature measurement performance of Li_0.9K_0.1NbO₃:Pr³⁺, Er³⁺ phosphor: (a)–(c) The emission spectra excited at 380, 808, and 980 nm, respectively; (d)–(f) the relationship between the bimodal green FIR and temperature corresponding to the up/down-conversion emission spectra in panel (a)–(c); (g)–(i) the sensitivity curves of temperature measurement of bimodal FIR corresponding to panel (d)–(f).

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图 7 源自于Li_0.9K_0.1NbO₃:Er³⁺和Li_0.9K_0.1NbO₃:Er³⁺, Pr³⁺荧光粉的上/下转换荧光机理图, 其中, VB表示价带, CB表示导带

Fig. 7. Proposed mechanism of up/down-conversion fluorescence of Li_0.9K_0.1NbO₃:Er³⁺ and Li_0.9K_0.1NbO₃:Er³⁺, Pr³⁺ phosphors. Therein, VB and CB represent valence band and conduction band, respectively.

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表 1 基于FIR技术下不同基质中掺杂Er³⁺的温度传感材料光学参数

Table 1. Optical parameters of temperature sensing materials doped with Er³⁺ in different substrates based on FIR technology

Materials	Wavelength/nm	S_r-Max/(10^–2 K^–1)	S_a-Max/(10^–2 K^–1)	References
SrSnO₃:Er	975 nm	0.997(294 K)	0.791(368 K)	[30]
BaBiNb₂O₉:Er	980 nm	0.959(300 K)	0.996(483 K)	[36]
La₂CaZnO₅:Er	378 nm	1.454(300 K)	—	[31]
Sr₂Gd₈(SiO₄)₆O₂:Er	379 nm	—	0.34(463 K)	[32]
Ca₃Bi(PO₄)₃:Er	376 nm	1.21(300 K)	0.312(473 K)	[33]
La₂Mo₂O₉:Er	980 nm	1.16(293 K)	0.527(493 K)	[37]
(K, Na)NbO₃:Er	980 nm 375 nm	0.96(303 K) 16.17(80 K)	0.28(433 K) 0.37(280 K)	[38]
Cs₃Bi₂Cl₉:Er	808 nm 980 nm	1.4(303 K) 1.38(303 K)	0.62(573 K) 0.61(573 K)	[13]
Li_0.9K_0.1NbO₃:Er	380 nm 808 nm 980 nm	0.97(303 K) 1.286(297 K) 1.221(297 K)	0.44(463 K) 0.89(443 K) 0.81(443 K)	This work

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表 2 基于FIR技术下不同基质中掺杂Er³⁺-Ln³⁺的温度传感材料光学参数

Table 2. Optical parameters of temperature sensing materials doped with Er³⁺-Ln³⁺ in different substrates based on FIR technology.

Materials	Wavelength/nm	S_r-Max/(10^–2 K^–1)	S_a-Max/(10^–2 K^–1)	References
La₂MgGeO₆:Bi, Er	980 nm	1.23(293 K)	0.94(473 K)	[39]
K₃Gd(PO₄)₂:Yb, Er, Tm	980 nm	1.35(300 K)	0.456(608 K)	[40]
NaLuF₄:Er, Tm	1532 nm	1.265(293 K)	0.4(519 K)	[41]
BiVO₄:Er, Tm	980 nm	1.1(293 K)	0.7(473 K)	[42]
BiVO₄:Er, Tm	1550 nm	1.1(293 K)	0.56(453 K)	[42]
Y₂SiO₅:Er, Tm	808 nm	0.395(298 K)	—	[29]
KYb(MoO₄)₂:Er, Gd	980 nm	1.1(303 K)	0.97(513 K)	[25]
KYb(MoO₄)₂:Er, La		1.1(303 K)	0.95(513 K)
KYb(MoO₄)₂:Er, Y		1.11(303 K)	0.91(513 K)
Li_0.9K_0.1NbO₃:Pr, Er	380 nm	1.12(296 K)	0.54(434 K)	This work
	808 nm	1.284(296 K)	1.12(443 K)
	980 nm	1.106(296 K)	0.83(443 K)

下载: 导出CSV

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Pr³⁺共掺杂调控的Li_0.9K_0.1NbO₃:Er³⁺荧光粉上/下转换双模式光学测温研究

Dual-mode up/down-conversion optical thermometry of Pr³⁺-regulated Li_0.9K_0.1NbO₃:Er³⁺ phosphors

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1.
西安建筑科技大学理学院, 西安　710055

2.
长安大学理学院, 西安　710064

通信作者: 高当丽, gaodangli@163.com

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1.
College of Science, Xi’an University of Architecture and Technology, Xi’an 710055, China

2.
College of Science, Chang’an University, Xi’an 710064, China

Corresponding author: Gao Dang-Li, gaodangli@163.com

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