Preparation and properties of Ga2S3-Sb2S3-Ag2S chalcogenide glasses and fibers

Mi Hao-Ting; Yang An-Ping; Huang Zi-Xuan; Tian Kang-Zhen; Li Yue-Bing; Ma Cheng; Liu Zi-Jun; Shen Xiang; Yang Zhi-Yong

doi:10.7498/aps.72.20221380

Abstract

With the rapid development of infrared technology and the wide applications of infrared optical components, the demand for infrared optical materials has risen significantly. Chalcogenide glass has been considered as one of the most popular infrared optical materials because of its wide infrared transmission range, high refractive index, low phonon energy, good rheological properties, low cost, etc. In this work, a new type of Ga₂S₃-Sb₂S₃-Ag₂S chalcogenide glass system is reported, and its glass forming domain is determined. The thermal stability and optical property, mid-infrared (MIR) emission of rare earth dopant, and fiber-forming property for the glasses are studied. The potential applications of the glasses in the MIR region are also evaluated. The experimental results show that the Ga₂S₃-Sb₂S₃-Ag₂S system has a glass forming domain of ~10%–30% Ga₂S₃, ~60%–80% Sb₂S₃ and ~0–15% Ag₂S (all in molar percentage). These glasses have a wide infrared transmission range of ~0.8–13.5 μm, relatively high linear refractive indices of~2.564–2.713 (at 10 μm), and relatviely large third-order nonlinear refractive indices of ~9.7×10^–14–15.7×10^–14 cm²/W (at 1.55 μm). These excellent properties make the Ga₂S₃-Sb₂S₃-Ag₂S glass promising material in the fields of infrared thermal imaging and nonlinear optics. Under the excitation of 1.32 µm laser, the rare earth dopant Dy³⁺ shows strong 2.91 μm and 4.41 μm MIR emissions in the glass. According to the J-O theory, the three strength parameters (Ω₂, Ω₄, Ω₆) of Dy³⁺ in 0.05% weight of Dy³⁺ doped 20Ga₂S₃-75Sb₂S₃-5Ag₂S glass are 7.38×10^–20 cm², 2.24×10^–20 cm² and 0.75×10^–20 cm², respectively. The quantum efficiencies of the 2.91 μm and 4.41 μm emissions are calculated to be 76.6% and 70.8%, respectively, while the stimulated emission cross sections of those two bands are 1.27×10^–20 cm² and 1.43×10^–20 cm², respectively. The fiber based on 20Ga₂S₃-75Sb₂S₃-5Ag₂S: 0.05% Dy³⁺ core glass and 20Ga₂S₃-70Sb₂S₃-10Ag₂S cladding glass is fabricated by rod tube method. The fiber has good transmission performance in the 2–8 μm wavelength range, and the minimum loss is ~3.5 dB/m at 5.7 μm. The Dy³⁺ ions show intense 2.93 μm and 4.45 μm MIR emissions in the fibers under 1.32 μm excitation. These results indicate that the Dy³⁺ doped Ga₂S₃-Sb₂S₃-Ag₂S glass fiber can be a promising candidate for MIR fiber laser medium.

Keywords:

Authors and contacts

1.
Jiangsu Key Laboratory of Advanced Laser Materials and Devices, School of Physics and Electronic Engineering, Jiangsu Normal University, Xuzhou 221116, China
2.
Hangzhou Institute of Optics and Fine Mechanics, Hangzhou 311421, China
3.
Laboratory of Infrared Materials and Devices, Advanced Technology Research Institute, Ningbo University, Ningbo 315211, China

Corresponding author: Yang An-Ping, apyang@jsnu.edu.cn ; Yang Zhi-Yong, yangzhiyong@jsnu.edu.cn

Funds: Project supported by the Joint Funds of the National Natural Science Foundation of China (Grant No. U21A2056) and Key Research and Development Program of Zhejiang Province, China (Grant No. 2021C01025)

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References

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[33]	Yang Z Y, Luo L, Chen W 2006 J. Am. Ceram. Soc. 89 2327
[34]	崔茂林 1987 玻璃工艺学(北京: 中国轻工业出版社) 第140—153页 Cui M L 1987 Glass Technology (Beijing: Light Industry Press) pp140–153 (in Chinese)
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[38]	Gai X, Choi D-Y, Madden S, Yang Z Y, Wang R P, Luther-Davies B 2012 Opt. Lett. 37 3870 Google Scholar
[39]	Choia Y G, Song J H 2009 J. Non-Cryst. Solids 355 48
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[42]	Chen D Q, Wang Y S, Yu Y L, Ma E, Hu Z J 2005 J. Phys. Condens. Matter 17 6545 Google Scholar
[43]	Yang A P, Sun M Y, Ren H, Lin H X, Feng X, Yang Z Y 2021 J. Lumin. 237 118169 Google Scholar
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Cited By

图 1 Ga₂S₃-Sb₂S₃-Ag₂S体系的玻璃形成区

Figure 1. Glass forming region of Ga₂S₃-Sb₂S₃-Ag₂S system.

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图 2 厚度为2 mm xGa₂S₃-ySb₂S₃-zAg₂S 玻璃的透射光谱

Figure 2. Transmission spectra of xGa₂S₃-ySb₂S₃-zAg₂S glasses with the thickness of 2 mm.

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图 3 (a) Dy³⁺掺杂20Ga₂S₃-75Sb₂S₃-5Ag₂S玻璃的吸收光谱, 插图是玻璃在940 nm红外相机下的照片; (b) 1.32 μm激光抽运时, Dy³⁺掺杂20Ga₂S₃-75Sb₂S₃-5Ag₂S玻璃的2—5 μm发射光谱

Figure 3. (a) Absorption spectra of Dy³⁺-doped 20Ga₂S₃-75Sb₂S₃-5Ag₂S glasses, the inset shows photos of the glasses under a 940 nm infrared camera; (b) 2–5 μm emission spectra of Dy³⁺-doped 20Ga₂S₃-75Sb₂S₃-5Ag₂S glasses under 1.32 μm laser excitation

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图 4 20Ga₂S₃-75Sb₂S₃-5Ag₂S:0.05%Dy³⁺/20Ga₂S₃-70Sb₂S₃-10Ag₂S光纤的传输损耗谱, 插图是光纤在940 nm红外相机下的照片

Figure 4. Attenuation of 20Ga₂S₃-75Sb₂S₃-5Ag₂S:0.05%Dy³⁺/20Ga₂S₃-70Sb₂S₃-10Ag₂S fiber, the inset is a photo of the fiber under a 940 nm infrared camera.

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图 5 20Ga₂S₃-75Sb₂S₃-5Ag₂S:0.05%Dy³⁺/20Ga₂S₃-70Sb₂S₃-10Ag₂S光纤在1.32 μm激发时的中红外发射光谱

Figure 5. MIR emission spectrum of 20Ga₂S₃-75Sb₂S₃-5Ag₂S:0.05%Dy³⁺/20Ga₂S₃-70Sb₂S₃-10Ag₂S fiber when excited at 1.32 μm.

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表 1 xGa₂S₃-ySb₂S₃-zAg₂S玻璃的特征温度

Table 1. Characteristic temperatures of xGa₂S₃-ySb₂S₃-zAg₂S glasses.

	x-y-z	T_g (±1℃)	T_x (±1℃)	ΔT/℃
Series A	20-80-0	240	357	117
	20-75-5	235	365	130
	20-70-10	232	349	117
	20-65-15	228	336	108
Series B	25-75-0	244	369	125
	20-75-5	235	365	130
	15-75-10	227	342	115
	10-75-15	210	319	109
Series C	10-80-10	216	313	97
	15-75-10	227	342	115
	20-70-10	232	349	117
	30-60-10	246	346	100

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表 2 xGa₂S₃-ySb₂S₃-zAg₂S玻璃的物理参数

Table 2. The physical parameters of xGa₂S₃-ySb₂S₃-zAg₂S glasses.

	x-y-z	d/(g·cm^–3)	V/ (cm³·mol^–1)	λ_S/nm	λ /μm	n₀ (@10 μm)
Series A	20-80-0	4.09	15.60	729	13.71	2.6430
	20-75-5	4.16	15.42	745	13.67	2.6380
	20-70-10	4.23	15.26	751	13.63	2.6261
	20-65-15	4.32	15.03	765	13.54	2.5990
Series B	25-75-0	4.06	15.46	741	13.53	2.6279
	20-75-5	4.16	15.42	745	13.67	2.6380
	15-75-10	4.26	15.32	760	13.80	2.6650
	10-75-15	4.39	15.29	773	13.94	2.6970
Series C	10-80-10	4.30	15.51	785	13.97	2.7130
	15-75-10	4.26	15.32	760	13.80	2.6650
	20-70-10	4.23	15.26	751	13.63	2.6261
	30-60-10	4.15	15.03	750	13.36	2.5641

DownLoad: CSV

表 3 xGa₂S₃-ySb₂S₃-zAg₂S 玻璃在1.55 μm波长的n₀和 n₂

Table 3. n₀ and n₂ of xGa₂S₃-ySb₂S₃-zAg₂S glasses at 1.55 μm.

x-y-z	n₀ (@1.55 μm)	n₂/ (10^–14 cm²·W^–1)
10-80-10	2.7802	15.7
15-75-10	2.7748	14.0
20-80-00	2.7516	12.4
20-75-05	2.7370	11.1
20-70-10	2.7255	10.6
25-75-00	2.6887	9.7

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表 4 Dy³⁺ 在20 Ga₂S₃-75 Sb₂S₃-5 Ag₂S玻璃中的辐射参数, λ, β, τ_rad, τ_mea分别是发射波长、荧光分支比、能级辐射寿命和实测荧光寿命

Table 4. Radiative parameters of Dy³⁺ in 20 Ga₂S₃-75 Sb₂S₃-5 Ag₂S glass, λ, β, τ_rad, τ_mea are emission wavelength, fluorescence branch ratio, radiative lifetime, and measured lifetime, respectively.

Transition	λ/μm	n₀	β/%	τ_rad/ms	τ_mea/ms	η/%	σ_em/(10^–20 cm)
⁶H_11/2→⁶H_13/2	4.41	2.70	20	2.74	1.94	70.8	1.43
⁶H_13/2→⁶H_15/2	2.91	2.71	80	4.95	3.79	76.6	1.27

DownLoad: CSV

[1]	Cai D W, Xie Y, Guo X, Wang P, and Tong L M 2021 Photonics 8 497 Google Scholar
[2]	Karami E, Tavoosi M, Ghasemi A, Loghmanestarki M R 2019 Ceram. Int. 45 7956 Google Scholar
[3]	Zhang L F, Guan F, Zhang L, Jiang Y G 2022 Opt. Mater. Express 12 1683 Google Scholar
[4]	Zhu J Q, Zhu H, Xu H L, Weng Z P, Wu H Z 2018 Infrared Phys. Technol. 92 13 Google Scholar
[5]	Shiryaev V S, Churbanov M F 2017 J. Non-Cryst. Solids 475 1 Google Scholar
[6]	Gui Y M, Guan Y N, Zhang X S, Zhang C Q, Xia K L, He L, Shen X, Liu Z J 2022 Opt. Express 30 21491 Google Scholar
[7]	Liu L T, Chen F Y, Cui J, Xiao X S, Xu Y T, Hou C Q, Cui X X, Guo H T 2021 Ceram. Int. 47 6388 Google Scholar
[8]	Lucas P, Yang Z Y, Fah M K, Luo T, Jiang S B, Boussard-Pledel C, Anne M-L, and Bureau B 2013 Opt. Mater. Express 3 1049 Google Scholar
[9]	Zhang X H, Bureau B, Lucas P, Boussard-Pledel C, Lucas J 2008 Chemistry 14 432 Google Scholar
[10]	田康振, 胡永胜, 任和, 祁思胜, 杨安平, 冯宪, 杨志勇 2021 物理学报 70 047801 Google Scholar Tian K Z, Hu Y S, Ren H, Qi S S, Yang A P, Feng X, Yang Z Y 2021 Acta Phys. Sin. 70 047801 Google Scholar
[11]	Li R, Zhou W J, Zhou C F, Qi Q Y, Li Y W, Yang Y T, Zhang W, Zhang P Q, Dai S X, Xu T F 2022 Ceram. Int. 48 7956
[12]	Yang A P, Zhang M J, Li L, Wang Y W, Zhang B, Yang Z Y, Tang D Y 2016 J. Am. Ceram. S℃. 99 12 Google Scholar
[13]	Huang X Y, Jiao Q, Lin C G, Ma H L, Zhang X H, Zhu E W, Liu X Y, Dai S X, Xu T F 2018 Sci. Rep. 8 1699 Google Scholar
[14]	Qiu J H, Yang A P, Zhang M J, Li L, Zhang B, Yang Z Y, Tang D Y 2017 J. Am. Ceram. Soc. 100 5107 Google Scholar
[15]	Yang A P, Qiu J H, Zhang M J, Ren H, Zhai C C, Qi S S, Zhang B, Tang D Y, Yang Z Y 2017 J. Alloys Compd. 695 1237 Google Scholar
[16]	Sun M Y, Yang A P, Zhang X H, Ma H L, Zhang M J, Tian K Z, Feng X, Yang Z Y 2019 J. Am. Ceram. Soc. 102 6600 Google Scholar
[17]	杨安平, 王雨伟, 张少伟, 李兴隆, 杨志杰, 李耀程, 杨志勇 2019 物理学报 68 017801 Google Scholar Yang A P, Wang Y W, Zhang S W, Li X L, Yang Z J, Li Y C, Yang Z Y 2019 Acta Phys. Sin. 68 017801 Google Scholar
[18]	Yang Y, Yang Z Y, Lucas P, Wang Y W, Yang Z J, Yang A P, Zhang B, Tao H Z 2016 J. Non-Cryst. Solids 440 38 Google Scholar
[19]	Zhang M J, Li L, Li T T, Wang F, Tian K Z, Tao H Z, Feng X, Yang A P, Yang Z Y 2019 Opt. Express 27 29287 Google Scholar
[20]	张鸣杰, 杨安平, 张斌, 任和, 郭威, 杨艳, 翟诚诚, 王雨伟, 杨志勇, 唐定远 2015 中国激光 42 08060001 Zhang M J, Yang A P, Zhang B, Ren H, Guo W, Yang Y, Zhai C C, Wang Y W, Yang Z Y, Tang D Y 2015 Chin. J. Lasers 42 08060001
[21]	Zhang M J, Yang Z Y, Zhao H, Yang A P, Li L, Tao H Z 2017 J. Alloys Compd. 722 166 Google Scholar
[22]	Wang T, Gai X, Wei W H, Wang R P, Yang Z Y, Shen X, Madden S, Luther-Davies B 2014 Opt. Mater. Express 4 1011 Google Scholar
[23]	Boyd R, Masters B 2009 J. Biomed. Opt. 14 029902 Google Scholar
[24]	Yang Z Y, Li B T, He F, Luo L, Chen W 2008 J. Non-Cryst. Solids 354 1198 Google Scholar
[25]	Shiryaev V S, Sukhanov M V, Velmuzhov A P, Karaksina E V, Kotereva T V, Snopatin G E, Denker B I, Galagan B I, Sverchkov S E, Koltashev V V, Plotnichenko V G 2021 J. Non-Cryst. Solids 567 120939 Google Scholar
[26]	Shiryaev V S, Velmuzhov A P, Tang Z Q, Churbanov M F, Seddon A B 2014 Opt. Mater. 37 18 Google Scholar
[27]	郭威, 张斌, 翟诚诚, 祁思胜, 余懿, 杨安平, 李雷, 杨志勇, 王荣平, 唐定远, 陶光明, Luther-Davies Barry 2016 无机材料学报 31 180 Google Scholar Guo W, Zhang B, Zhai C C, Qi S S, Yu Y, Yang A P, Li L, Yang Z Y, Wang R P, Tang D Y, Tao G M, Luther-Davies B 2016 J. Inorg. Mater. 31 180 Google Scholar
[28]	Tichy L, Ticha H 1995 J. Non-Cryst. Solids 189 141 Google Scholar
[29]	Luo Y R 2007 Comprehensive Handbook of Chemical Bond Energies (Boca Raton: CRC Press) p1687
[30]	Dean J A 1998 Lange's handbook of chemistry (New York: McGraw-Hill Professional) p1561
[31]	Fraenkl M, Frumarova B, Podzemna V, Slang S, Benes L, Vlcek M, Wagner T 2018 J. Non-Cryst. Solids 499 412 Google Scholar
[32]	Ma B C, Jiao Q, Zhang Y T, Sun X, Yin G L, Zhang X H, Ma H L, Liu X Y, Dai S X 2020 Ceram. Int. 46 6544 Google Scholar
[33]	Yang Z Y, Luo L, Chen W 2006 J. Am. Ceram. Soc. 89 2327
[34]	崔茂林 1987 玻璃工艺学(北京: 中国轻工业出版社) 第140—153页 Cui M L 1987 Glass Technology (Beijing: Light Industry Press) pp140–153 (in Chinese)
[35]	Dimitrov V, Komatsu T 2010 J. Univ. Chem. Technol. Metall. 45 219
[36]	Nakamoto K 2009 Infrared and Raman Spectra of Inorganic and Coordination Compounds (New York: John Wiley) pp419– 427
[37]	Gleason B, Richardson K, Sisken L, Smith C 2016 Int. J. Appl. Glass Sci. 7 374 Google Scholar
[38]	Gai X, Choi D-Y, Madden S, Yang Z Y, Wang R P, Luther-Davies B 2012 Opt. Lett. 37 3870 Google Scholar
[39]	Choia Y G, Song J H 2009 J. Non-Cryst. Solids 355 48
[40]	Judd B 1962 Phys. Rev. 127 750 Google Scholar
[41]	Ofelt G 1962 J. Chem. Phys. 37 511 Google Scholar
[42]	Chen D Q, Wang Y S, Yu Y L, Ma E, Hu Z J 2005 J. Phys. Condens. Matter 17 6545 Google Scholar
[43]	Yang A P, Sun M Y, Ren H, Lin H X, Feng X, Yang Z Y 2021 J. Lumin. 237 118169 Google Scholar
[44]	Zhang M J, Yang A P, Peng Y F, Zhang B, Ren H, Guo W, Yang Y, Zhai C C, Wang Y W, Yang Z Y, Tang D Y 2015 Mater. Res. Bull. 70 55 Google Scholar
[45]	Schweizer T, Hewak D W, Samson B N, Payne D N 1996 Opt. Lett. 21 1594 Google Scholar

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Vol. 72, Issue 4 - 2023-02-20

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Preparation and properties of Ga₂S₃-Sb₂S₃-Ag₂S chalcogenide glasses and fibers

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Corresponding author: Yang An-Ping, apyang@jsnu.edu.cn ; Yang Zhi-Yong, yangzhiyong@jsnu.edu.cn

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