Dy3+: Y3Al5O12晶体的光谱与黄色激光性能

doi:10.15541/jim20220386

无机材料学报 ›› 2023, Vol. 38 ›› Issue (3): 350-356.DOI: 10.15541/jim20220386

Dy³⁺: Y₃Al₅O₁₂晶体的光谱与黄色激光性能

杨佳雪¹^,²(), 李雯¹^,³, 王燕¹^,⁴(), 朱昭捷¹^,⁴, 游振宇¹^,⁴, 李坚富¹^,⁴, 涂朝阳¹^,⁴()

1.中国科学院福建物质结构研究所, 福州 350002
2.福州大学化学学院, 福州 350116
3.福州大学材料科学与工程学院, 福州 350116
4.中国福建光电信息科学与技术创新实验室(闽都创新实验室), 福州 350108

收稿日期:2022-07-05 修回日期:2022-08-16 出版日期:2021-11-16 网络出版日期:2022-11-16
通讯作者: 王燕, 研究员. E-mail: wy@fjirsm.ac.cn;
涂朝阳, 研究员. E-mail: tcy@fjirsm.ac.cn
作者简介:杨佳雪(1995-), 女, 硕士研究生. E-mail: yangjiaxue@fjirsm.ac.cn

Spectroscopic and Yellow Laser Features of Dy³⁺: Y₃Al₅O₁₂ Single Crystals

YANG Jiaxue¹^,²(), LI Wen¹^,³, WANG Yan¹^,⁴(), ZHU Zhaojie¹^,⁴, YOU Zhenyu¹^,⁴, LI Jianfu¹^,⁴, TU Chaoyang¹^,⁴()

1. Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China
2. College of Chemistry, Fuzhou University, Fuzhou 350116, China
3. School of Materials Science and Engineering, Fuzhou University, Fuzhou 350116, China
4. Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou 350108, China

Received:2022-07-05 Revised:2022-08-16 Published:2021-11-16 Online:2022-11-16
Contact: WANG Yan, professor. E-mail: wy@fjirsm.ac.cn;
TU Chaoyang, professor. E-mail: tcy@fjirsm.ac.cn
About author:YANG Jiaxue (1995-), female, Mater candidate. E-mail: yangjiaxue@fjirsm.ac.cn
Supported by:
National Natural Science Foundation of China(51872286);National Natural Science Foundation of China(51832007);Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China(2021ZR204);Science and Technology Plan Leading Project of Fujian Province(2022H0043);Science and Technology Plan Leading Project of Fujian Province(2020H0036);Natural Science Foundation of Jiangxi Province(20181BAB211009)

摘要/Abstract

摘要：

近年来, 黄色激光晶体在激光显示、激光医疗、激光雷达(光探测和测距)、玻色-爱因斯坦凝聚、原子冷却和俘获等领域具有广泛的应用, 吸引了研究人员极大的兴趣。随着蓝光LD泵浦源的商用化, 直接泵浦Dy³⁺掺杂激光晶体可输出黄色激光, 对应⁴F_9/2→⁶H_13/2跃迁。本工作采用提拉法生长了Dy³⁺掺杂浓度分别为0.5%、1.0%、2.0%、3.0%和4.0%(原子分数)的Dy³⁺: Y₃Al₅O₁₂(Dy:YAG)晶体, 并分析了晶体开裂的原因。基于Judd-Ofelt理论计算了J-O强度参数, 并利用其评估了不同掺杂浓度的Dy:YAG晶体的其它激光参数。综合讨论了Dy³⁺掺杂浓度对荧光分支比、受激发射截面、量子效率等光谱性能的影响。在五个晶体样品中, 1.0%Dy: YAG晶体在447 nm激发下实现了582 nm最大的受激发射截面值和最强的荧光强度值, 荧光寿命较长, 达到0.823 ms。与之相比, 2.0%Dy: YAG晶体发射参数值略低, 但是其吸收系数更大。研究结果表明, 激光二极管泵浦的Dy:YAG黄色激光晶体中Dy³⁺离子的浓度为1.0%和2.0%较为合适, 并基于2.0%Dy: YAG晶体实现了连续黄色激光输出, 最大功率为166.8 μW, 激光峰值波长为582.5 nm。

关键词: YAG晶体, Dy³⁺, 晶体生长, 荧光特性, 黄色激光

Abstract:

In recent years, yellow laser crystals have raised great attentions owing to their comprehensive applications in the fields such as laser display, laser medical treatment, light detection and ranging (LIDAR), Bose-Einstein condensates, and atomic cooling and trapping. With the development of commercial blue light LD, the direct pumping of Dy³⁺ doped laser crystals has realized yellow laser based on its transition ⁴F_9/2→⁶H_13/2. In this work, Dy³⁺: Y₃Al₅O₁₂ (Dy: YAG) crystals with 0.5%, 1.0%, 2.0%, 3.0%, and 4.0% (atomic fraction) nominal concentration of Dy³⁺ were grown using Czochralski method, the reason of crystal crack was discussed. Based on Judd-Ofelt (J-O) theory, the J-O intensity parameters and utilization, and other laser parameters of Dy: YAG crystals with different doping concentrations were evaluated. The effect of the doping concentration of Dy³⁺on the spectroscopic performances like fluorescence branching ratio, stimulated emission cross-section, quantum efficiency, were analyzed comprehensively. Among all the five crystals, 1.0% Dy: YAG has the largest stimulated emission cross-section for 582 nm yellow emission, an intense fluorescence intensity with the 447 nm excitation, and a longer decay time of 0.823 ms. The fluorescence intensity and stimulated emission cross-section of 2.0% Dy: YAG are slightly less than that of 1.0% Dy: YAG, but the former has a higher absorption coefficient. Hence, the spectroscopic analysis results show that 1.0% and 2.0% are the suitable concentrations of Dy³⁺ ion in YAG crystal for yellow laser operation by diode pumping. The continuous wave laser with peak at 582.5 nm and the maximum output power of 166.8 μW yellow laser operation were realized in 2.0% Dy: YAG crystal.

Key words: YAG crystal, Dy³⁺, crystal growth, fluorescence features, yellow laser

中图分类号:

TN244

杨佳雪, 李雯, 王燕, 朱昭捷, 游振宇, 李坚富, 涂朝阳. Dy³⁺: Y₃Al₅O₁₂晶体的光谱与黄色激光性能[J]. 无机材料学报, 2023, 38(3): 350-356.

YANG Jiaxue, LI Wen, WANG Yan, ZHU Zhaojie, YOU Zhenyu, LI Jianfu, TU Chaoyang. Spectroscopic and Yellow Laser Features of Dy³⁺: Y₃Al₅O₁₂ Single Crystals[J]. Journal of Inorganic Materials, 2023, 38(3): 350-356.

图/表 8

Fig. 1 Photos of the as-grown single crystals

Fig. 2 Absorption spectra of Dy: YAG crystals

Table 1 Concentration, effective segregation coefficient and absorption cross-section of Dy3+ in YAG crystal

Crystal	c/% (in atomic)	k_eff	N_c/cm^-3	α/cm^-1	σ_abs/cm²
0.5% Dy: YAG	0.239	0.478	3.31×10¹⁹	0.055	1.66×10^-21
1.0% Dy: YAG	0.479	0.479	6.61×10¹⁹	0.103	1.56×10^-21
2.0% Dy: YAG	0.970	0.485	1.33×10²⁰	0.215	1.61×10^-21
3.0% Dy: YAG	1.427	0.475	1.95×10²⁰	0.338	1.73×10^-21
4.0% Dy: YAG	1.975	0.494	2.69×10²⁰	0.430	1.60×10^-21

Table 2 Experimental line strength, calculated line strength, and J-O intensity parameters of Dy: YAG crystals

⁶H_15/2→	$λ ¯$ /nm	n	0.5%Dy: YAG			1.0%Dy: YAG			2.0%Dy: YAG			3.0%Dy: YAG			4.0%Dy: YAG
⁶H_15/2→	$λ ¯$ /nm	n	S_exp/ (×10^-20, cm²)		S_cal/ (×10^-20, cm²)	S_exp/ (×10^-20, cm²)		S_cal/ (×10^-20, cm²)	S_exp/ (×10^-20, cm²)		S_cal/ (×10^-20, cm²)	S_exp/ (×10^-20, cm²)		S_cal/ (×10^-20, cm²)	S_exp/ (×10^-20, cm²)		S_cal/ (×10^-20, cm²)
⁴M_17/2+⁶P_3/2+ ⁴G_9/2+⁴I_9/2	327	1.89	0.447		0.298	0.460		0.320	0.526		0.323	0.498		0.327	0.467		0.341
⁶P_7/2+⁴I_11/2	353	1.88	0.905		0.723	1.128		0.850	1.371		1.182	1.719		1.454	1.648		1.403
⁶P_5/2+⁴M_19/2	367	1.87	0.733		0.474	0.806		0.511	0.907		0.525	0.898		0.540	0.918		0.560
⁴K_17/2+⁴M_21/2+ ⁴I_13/2+⁴F_7/2	387	1.86	0.651		0.729	0.723		0.793	0.801		0.854	0.851		0.908	0.873		0.925
⁴I_15/2	451	1.85	0.257		0.178	0.253		0.191	0.187		0.191	0.213		0.192	0.227		0.199
⁶F_3/2	755	1.82	0.217		0.158	0.189		0.170	0.202		0.171	0.225		0.173	0.205		0.181
⁶F_5/2	804	1.82	1.083		0.909	1.140		0.975	1.266		0.983	1.252		0.996	1.228		1.039
⁶F_7/2	908	1.82	2.07		2.057	2.361		2.226	2.243		2.328	2.462		2.426	2.565		2.502
⁶H_7/2+⁶F_9/2	1088	1.81	2.577		2.741	2.74		3.022	3.249		3.403	3.480		3.731	3.528		3.767
RMS/(×10^-20, cm²)				0.180			0.230			0.237			0.246			0.226
Ω_t₍_t_{=2, 4, 6)}/(×10^-20, cm²)				Ω₂=0.793 Ω₄=1.284 Ω₆=2.634			Ω₂=0.747 Ω₄=1.520 Ω₆=2.825			Ω₂=0.498 Ω₄=2.155 Ω₆=2.848			Ω₂=0.312 Ω₄=2.674 Ω₆=2.887			Ω₂=0.142 Ω₄=2.573 Ω₆=3.011

Table 2 Experimental line strength, calculated line strength, and J-O intensity parameters of Dy: YAG crystals

⁶H_15/2→	$λ ¯$ /nm	n	0.5%Dy: YAG			1.0%Dy: YAG			2.0%Dy: YAG			3.0%Dy: YAG			4.0%Dy: YAG
⁶H_15/2→	$λ ¯$ /nm	n	S_exp/ (×10^-20, cm²)		S_cal/ (×10^-20, cm²)	S_exp/ (×10^-20, cm²)		S_cal/ (×10^-20, cm²)	S_exp/ (×10^-20, cm²)		S_cal/ (×10^-20, cm²)	S_exp/ (×10^-20, cm²)		S_cal/ (×10^-20, cm²)	S_exp/ (×10^-20, cm²)		S_cal/ (×10^-20, cm²)
⁴M_17/2+⁶P_3/2+ ⁴G_9/2+⁴I_9/2	327	1.89	0.447		0.298	0.460		0.320	0.526		0.323	0.498		0.327	0.467		0.341
⁶P_7/2+⁴I_11/2	353	1.88	0.905		0.723	1.128		0.850	1.371		1.182	1.719		1.454	1.648		1.403
⁶P_5/2+⁴M_19/2	367	1.87	0.733		0.474	0.806		0.511	0.907		0.525	0.898		0.540	0.918		0.560
⁴K_17/2+⁴M_21/2+ ⁴I_13/2+⁴F_7/2	387	1.86	0.651		0.729	0.723		0.793	0.801		0.854	0.851		0.908	0.873		0.925
⁴I_15/2	451	1.85	0.257		0.178	0.253		0.191	0.187		0.191	0.213		0.192	0.227		0.199
⁶F_3/2	755	1.82	0.217		0.158	0.189		0.170	0.202		0.171	0.225		0.173	0.205		0.181
⁶F_5/2	804	1.82	1.083		0.909	1.140		0.975	1.266		0.983	1.252		0.996	1.228		1.039
⁶F_7/2	908	1.82	2.07		2.057	2.361		2.226	2.243		2.328	2.462		2.426	2.565		2.502
⁶H_7/2+⁶F_9/2	1088	1.81	2.577		2.741	2.74		3.022	3.249		3.403	3.480		3.731	3.528		3.767
RMS/(×10^-20, cm²)				0.180			0.230			0.237			0.246			0.226
Ω_t₍_t_{=2, 4, 6)}/(×10^-20, cm²)				Ω₂=0.793 Ω₄=1.284 Ω₆=2.634			Ω₂=0.747 Ω₄=1.520 Ω₆=2.825			Ω₂=0.498 Ω₄=2.155 Ω₆=2.848			Ω₂=0.312 Ω₄=2.674 Ω₆=2.887			Ω₂=0.142 Ω₄=2.573 Ω₆=3.011

Table 3 Spontaneous emission transition rate (A) and fluorescence branching ratio (β) of Dy: YAG crystals

⁴F_9/2→^2S+1L_J	0.5%Dy: YAG		1.0%Dy: YAG		2.0%Dy: YAG		3.0%Dy: YAG		4.0%Dy: YAG
⁴F_9/2→^2S+1L_J	A/s^-1	β/%	A/s^-1	β/%	A/s^-1	β/%	A/s^-1	β/%	A/s^-1	β/%
⁶F_1/2	0.08	0.01	0.10	0.01	0.14	0.01	0.17	0.02	0.16	0.02
⁶F_3/2	0.15	0.02	0.16	0.02	0.16	0.02	0.16	0.02	0.17	0.02
⁶F_5/2	1.82	0.20	1.81	0.19	1.54	0.15	1.34	0.13	1.05	0.10
⁶F_7/2	13.63	1.49	14.26	1.46	7.29	1.53	8.21	1.58	8.18	1.57
⁶H_5/2	4.02	0.44	4.58	0.47	5.78	0.58	6.78	0.66	6.67	0.65
⁶H_7/2+⁶F_9/2	54.73	5.96	59.10	6.04	49.39	6.71	56.13	7.19	55.44	7.10
⁶H_9/2	17.78	1.94	18.84	1.93	15.42	1.98	16.34	2.02	16.13	1.99
⁶H_11/2	43.30	4.72	44.21	4.52	25.93	4.26	24.99	4.06	23.05	3.85
⁶H_13/2	456.91	49.79	483.85	49.46	482.81	48.22	486.21	47.34	479.08	46.58
⁶H_15/2	325.23	35.44	351.44	35.92	365.79	36.54	379.80	36.98	392.16	38.13
τ_r/ms	1.090		1.022		0.999		0.974		0.972

Fig. 3 Emission spectra of YAG crystals with different Dy3+ concentrations excited by 447 nm (a) and variation of intensity of 582 nm and 4F9/2 level lifetime with Dy3+ concentrations in Dy: YAG crystals (b)

Table 4 Emission property parameters of Dy3+ in YAG and other crystals

Crystal	τ_r(⁴F_9/2level)/ms	τ(⁴F_9/2level)/ms	σ_emfor yellow emission/(×10^-21, cm²)	σ_emτ/(×10^-21, cm²∙ms)	η/%	Ref.
0.5%Dy: YAG	1.090	0.894	2.36	2.110	82.02	This work
1.0%Dy: YAG	1.022	0.823	2.71	2.230	80.53
2.0%Dy: YAG	0.999	0.688	2.66	1.830	68.87
3.0%Dy: YAG	0.974	0.571	2.54	1.450	58.62
4.0%Dy: YAG	0.972	0.471	2.49	1.170	48.46
1.0%Dy³⁺: Gd₃Ga₃Al₂O₁₂	0.596	0.573	3.20	1.834	96.14	[13]
3.0%Dy³⁺: Lu₂O₃	0.756	0.112	7.10	7.952	14.80	[14]
2.0%Dy³⁺: CeF₃	3.747	1.530	9.259	0.1417	40.83	[17]
1.0%Dy³⁺: GdScO₃	0.650	0.459	4.10	1.882	70.60	[34]
2.0%Dy³⁺: Gd₃Ga₅O₁₂	1.107	0.790	2.62	2.070	71.40	[35]
2.0%Dy³⁺: LaF₃	1.700	1.370	7.00	9.590	80.59	[36]

Fig. 4 Laser spectra (a) and variation of output power with absorbed pump power of 2.0%Dy: YAG crystal (b)

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Dy³⁺: Y₃Al₅O₁₂晶体的光谱与黄色激光性能

Spectroscopic and Yellow Laser Features of Dy³⁺: Y₃Al₅O₁₂ Single Crystals

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