结合高分辨率X射线光电子能谱和拉曼散射研究GexGa8S92–x玻璃结构

许思维; 王训四; 沈祥

doi:10.7498/aps.72.20221653

摘要

本文在固定Ga原子含量为8%的情况下, 结合高分辨率X射线光电子能谱和拉曼散射光谱对硫系玻璃Ge_xGa₈S_92–x(x = 24%, 26.67%, 29.6%, 32%和36%)的结构进行了研究. 通过分析玻璃结构中各单元结构的演变情况, 发现玻璃内部网络结构主要为S原子桥接GeS₄和GaS₄四面体结构. 随着Ge含量的逐渐增大, S链状或环状结构单元迅速减少, 并消失于Ge_26.67Ga₈S_65.33玻璃组分中; 而类乙烷结构S₃Ge-GeS₃中的Ge—Ge同极键和S₃Ge/Ga-Ga/GeS₃结构中的M—M (Ge—Ge, Ga—Ga或Ge—Ga)同极键同时出现于Ge_29.6Ga₈S_62.4玻璃中, 并且其结构数量随着Ge含量的增大而逐渐增加. 由此可以判定, 首先, 在硫系玻璃Ge_xGa₈S_92–x结构中Ge和Ga原子均主要以4配位的形式出现, 而S原子则主要以2配位的形式出现. 其次, M—M键的存在导致纳米相分离, 玻璃网络结构的有序化程度降低.

关键词:

Abstract

In this paper, the structures of chalcogenide glasses Ge_xGa₈S_92–x (x = 24%, 26.67%, 29.6%, 32% and 36%) at a fixed Ga atomic content of 8% are studied by high-resolution X-ray photoelectron spectroscopy and Raman scattering spectra. In order to quantify the evolutions of the different structural units in Ge_xGa₈S_92–x glasses, the number of double peaks in the Ge 3d, Ga 3d and S 2p spectra are determined by iterative fitting method, the binding energy and the full width at half maximum of each peak, and the relative ratio of the integral area of each decomposed peak to that of the whole area of the X-ray photoelectron spectroscopy are thus achieved. On the other hand, the Raman scattering spectra of Ge_xGa₈S_92–x glass are decomposed into multiple Gaussians based on the structural units. We use the iterative method to simulate the position of peak center, full width at half maximum, and height of each Raman peak. By analyzing the evolution of each unit structure in the glasses, it is found that the network structure of glass network is mainly formed by S atom bridging the tetrahedral structure of GeS₄ and GaS₄. The S chains or rings structural units are formed in Ge₂₄Ga₈S₆₈ glass, indicating that S atoms are in excess in the chemical composition of the glass, so there are enough S atoms around Ge and Ga atoms, forming heteropolar Ge—S and Ga—S bonds. With the gradual increase of Ge content, S chains or rings structure units rapidly disappear in Ge_26.67Ga₈S_65.33 glass. The Ge—Ge homopolar bonds in the ethane-like structure S₃Ge—GeS₃ and the M—M (Ge—Ge, Ga—Ga or Ge—Ga) homopolar bonds in the S₃Ge/Ga—Ga/GeS₃ structure simultaneous appear in the Ge_29.6Ga₈S_62.4 glass, and the number of structures increases gradually with the increase of Ge content. This is mainly due to the insufficient number of S atoms in the Ge-Ga-S glass. Once S atoms are lacking, the excess Ge and Ga atoms can only combine with themselves to form the homopolar bond M—M. It can be concluded below. Firstly, Ge and Ga atoms appear mainly in the form of 4-coordination, while S atoms occur mainly in the form of 2-coordination in the chalcogenide glasses of Ge_xGa₈S_92–x. Secondly, the existence of M—M bond leads the nanophase to separate, and the ordering degree of glass network structure to decrease .

Keywords:

作者及机构信息

1.
湖南文理学院数理学院, 常德　415000

2.
宁波大学高等技术研究院, 浙江省光电探测材料及器件重点实验室, 宁波　315211

通信作者: 许思维, xusiwei1227@163.com

基金项目: 国家自然科学基金(批准号: 62004067)和湖南省教育厅青年项目(批准号: 21B0620)资助的课题.

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 No. 62004067), and the Research Foundation of Education Bureau of Hunan Province, China (Grant No. 21B0620).

文章全文 : translate this paragraph

参考文献

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[22]	Golovchak R, Calvez L, Petracovschi E, Bureau B, Savitskii D, Jain H 2013 Mater. Chem. Phys. 138 909 Google Scholar
[23]	Kotsalas I P, Papadimitriou D, Raptis C, Vlcek M, Frumar M 1998 J. Non-Cryst. Solids 226 85 Google Scholar
[24]	Wang K K, Wang W F, Lin C G, Shen X, Dai S X, Chen F F 2022 Ceram. Int. 48 11209 Google Scholar
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[26]	Velmuzhov A P, Sukhanov M V, Tyurina E A, Plekhovich A D, Fadeeva D A, Ketkova L A, Churbanov M F, Shiryaev V S 2021 J. Non-Cryst. Solids 554 120615 Google Scholar
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[28]	Zhang W, Fu J, Shen X, Chen Y, Dai S X, Chen F, Li J, Xu T F 2013 J. Non-Cryst. Solids 377 191 Google Scholar
[29]	Rana A, Singh B P, Sharma R 2019 J. Non-Cryst. Solids 523 119597 Google Scholar
[30]	Niu L, Chen Y M, Shen X, Xu T F 2020 Chin. Phys. B 29 087803 Google Scholar
[31]	Wang X F, Gu S X, Yu J G, Zhao X J, Tao H Z 2004 J. Solid State Commun. 130 459 Google Scholar
[32]	Hannon A C, Aitken B G 1999 J. Non-Cryst. Solids 256–257 73 Google Scholar
[33]	Masselin P, Coq D L, Cuisset A, Bychkov E 2012 Opt. Mater. Express 2 1768 Google Scholar
[34]	Pauling L 1960 The Nature of the Chemical Bond (Ithaca: Cornell University Press) pp113–121
[35]	Xu Q, Yang X Y, Zhang M J, Wang R P 2019 Mater. Res. Express 6 085212 Google Scholar
[36]	Golovchak R, Nazabal V, Bureau B, Oelgoetz J, Kovalskiy A, Jain H 2018 J. Non-Cryst. Solids 499 237 Google Scholar
[37]	Srivastava C P, Van De Vondel D F, Van Der Kelen G P 1977 Inorg. Chim. Acta 23 L29 Google Scholar
[38]	Pethes I, Nazabal V, Chahal R, Bureau B, Kaban I, Belin S, Jovari P 2016 J. Alloys Compd. 673 149 Google Scholar
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施引文献

图 1 Ge_xGa₈S_92–x玻璃的拉曼散射光谱分峰拟合图

Fig. 1. Raman scattering spectra of Ge_xGa₈S_92–x glasses and their decompositions.

下载: 全尺寸图片幻灯片

图 2 Ge_xGa₈S_92-x玻璃的 S 2 p 的XPS分解

Fig. 2. S 2 p spectra of Ge_xGa₈S_92-x glasses and their decompositions.

下载: 全尺寸图片幻灯片

图 3 Ge_xGa₈S_92–x玻璃的Ge 3d 的XPS分解

Fig. 3. Ge 3d spectra of Ge_xGa₈S_92–x glasses and their decompositions.

下载: 全尺寸图片幻灯片

图 4 Ge_xGa₈S_92–x玻璃的Ga 3d 的XPS分解

Fig. 4. Ga 3d spectra of Ge_xGa₈S_92–x glasses and their decompositions.

下载: 全尺寸图片幻灯片

表 1 拉曼散射光谱分峰拟合中各个结构单元的相对比例

Table 1. Relative ratio of the different structural units derived from the decomposed Raman scattering spectra.

	S₃Ge/Ga-Ga/GeS₃ /%	S₃Ge-GeS₃ /%	Ge/GaS₄ (v₂)/%	GeS₄ (CS) /%	GeS₄ (ES) /%	GaS₄ (F₂) /%	S₃Ge-S- GeS₃ /%	S_n chains /%
Ge₂₄Ga₈S₆₈	0	0	9.43	50.76	12.79	15.31	8.89	2.82
Ge_26.67Ga₈S_65.33	0	0	8.27	54.69	12.84	14.73	9.47	0
Ge_29.6Ga₈S_62.4	4.98	8.52	7.48	47.36	12.22	11.21	8.23	0
Ge₃₂Ga₈S₆₀	9.09	11.81	6.04	45.27	10.13	10.61	7.05	0
Ge₃₆Ga₈S₅₆	15.89	13.31	4.62	43.71	8.31	9.01	5.15	0

下载: 导出CSV

表 2 Ge_xGa₈S_92–x玻璃的Ge 3d, Ga 3d 和S 2p 的XPS的拟合参数

Table 2. The fitting parameters for the decomposed Ge 3d, Ga 3d and S 2p spectra of Ge_xGa₈S_92–x glasses.

		Structural unit
		S-S-S	S-S-Ge/Ga	Ge/Ga -S- Ge/Ga	GeS₄	Ge-Ge/Ga-related structure	GaS₄	Ga-Ge/Ga- related structure
Ge₂₄Ga₈S₆₈	BE/eV	163.13	162.26	161.66	30.51	—	19.87	19.56
	FWHM/eV	1.11	1.03	1.13	1.17		0.98	0.98
	Content/%	4.98	19.17	75.85	100		72.25	27.75
Ge_26.67Ga₈S_65.33	BE/eV	—	162.13	161.58	30.44	—	19.86	19.58
	FWHM/eV		1.12	1.08	1.13		1.02	1.18
	Content/%		11.97	88.03	100		61.94	38.06
Ge_29.6Ga₈S_62.4	BE/eV	—	162.25	161.69	30.56	29.61	19.88	19.56
	FWHM/eV		1.17	1.09	1.11	1.11	1.05	1.06
	Content/%		5.54	94.46	85.41	14.59	53.41	46.59
Ge₃₂Ga₈S₆₀	BE/eV	—	—	161.58	30.58	29.81	19.89	19.51
	FWHM/eV			1.09	1.08	0.99	0.89	0.86
	Content/%			100	80.98	19.02	44.05	55.95
Ge₃₆Ga₈S₅₆	BE/eV	—	—	161.66	30.49	29.72	19.83	19.49
	FWHM/eV			1.16	1.07	1.11	0.87	0.89
	Content/%			100	73.26	26.74	39.53	60.47

下载: 导出CSV

[1]	Wang R P 2014 Amorphous Chalcogenides: Advances and Applications (Singapore: Pan Stanford Publisher) pp178–193
[2]	Tanaka K, Shimakawa K 2011 Amorphous Chalcogenide Semiconductors and Related Materials (New York: Springer International Publishing) pp115–135
[3]	许思维, 杨晓宁, 杨大鑫, 王训四, 沈祥 2021 物理学报 70 167101 Google Scholar Xu S W, Yang X N, Yang D X, Wang X S, Shen X 2021 Acta Phys. Sin. 70 167101 Google Scholar
[4]	Choi D Y, Madden S, Rode A, Wang R P, Luther-Davies B 2007 Appl. Phys. Lett. 91 011115 Google Scholar
[5]	Kim Y, Saienga J, Martin S W 2006 J. Phys. Chem. B 110 16318 Google Scholar
[6]	张兴迪, 吴越豪, 杨正胜, 戴世勋, 张培晴, 张巍, 徐铁锋, 张勤远 2016 物理学报 65 144205 Google Scholar Zhang X D, Wu Y H, Yang Z S, Dai S X, Zhang P Q, Zhang W, Xu T F, Zhang Q Y 2016 Acta Phys. Sin. 65 144205 Google Scholar
[7]	汪俊, 冯赞, 吴国林, 汪金晶, 焦凯, 王弦歌, 刘佳, 梁晓林, 徐铁松, 钟明辉, 肖晶, 赵浙明, 刘自军, 刘永兴, 王训四 2020 发光学报 41 1343 Google Scholar Wang J, Feng Z, Wu G L, Wang J J, Jiao K, Wang X G, Liu J, Liang X L, Xu T S, Zhong M H, Xiao J, Zhao Z M, Liu Z J, Liu Y X, Wang X S 2020 Chin. J. Lumin. 41 1343 Google Scholar
[8]	戴世勋, 彭波, 乐放达, 王训四, 沈祥, 徐铁峰, 聂秋华 2010 物理学报 59 3547 Google Scholar Dai S X, Peng B, Le F D, Wang X S, Shen X, Xu T F, Nie Q H 2010 Acta Phys. Sin. 59 3547 Google Scholar
[9]	任晶, 卢小送, 王鹏飞 2019 光子学报 48 1148007 Google Scholar Ren J, Lu X S, Wang P F 2019 Acta Photonica Sin. 48 1148007 Google Scholar
[10]	Yang Z, Wang R P, Chen Y M, Li Q L, Shen X, Xu T F 2020 Opt. Mater. 100 109677 Google Scholar
[11]	Ren J, Wagner T, Bartos M, Frumar M, Oswald J, Kincl M, Frumarova B, Chen G R 2011 J. Appl. Phys. 109 033105 Google Scholar
[12]	Golovchak R, Shpotyuk O, Kozyukhin S, Shpotyuk M, Kovalskiy A, Jain H 2011 J. Non-Cryst. Solids 357 1797 Google Scholar
[13]	Zhu E W, Liu Y X, Sun X, Yin G L, Jiao Q, Dai S X, Lin C G 2019 J. Non-Cryst. Solids 1 100015 Google Scholar
[14]	Bureau B, Troles J, Floch M L, Guenot P, Smektala F, Lucas J 2003 J. Non-Cryst. Solids 319 145 Google Scholar
[15]	Nazabal V, Charpentier F, Adam J L, Nemec P, Lhermite H, Anne M L B, Charrier J, Guin J P, Moréac A 2011 Int. J. Appl. Ceram. Technol. 8 990 Google Scholar
[16]	Pethes I, Chahal R, Nazabal V, Prestipino C, Trapananti A, Michalik S, Jóvári P 2016 J. Phys. Chem. B 120 9204 Google Scholar
[17]	Golovchak R, Kovalskiy A, Miller A C, Jain H, Shpotyuk O 2007 Phys. Rev. B 76 125208 Google Scholar
[18]	Golovchak R, Shpotyuk O, Kozyukhin S, Kovalskiy A, Miller A C, Jain H 2009 J. Appl. Phys. 105 103704 Google Scholar
[19]	Kondrat O, Holomb R, Csik A, Takats V, Veres M, Mitsa V 2017 Nanoscale Res. Lett. 12 149 Google Scholar
[20]	Xu S W, Wang R P, Luther-Davies B, Kovalskiy A, Miller A C, Jain H 2014 J. Appl. Phys. 115 083518 Google Scholar
[21]	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
[22]	Golovchak R, Calvez L, Petracovschi E, Bureau B, Savitskii D, Jain H 2013 Mater. Chem. Phys. 138 909 Google Scholar
[23]	Kotsalas I P, Papadimitriou D, Raptis C, Vlcek M, Frumar M 1998 J. Non-Cryst. Solids 226 85 Google Scholar
[24]	Wang K K, Wang W F, Lin C G, Shen X, Dai S X, Chen F F 2022 Ceram. Int. 48 11209 Google Scholar
[25]	Li Z B, Lin C G, Nie Q H, Dai S X 2013 J. Am. Ceram. Soc. 96 125 Google Scholar
[26]	Velmuzhov A P, Sukhanov M V, Tyurina E A, Plekhovich A D, Fadeeva D A, Ketkova L A, Churbanov M F, Shiryaev V S 2021 J. Non-Cryst. Solids 554 120615 Google Scholar
[27]	Li Z B, Lin C G, Nie Q H, Dai S X 2013 Appl. Phys. A 112 939 Google Scholar
[28]	Zhang W, Fu J, Shen X, Chen Y, Dai S X, Chen F, Li J, Xu T F 2013 J. Non-Cryst. Solids 377 191 Google Scholar
[29]	Rana A, Singh B P, Sharma R 2019 J. Non-Cryst. Solids 523 119597 Google Scholar
[30]	Niu L, Chen Y M, Shen X, Xu T F 2020 Chin. Phys. B 29 087803 Google Scholar
[31]	Wang X F, Gu S X, Yu J G, Zhao X J, Tao H Z 2004 J. Solid State Commun. 130 459 Google Scholar
[32]	Hannon A C, Aitken B G 1999 J. Non-Cryst. Solids 256–257 73 Google Scholar
[33]	Masselin P, Coq D L, Cuisset A, Bychkov E 2012 Opt. Mater. Express 2 1768 Google Scholar
[34]	Pauling L 1960 The Nature of the Chemical Bond (Ithaca: Cornell University Press) pp113–121
[35]	Xu Q, Yang X Y, Zhang M J, Wang R P 2019 Mater. Res. Express 6 085212 Google Scholar
[36]	Golovchak R, Nazabal V, Bureau B, Oelgoetz J, Kovalskiy A, Jain H 2018 J. Non-Cryst. Solids 499 237 Google Scholar
[37]	Srivastava C P, Van De Vondel D F, Van Der Kelen G P 1977 Inorg. Chim. Acta 23 L29 Google Scholar
[38]	Pethes I, Nazabal V, Chahal R, Bureau B, Kaban I, Belin S, Jovari P 2016 J. Alloys Compd. 673 149 Google Scholar
[39]	Sun Y H, Zhang Z, Yang Z, Niu L, Wu J, Wei T X, Yan K L, Sheng Y, Wang X S, Wang R P 2021 Opt. Mater. Express 11 2413 Google Scholar

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结合高分辨率X射线光电子能谱和拉曼散射研究Ge_xGa₈S_92–x玻璃结构

Structure of Ge_xGa₈S_92–x glasses studied by high-resolution X-ray photoelectron spectroscopy and Raman scattering

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Abstract

作者及机构信息

1.
湖南文理学院数理学院, 常德　415000

2.
宁波大学高等技术研究院, 浙江省光电探测材料及器件重点实验室, 宁波　315211

通信作者: 许思维, xusiwei1227@163.com

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

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