Effect of substitution of S for Se on structure and physical properties in Ge11.5As24Se64.5–xSx glass

Xu Si-Wei; Yang Xiao-Ning; Yang Da-Xin; Wang Xun-Si; Shen Xiang

doi:10.7498/aps.70.20210536

Abstract

In this paper, chalcogenide glasses Ge_11.5As₂₄Se_64.5–xS_x (x = 0, 16.125%, 32.25%, 48.375% and 64.5%) are prepared and their optical properties are studied in order to select the best components for the use in optical devices. The values of laser damage threshold, refractive index, and third-order nonlinear refractive index, as well as the absorption spectra of the glasses are measured. The results show that the linear and third-order nonlinear refractive indices of the glass decrease gradually, the glass optical band gap increases gradually, and the laser damage threshold increases continuously after the high threshold component S atoms have been introduced gradually. We further investigate the structural origins of these changes in physical properties by Raman scattering spectra and high resolution X-ray photoelectron spectroscopy. By analyzing the evolution process of different structural units in the glass, it is found that the heteropolar bonds (Ge—Se/S, As—Se/S) are dominant in these glass network structures, and compared with Se, and that Ge and As prefer to bond with S. As the ratio of S/Se increases, the number of chemical bonds related to Se (Ge—Se, As—Se and Se—Se) decreases gradually, while the number of chemical bonds related to Se (Ge—S, As—S and S—S) increases gradually, which has little effect on the change of the topological structure of glass. It can be concluded that the main reason for the change of physical properties of glass is the difference of the strength between chemical bonds in the glass structural system.

Keywords:

Authors and contacts

1.
College of Mathematics and Physics, Hunan University of Arts and Science, Changde 415000, China
2.
Key Laboratory of Photoelectric Materials and Devices of Zhejiang Province, The Research Institute of Advanced Technologies, Ningbo University, Ningbo 315211, China

Corresponding author: Xu Si-Wei, xusiwei1227@163.com

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 62004067, 11847159), the Natural Science Foundation of Hunan Province, China (Grant No. 2019JJ50410), and the Research Foundation of Education Bureau of Hunan Province, China (Grant No. 18C0744)

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References

[1]	Wang R P 2014 Amorphous Chalcogenides: Advances and Applications (Singapore: Pan Stanford Publisher) pp97−118
[2]	Tanaka K, Shimakawa K 2011 Amorphous Chalcogenide Semiconductors and Related Materials (New York: Springer International Publishing) pp118−122
[3]	Niu L, Chen Y M, Shen X, Xu T F 2020 Chin. Phys. B 29 087803 Google Scholar
[4]	许思维, 王丽, 沈祥 2015 物理学报 64 223302 Google Scholar Xu S W, Wang L, Shen X 2015 Acta Phys. Sin. 64 223302 Google Scholar
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[13]	Choi D Y, Madden S, Rode A, Wang R P, Luther-Davies B 2007 Appl. Phys. Lett. 91 011115 Google Scholar
[14]	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
[15]	Wang T, Gulbiten O, Wang R P, Yang Z Y, Smith A, Luther-Davies B, Lucas P 2014 J. Phys. Chem. B 118 1436 Google Scholar
[16]	Wang R P, Yan K L, Yang Z Y, Luther-Davies B 2015 J. Non-Cryst. Solids 427 16 Google Scholar
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[18]	Wang R P, Smith A, Luther-Davies B, Kokkonen H, Jackson I 2009 J. Appl. Phys. 105 056109 Google Scholar
[19]	Cernosek Z, Cernoskova E, Todorov R, Holubova J 2020 J. Solid State Chem. 291 121599 Google Scholar
[20]	Wang R P, Smith A, Prasad A, Choi D Y, Luther-Davies B 2009 J. Appl. Phys. 106 043520 Google Scholar
[21]	Yang G, Bureau B, Rouxel T, Gueguen Y, Gulbiten O, Roiland C, Soignard E, Yarger J L, Troles J, Sangleboeuf J C, Lucas P 2010 Phys. Rev. B 82 195206 Google Scholar
[22]	徐航, 彭雪峰, 戴世勋, 徐栋, 张培晴, 许银生, 李杏, 聂秋华 2016 物理学报 65 154207 Google Scholar Xu H, Peng X F, Dai S X, Xu D, Zhang P Q, Xu Y S, Li X, Nie Q H 2016 Acta Phys. Sin. 65 154207 Google Scholar
[23]	Jackson K, Briley A, Grossman S, Porezag D V, Pederson M R 1999 Phys. Rev. B 60 14985 Google Scholar
[24]	Mei Q, Saienga J, Schrooten J, Meyer B, Martin S W 2003 J. Non-Cryst. Solids 324 264 Google Scholar
[25]	Zhang Y, Xu Y S, You C Y, Xu D, Tang J Z, Zhang P Q, Dai S X 2017 Opt. Express 25 8886 Google Scholar
[26]	Frumarova B, Nemec P, Frumar M, Oswald J, Vlcek M 1999 J. Non-Cryst. Solids 256-257 266 Google Scholar
[27]	Kotsalas I P, Papadimitriou D, Raptis C, Vlcek M, Frumar M 1998 Journal of Non-Cryst. Solids 226 85
[28]	Rana A, Singh B P, Sharma R 2019 J. Non-Cryst. Solids 523 119597 Google Scholar
[29]	Musgraves J D, Wachtel P, Gleason B, Richardson K 2014 J. Non-Cryst. Solids 386 61 Google Scholar
[30]	Nefedov V I 1988 X-Ray Photoelectron Spectroscopy of Solid Surfaces (Boca Raton: CRC Press) pp97−128
[31]	Wang R P, Choi D Y, Rode A V, Madden S J, Luther-Davies B 2007 J. Appl. Phys. 101 113517 Google Scholar
[32]	Xu S W, Wang R P, Luther-Davies B, Kovalskiy A, Miller A C, Jain H 2014 J. Appl. Phys. 115 083518 Google Scholar
[33]	Luo Y R 2007 Comprehensive Handbook of Chemical Bond Energies (Boca Raton: CRC Press) pp431−488
[34]	Kovalskiy A, Jain H, Miller A C, Golovchak R Y, Shpotyuk O I 2006 J. Phys. Chem. B 110 22930 Google Scholar
[35]	Opletal G, Drumm D W, Wang R P, Russo S P 2014 J. Phys. Chem. A 118 4790 Google Scholar
[36]	Li Q L, Wang R P, Xu F, Wang X S, Yang Z Y, Gai X 2020 Opt. Mater. Express 10 1413 Google Scholar
[37]	Lu X S, Li J H, Yang L, Zhang R N, Zhang Y D, Ren J, Galca A C, Secu M, Farrell G, Wang P F 2020 J. Non-Cryst. Solids 528 119757 Google Scholar

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图 1 Ge_11.5As₂₄Se_64.5–xS_x玻璃制备的流程图

Figure 1. Flow chart of Ge_11.5As₂₄Se_64.5–xS_x glasses fabrication.

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图 2 Ge_11.5As₂₄Se_64.5–xS_x玻璃的拉曼散射光谱分峰拟合图

Figure 2. Raman scattering spectra of Ge_11.5As₂₄Se_64.5–xS_x glasses and their decompositions.

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图 3 (a) Ge_11.5As₂₄Se_64.5–xS_x 玻璃的S2p 的XPS分解; (b) Ge_11.5As₂₄Se_64.5–xS_x 玻璃的Se3d 的XPS分解

Figure 3. (a) S2p spectra of Ge_11.5As₂₄Se_64.5–xS_x glasses and their decompositions; (b) Se3d spectra of Ge_11.5As₂₄Se_64.5–xS_x glasses and their decompositions.

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图 4 (a) Ge_11.5As₂₄Se_64.5–xS_x 玻璃的Ge3d 的XPS分解; (b) Ge_11.5As₂₄Se_64.5–xS_x 玻璃的As3d 的XPS分解

Figure 4. (a) Ge3d spectra of Ge_11.5As₂₄Se_64.5–xS_x glasses and their decompositions; (b) As3d spectra of Ge_11.5As₂₄Se_64.5–xS_x glasses and their decompositions.

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表 1 Ge_11.5As₂₄Se_64.5–xS_x的组分与光学参数(n, I_th, E_g和n₂)

Table 1. Compositions and optical parameters (n, I_th, E_g and n₂) of Ge_11.5As₂₄Se_64.5–xS_x glasses.

Ge_11.5As₂₄ Se_64.5–xS_x	n	I_th/(W·cm^–2)	E_g/eV	n₂/(10^–14 W·cm^–2)
x = 0	2.639	3.95 × 10⁵	1.859	7.411
x = 16.125	2.546	14.78 × 10⁵	1.898	5.498
x = 32.25	2.451	21.40 × 10⁵	1.979	3.679
x = 48.375	2.378	35.29 × 10⁵	2.069	2.751
x = 64.5	2.261	—	2.347	2.187

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表 2 拉曼散射光谱分峰拟合中各个结构单元的相对比例

Table 2. Relative ratio of the different structural units derived from the decomposed Raman scattering spectra.

	Ge Se_4/2 (CS) /%	Ge Se_4/2 (ES) /%	As Se_3/2/%	Se-Se/%	As-Se/%	As S_3/2/%	Ge S_4/2 (CS)/%	Ge S_4/2 (ES)/%	As-S/%	S-S/%
Ge_11.5As₂₄Se_64.5	14.79	7.52	45.36	9.28	23.05	0	0	0	0	0
Ge_11.5As₂₄Se_48.375S_16.125	10.24	6.97	36.36	6.27	21.57	5.96	2.35	7.63	2.65	0
Ge_11.5As₂₄Se_32.25S_32.25	4.98	4.63	25.65	2.09	19.08	16.26	9.47	11.92	5.61	0.31
Ge_11.5As₂₄Se_16.125S_48.375	0.94	2.20	13.92	0.58	16.84	26.16	11.94	19.16	7.47	0.79
Ge_11.5As₂₄S_64.5	0	0	0	0	0	41.64	14.55	29.21	13.52	1.08

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表 3 Ge_11.5As₂₄Se_64.5–xS_x 玻璃的Ge3d, As3d, Se3d 和S2p 的XPS的拟合参数

Table 3. The fitting parameters for the decomposed Ge3d, As3d, Se3d and S2p spectra of Ge_11.5As₂₄Se_64.5–xS_x glasses.

		Structural unit
		Se-Se- Ge/As	As/Ge-Se-Ge/As	S-S- Ge/As	As/Ge-S-Ge/As	AsSe/S_3/2	As-As- related structure	GeSe/S_4/2	Ge-Ge- related structure
Ge_11.5As₂₄Se_64.5	BE/eV	54.9	54.5	—	—	43.0	—	31.3	—
	FWHM/eV	1.11	1.13			1.03		1.01
	Content/%	18	82			100		100
Ge_11.5As₂₄ Se_48.375S_16.125	BE/eV	55.0	54.6	—	162.1	42.9	—	31.3	—
	FWHM/ eV	1.10	1.18		1.12	1.03		1.10
	Content/%	13	87		100	100		100
Ge_11.5As₂₄ Se_32.25S_32.25	BE/eV	54.9	54.5	162.4	162.1	43.0	—	31.4	—
	FWHM/ eV	1.09	1.11	1.21	1.23	1.15		1.04
	Content/%	11	89	6	94	100		100
Ge_11.5As₂₄ Se_16.125S_48.375	BE/eV	55.0	54.6	162.3	162.0	42.9	—	31.2	—
	FWHM/ eV	1.11	1.14	1.25	1.11	1.11		1.14
	Content/%	8	92	12	88	100		100
Ge_11.5As₂₄S_64.5	BE/eV	—	—	162.3	162.1	42.8	—	31.3	—
	FWHM/ eV			1.21	1.12	1.03		1.09
	Content/%			16	84	100		100

DownLoad: CSV

[1]	Wang R P 2014 Amorphous Chalcogenides: Advances and Applications (Singapore: Pan Stanford Publisher) pp97−118
[2]	Tanaka K, Shimakawa K 2011 Amorphous Chalcogenide Semiconductors and Related Materials (New York: Springer International Publishing) pp118−122
[3]	Niu L, Chen Y M, Shen X, Xu T F 2020 Chin. Phys. B 29 087803 Google Scholar
[4]	许思维, 王丽, 沈祥 2015 物理学报 64 223302 Google Scholar Xu S W, Wang L, Shen X 2015 Acta Phys. Sin. 64 223302 Google Scholar
[5]	Xu S W, Wang R P, Yang Z Y, Wang L, Luther-Davies B 2016 Chin. Phys. B 25 057105 Google Scholar
[6]	乔北京, 陈飞飞, 黄益聪, 戴世勋, 聂秋华, 徐铁峰 2015 物理学报 64 154216 Google Scholar Qiao B J, Chen F F, Huang Y C, Dai S X, Nie Q H, Xu T F 2015 Acta Phys. Sin. 64 154216 Google Scholar
[7]	Eggleton B J, Luther-Davies B, Richardson K 2011 Nat. Photonics 5 141 Google Scholar
[8]	Ren J, Lu X S, Lin C G, Jain R K 2020 Opt. Express 28 21522 Google Scholar
[9]	Wang R P, Bulla D, Smith A, Wang T, Luther-Davies B 2011 J. Appl. Phys. 109 023517 Google Scholar
[10]	Lin H T, Song Y, Huang Y Z, Kita D, Deckoff-Jones S, Wang K Q, Li L, Li J Y, Zheng H Y, Luo Z Q, Wang H Z, Novak S, Yadav A, Huang C C, Shiue R J, Englund D, Gu T, Hewak D, Richardson K, Kong J, Hu J J 2017 Nat. Photonics 11 798 Google Scholar
[11]	Wang L L, Zeng J H, Zhu L, Yang D D, Zhang Q, Zhang P Q, Wang X S, Dai S X 2018 Appl. Opt. 57 10044 Google Scholar
[12]	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
[13]	Choi D Y, Madden S, Rode A, Wang R P, Luther-Davies B 2007 Appl. Phys. Lett. 91 011115 Google Scholar
[14]	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
[15]	Wang T, Gulbiten O, Wang R P, Yang Z Y, Smith A, Luther-Davies B, Lucas P 2014 J. Phys. Chem. B 118 1436 Google Scholar
[16]	Wang R P, Yan K L, Yang Z Y, Luther-Davies B 2015 J. Non-Cryst. Solids 427 16 Google Scholar
[17]	Kotsalas I P, Papadimitriou D, Raptis C, Vlcek M, Frumar M 1998 J. Non-Cryst. Solids 226 85 Google Scholar
[18]	Wang R P, Smith A, Luther-Davies B, Kokkonen H, Jackson I 2009 J. Appl. Phys. 105 056109 Google Scholar
[19]	Cernosek Z, Cernoskova E, Todorov R, Holubova J 2020 J. Solid State Chem. 291 121599 Google Scholar
[20]	Wang R P, Smith A, Prasad A, Choi D Y, Luther-Davies B 2009 J. Appl. Phys. 106 043520 Google Scholar
[21]	Yang G, Bureau B, Rouxel T, Gueguen Y, Gulbiten O, Roiland C, Soignard E, Yarger J L, Troles J, Sangleboeuf J C, Lucas P 2010 Phys. Rev. B 82 195206 Google Scholar
[22]	徐航, 彭雪峰, 戴世勋, 徐栋, 张培晴, 许银生, 李杏, 聂秋华 2016 物理学报 65 154207 Google Scholar Xu H, Peng X F, Dai S X, Xu D, Zhang P Q, Xu Y S, Li X, Nie Q H 2016 Acta Phys. Sin. 65 154207 Google Scholar
[23]	Jackson K, Briley A, Grossman S, Porezag D V, Pederson M R 1999 Phys. Rev. B 60 14985 Google Scholar
[24]	Mei Q, Saienga J, Schrooten J, Meyer B, Martin S W 2003 J. Non-Cryst. Solids 324 264 Google Scholar
[25]	Zhang Y, Xu Y S, You C Y, Xu D, Tang J Z, Zhang P Q, Dai S X 2017 Opt. Express 25 8886 Google Scholar
[26]	Frumarova B, Nemec P, Frumar M, Oswald J, Vlcek M 1999 J. Non-Cryst. Solids 256-257 266 Google Scholar
[27]	Kotsalas I P, Papadimitriou D, Raptis C, Vlcek M, Frumar M 1998 Journal of Non-Cryst. Solids 226 85
[28]	Rana A, Singh B P, Sharma R 2019 J. Non-Cryst. Solids 523 119597 Google Scholar
[29]	Musgraves J D, Wachtel P, Gleason B, Richardson K 2014 J. Non-Cryst. Solids 386 61 Google Scholar
[30]	Nefedov V I 1988 X-Ray Photoelectron Spectroscopy of Solid Surfaces (Boca Raton: CRC Press) pp97−128
[31]	Wang R P, Choi D Y, Rode A V, Madden S J, Luther-Davies B 2007 J. Appl. Phys. 101 113517 Google Scholar
[32]	Xu S W, Wang R P, Luther-Davies B, Kovalskiy A, Miller A C, Jain H 2014 J. Appl. Phys. 115 083518 Google Scholar
[33]	Luo Y R 2007 Comprehensive Handbook of Chemical Bond Energies (Boca Raton: CRC Press) pp431−488
[34]	Kovalskiy A, Jain H, Miller A C, Golovchak R Y, Shpotyuk O I 2006 J. Phys. Chem. B 110 22930 Google Scholar
[35]	Opletal G, Drumm D W, Wang R P, Russo S P 2014 J. Phys. Chem. A 118 4790 Google Scholar
[36]	Li Q L, Wang R P, Xu F, Wang X S, Yang Z Y, Gai X 2020 Opt. Mater. Express 10 1413 Google Scholar
[37]	Lu X S, Li J H, Yang L, Zhang R N, Zhang Y D, Ren J, Galca A C, Secu M, Farrell G, Wang P F 2020 J. Non-Cryst. Solids 528 119757 Google Scholar

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Effect of substitution of S for Se on structure and physical properties in Ge_11.5As₂₄Se_64.5–xS_x glass

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Corresponding author: Xu Si-Wei, xusiwei1227@163.com

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