Ho:BaF2晶体在近红外-中红外波段光谱性能分析

doi:10.15541/jim20250349

无机材料学报 ›› 2026, Vol. 41 ›› Issue (5): 595-603.DOI: 10.15541/jim20250349 CSTR: 32189.14.10.15541/jim20250349

Ho:BaF₂晶体在近红外-中红外波段光谱性能分析

钱新宇¹(), 王无敌¹, 郭俊尧¹, 任永春¹, 董建树¹, 王庆国¹(), 唐慧丽¹, 张晨波¹, 徐晓东², 董永军³, 华伟⁴, 徐军¹()

¹ 同济大学高等研究院, 物理科学与工程学院, 先进微结构材料教育部重点实验室, 上海 200092
² 江苏师范大学物理与电子工程学院, 江苏省先进激光材料与器件重点实验室, 徐州 221116
³ 上海芯飞睿科技有限公司, 上海 300444
⁴ 宁波镭晶科技有限公司, 宁波 315500

收稿日期:2025-09-02 修回日期:2025-10-08 出版日期:2026-05-20 网络出版日期:2025-11-26
通讯作者: 徐军, 教授. E-mail: 15503@tongji.edu.cn;
王庆国, 高级工程师. E-mail: qgwang@tongji.edu.cn
作者简介:钱新宇(1998-), 男, 博士研究生. E-mail: 894742295@qq.com
基金资助:
国家重点研发计划(2022YFB3605701);国家重点研发计划(2023YFB3507401);国家自然科学基金(62275198);国家自然科学基金(52032009)

Spectroscopic Analysis of Ho:BaF₂ Crystals in the NIR to MIR Spectral Region

QIAN Xinyu¹(), WANG Wudi¹, GUO Junyao¹, REN Yongchun¹, DONG Jianshu¹, WANG Qingguo¹(), TANG Huili¹, ZHANG Chenbo¹, XU Xiaodong², DONG Yongjun³, HUA Wei⁴, XU Jun¹()

¹ Key Laboratory of Advanced Micro-Structured Materials, School of Physical Science and Engineering, Institute for Advanced Study, Tongji University, Shanghai 200092, China
² Jiangsu Provincial Key Laboratory of Advanced Laser Materials and Devices, School of Physics and Electronic Engineering, Jiangsu Normal University, Xuzhou 221116, China
³ Shanghai Xinfeirui Technology Co., Ltd., Shanghai 300444, China
⁴ Ningbo Leijing Technology Co., Ltd., Ningbo 315500, China

Received:2025-09-02 Revised:2025-10-08 Published:2026-05-20 Online:2025-11-26
Contact: XU Jun, professor. E-mail: 15503@tongji.edu.cn;
WANG Qingguo, senior engineer. E-mail: qgwang@tongji.edu.cn
About author:QIAN Xinyu (1998-), male, PhD candidate. E-mail: 894742295@qq.com
Supported by:
National Key R&D Program of China(2022YFB3605701);National Key R&D Program of China(2023YFB3507401);National Natural Science Foundation of China(62275198);National Natural Science Foundation of China(52032009)

摘要/Abstract

摘要：

1~3 μm红外激光在医疗、环境监测和高功率激光系统中具有重要应用价值, 其中Ho³⁺离子因其覆盖近红外至中红外多个发射通道而受到广泛关注。本工作系统研究了Ho:BaF₂晶体的结构与光谱特性, 并筛选不同发射波段的最佳掺杂浓度, 以实现高效多波段激光输出。采用温度梯度法(Temperature gradient technique, TGT)成功生长出原子比0.5%~3.0% Ho:BaF₂单晶。通过一系列表征手段进行结构和组分分析, 并利用吸收光谱、荧光光谱和寿命测试表征其光谱性能。同时结合Judd-Ofelt理论计算辐射跃迁参数。所有晶体均呈现立方晶系, 理论掺杂浓度和实际掺杂浓度接近1且分布均匀。光谱分析表明, ~1.2 μm (⁵I₆→⁵I₈)和~2.05 μm (⁵I₇→⁵I₈)的最优掺杂浓度为原子比2.0%(光谱品质因子Q分别为24.29×10^-21和67.53×10^-21 cm²·ms), 而~2.85 μm (⁵I₆→⁵I₇)的最优掺杂浓度为原子比1.0% (Q=44.52×10^-21 cm²·ms)。其中, BaF₂基质声子能量低(~346 cm^-1)及抗Ho³⁺离子团簇形成倾向较弱的特性使其在~2.05 μm处获得了3.81×10^-21 cm²的最大发射截面, 性能优于YAG、CaF₂等传统基质。相较于氧化物基质, BaF₂晶体具有更低的无辐射损耗和更强的抗浓度猝灭能力, 有助于实现更高有效掺杂浓度与稳定的多波段激光输出。Ho:BaF₂晶体展现出作为高效多波段红外激光增益介质的巨大潜力。

关键词: 氟化钡晶体, Ho³⁺离子掺杂, 中红外激光, 光谱性能

Abstract:

Infrared lasers in the 1-3 μm region are increasingly important for applications in medical treatment, atmospheric monitoring, and high-power laser systems. Holmium ions (Ho³⁺) are particularly attractive because of their multiple emission channels covering near to mid infrared ranges. This work aims to systematically evaluate the structural and spectroscopic properties of Ho:BaF₂ crystals and determine the optimal doping concentrations for efficient multi-band laser operation. High-quality Ho:BaF₂ single crystals with concentrations of 0.5%-3.0% (in atom) were grown using the temperature gradient technique (TGT). Structural characterization was performed, while spectroscopic properties were analyzed via absorption, fluorescence, and lifetime measurements. Judd-Ofelt analysis was further applied to calculate radiative parameters. All samples exhibited cubic structures, with doping segregation ratios close to unity and uniform Ho³⁺ distribution. Spectroscopic evaluation revealed optimal doping concentrations of 2.0% (in atom) for ~1.2 μm (⁵I₆→⁵I₈, spectral quality factor Q=24.29×10^-21 cm²·ms) and ~2.05 μm (⁵I₇→⁵I₈, Q=67.53×10^-21 cm²·ms), and 1.0% (in atom) for ~2.85 μm (⁵I₆→⁵I₇, Q=44.52×10^-21 cm²·ms). BaF₂ host, with its low phonon energy (~346 cm^-1) and anti-clustering characteristics, enabled enhanced emission performance, including a maximum emission cross-section of 3.81×10^-21 cm² at ~2.05 μm. These results outperform traditional hosts such as YAG and CaF₂. Compared to oxide hosts, BaF₂ offers superior lifetime, reduced non-radiative losses, and greater resistance to concentration quenching. The findings indicate that Ho:BaF₂ supports higher effective doping levels, making it particularly promising for high-power and ultrafast laser applications. Ho:BaF₂ crystals demonstrate excellent potential as efficient, multi-wavelength infrared laser gain media.

Key words: BaF₂ crystal, Ho³⁺ doping, mid-infrared laser, spectroscopic characteristic

中图分类号:

TQ174

钱新宇, 王无敌, 郭俊尧, 任永春, 董建树, 王庆国, 唐慧丽, 张晨波, 徐晓东, 董永军, 华伟, 徐军. Ho:BaF₂晶体在近红外-中红外波段光谱性能分析[J]. 无机材料学报, 2026, 41(5): 595-603.

QIAN Xinyu, WANG Wudi, GUO Junyao, REN Yongchun, DONG Jianshu, WANG Qingguo, TANG Huili, ZHANG Chenbo, XU Xiaodong, DONG Yongjun, HUA Wei, XU Jun. Spectroscopic Analysis of Ho:BaF₂ Crystals in the NIR to MIR Spectral Region[J]. Journal of Inorganic Materials, 2026, 41(5): 595-603.

图/表 10

图1 Ho3+离子红外波段发光的能级图

Fig. 1 Energy level diagram of Ho3+ ions for luminescence in the red spectral region

图2 多孔坩埚TGT生长的Ho:BaF2系列晶体

Fig. 2 Ho:BaF2 single crystals grown by porous-crucible TGT

图3 Ho:BaF2晶体和BaF2晶体标准样品的XRD图谱

Fig. 3 XRD patterns of Ho:BaF2 single crystals and BaF2 reference sample

表1 BaF2晶体中Ho3+离子掺杂实际浓度和掺杂偏析系数

Table 1 Actual concentration and doping segregation ratio of Ho3+ ions in BaF2 crystals

Sample	Initial concentration/% (in atom)	Actual concentration/% (in atom)	Doping segregation ratio
1	0.5	0.52	1.04
2	1.0	0.91	0.91
3	1.5	1.37	0.91
4	2.0	1.87	0.94
5	3.0	2.73	0.91

图4 Ho:BaF2晶体的吸收光谱

Fig. 4 Absorption spectra of the Ho:BaF2 crystals (a) 400-2200 nm range; (b) 5I8→5F5 transition; (c) 5I8→5I6 transition; (d) 5I8→5I7 transition. Colorful figures are available on website

表2 Ho:BaF2系列晶体在637 nm (5I8→5F5跃迁)、1157 nm (5I8→5I6跃迁)、1950 nm (5I8→5I7跃迁)的吸收截面和半高峰宽

Table 2 Absorption cross-sections (σabs) and full width at half maximum (FWHM) of Ho:BaF2 crystals at 637 nm (5I8 → 5F5 transition), 1157 nm (5I8 → 5I6 transition), and 1950 nm (5I8 → 5I7 transition)

Gain medium	Concentration/% (in atom)	637 nm (⁵I₈→⁵F₅)		1157nm (⁵I₈→⁵I₆)		1950 nm (⁵I₈→⁵I₇)
Gain medium	Concentration/% (in atom)	σ_abs/(×10^-21, cm²)	FWHM/nm	σ_abs/(×10^-21, cm²)	FWHM/nm	σ_abs/(×10^-21, cm²)	FWHM/nm
BaF₂	0.5	4.022	12	1.212	50	2.865	117
	1.0	5.150	12	1.572	49	3.570	112
	1.5	5.986	12	1.851	48	4.140	102
	2.0	6.041	11	1.835	48	4.181	97
	3.0	6.457	11	1.923	49	4.423	95

表3 Ho:BaF2系列晶体的J-O强度参数Ωt (t=2, 4, 6)和实验与理论振子强度的均方差值(RMSΔS)

Table 3 J-O intensity parameters Ωt (t=2, 4, 6) and root mean square deviation (RMSΔS) for experimental and theoretical oscillator strengths in Ho:BaF2 crystals

Concentration/% (in atom)	Ω₂/(×10^-20, cm²)	Ω₄/(×10^-20, cm²)	Ω₆/(×10^-20, cm²)	Ω₄/Ω₆	RMSΔS/(×10^-21, cm²)
0.5	0.482	1.792	0.904	1.983	0.469
1.0	0.459	2.178	1.088	2.001	0.476
1.5	0.533	2.493	1.251	1.993	0.457
2.0	0.506	2.554	1.303	1.961	0.430
3.0	0.559	2.697	1.391	1.938	0.427

表4 Ho:BaF2晶体的红外波段各发射跃迁的半高峰宽(FWHM)、荧光分支比(β)、能级辐射寿命(τrad)、发射截面(σem)、荧光寿命(τ)和光谱品质因子(Q)

Table 4 Infrared emission transition parameters of Ho:BaF2 crystals, including full width at half maximum (FWHM), fluorescence branching ratio (β), radiative lifetime of energy levels (τrad), emission cross section (σem), fluorescence lifetime (τ), and spectroscopic quality factor (Q)

Transition	Concentration/% (in atom)	FWHM/nm	β/%	τ_rad/ms	σ_em/(×10^-21, cm²)	τ/ms	Q/(×10^-21, cm²·ms)
~1.2 μm (⁵I₆→⁵I₈)	0.5	23.00	80.43	12.01	2.47	8.71	21.51
	1.0	22.90	81.95	10.16	3.01	8.05	24.23
	1.5	31.63	82.94	8.95	2.83	7.49	21.20
	2.0	24.69	83.21	8.64	3.36	7.23	24.29
	3.0	26.03	83.64	8.14	3.64	6.39	23.26
~2.05 μm (⁵I₇→⁵I₈)	0.5	151.26	-	22.83	2.69	15.49	41.67
	1.0	147.85	-	20.21	3.11	16.27	50.60
	1.5	144.99	-	18.36	3.49	17.22	60.10
	2.0	144.45	-	17.88	3.60	18.76	67.53
	3.0	144.23	-	17.07	3.81	15.68	59.74
~2.85 μm (⁵I₆→⁵I₇)	0.5	116.70	19.57	12.01	4.77	8.71	41.55
	1.0	115.09	18.05	10.16	5.53	8.05	44.52
	1.5	114.01	17.06	8.95	5.81	7.49	43.52
	2.0	115.53	16.79	8.64	5.61	7.23	40.56
	3.0	115.04	16.36	8.14	6.09	6.39	38.91

图5 Ho:BaF2晶体各红外波段的荧光光谱和各能级荧光寿命

Fig. 5 Fluorescence spectra in the infrared region and fluorescence lifetimes of the Ho:BaF2 crystals (a) 5I6→5I8 emission transition; (b) 5I7→5I8 emission transition; (c) 5I6→5I7 emission transition; (d) Lifetime of the 5I7 level; (e) Lifetime of the 5I6 level. Colorful figures are available on website

表5 Ho:BaF2晶体与其他基质晶体在红外波段的光谱性能比较

Table 5 Comparative analysis of infrared spectral characteristics in Ho:BaF2 versus alternative gain medium

Waveband	Gain medium	τ/ms	Q/(×10^-21, cm²·ms)	Ref.
~1.2 μm	2.0% Ho:BaF₂	7.23	24.29	This work
	YSGG	0.643	6.43	[44]
	Nano glass	7.8	21.06	[45]
	BaF₂ Nano crystals	2.87	17.22	[46]
~2.05 μm	2.0% Ho:BaF₂	17.76	67.53	This work
	YAG	7.8	62.4	[47]
	CaF₂	11.52	46.81	[41]
	CNGG	6.41	40.38	[48]
	GdScO₃	6.13	30.04	[49]
~2.85 μm	1.0% Ho:BaF₂	8.05	44.52	This work
	LuAG	0.13	20.15	[50]
	LLF	1.83	30.61	[51]
	PbF₂	5.40	77.76	[52]

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Ho:BaF₂晶体在近红外-中红外波段光谱性能分析

Spectroscopic Analysis of Ho:BaF₂ Crystals in the NIR to MIR Spectral Region

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