Optical properties and microstructure of two Ge-Sb-Se thin films

Pan Lei; Song Bao-An; Xiao Chuan-Fu; Zhang Pei-Qing; Lin Chang-Gui; Dai Shi-Xun

doi:10.7498/aps.69.20200145

Abstract

Multipoint Cauchy method (MCM) is presented to investigate the refractive index and dispersion for each of Ge₂₀Sb₁₅Se₆₅ and Ge₂₈Sb₁₂Se₆₀ chalcogenide thin films at any wavelength in the transmission spectrum based on the regional approach method and Cauchy fitting. We theoretically calculate and compare the refractive index and dispersion curves obtained by using six different models. The results show that the most accurate results are obtained by the MCM. Two Ge—Sb—Se films are prepared by magnetron sputtering experimentally, and transmission spectrum curves are measured by Fourier infrared spectrometer, the noise is removed by segmental filtering and then the refractive index, dispersion, absorption coefficient, and optical band gap of the two films ina range of 500–2500 nm are obtained by the MCM. The results show that the refractive index of Ge₂₈Sb₁₂Se₆₀ film is larger than that of Ge₂₀Sb₁₅Se₆₅ film, which is caused by the higher polarizability and density of the former. The refractive indexes of both films decrease with wavelength increasing, so the long waves travel faster than short waves in the two films. The optical band gap of Ge₂₈Sb₁₂Se₆₀ film (1.675 eV) is smaller than that of Ge₂₀Sb₁₅Se₆₅ film (1.729 eV), and the corresponding wavelengths of the two are 740.3 nm and 717.2 nm. Finally, the microstructures of the two films are characterized by Raman spectra, and the reasons why the two chalcogenide films have different optical properties are explained from the bonding properties between the atoms.

Keywords:

Authors and contacts

1.
Faculty of Electrical Engineering and Computer Science, Ningbo University, Ningbo 315211, China
2.
Zhejiang Key Laboratory of Photoelectric Detection Materials and Devices, Ningbo University, Ningbo 315211, China
3.
Advanced Technology Research Institute, Ningbo University, Ningbo 315211, China

Corresponding author: Song Bao-An, songbaoan@nbu.edu.cn

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References

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[2]	Yamada N, Ohno E, Akahira N 1987 Jpn. J. Appl. Phys. 26 61
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[4]	Yang Z, Wilhelm A A, Lucas P 2010 J. Am. Ceram. Soc. 93 1941
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[6]	Alias M S, Dursun I, Saidaminov M I 2016 Opt. Express 24 16586 Google Scholar
[7]	Rodenhausen K B, Schmidt D, Kasputis T 2012 Opt. Express 20 5419 Google Scholar
[8]	Onodera H, Awai I, Ikenoue J 1983 Appl. Opt. 22 1194 Google Scholar
[9]	Zhang G, Sasaki K 1988 Appl. Opt. 27 1358 Google Scholar
[10]	Wang H 1994 Fiber Integr. Opt. 13 293 Google Scholar
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[17]	Sharma N, Sharda S, Sharma V 2012 Mater. Chem. Phys. 136 967 Google Scholar
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[21]	Jin Y, Song B, Lin C 2017 Opt. Express 25 31273 Google Scholar
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Cited By

图 1 镀在透明二氧化硅玻璃衬底上的薄膜结构示意图

Figure 1. Schematic of the structure of a thin film coated on a transparent silica glass substrate.

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图 2 在有限玻璃基板上的Si-H薄膜的透射率曲线

Figure 2. Transmittance curve of Si-H thin film on finite glass substrate.

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图 3 六种不同模型得到的薄膜折射率和色散比较

Figure 3. Comparison of refractive index and dispersion of thin film obtained by six different models.

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图 4 六种色散模型(包含多点柯西法)得到的折射率和色散与真实值差值随波长变化关系　(a)折射率差与波长的关系; (b)色散差与波长的关系

Figure 4. Relation between the refractive index and the dispersion obtained by six dispersion models (include MCM) and the true value as a function of wavelength: (a) Δn vs. wavelength; (b) ΔD vs. wavelength.

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图 5 五种滤波方法去噪声比较　(a) Adjacent averaging方法; (b) Savitaky-Golay方法; (c) percentile filter方法; (d) FFT filter方法; (e)分段拟合法

Figure 5. Comparison of five filtering methods to reduce noise: (a) Adjacent averaging method; (b) Savitaky-Golay method; (c) percentile filter method; (d) FFT filter method; (e) piecewise fitting method.

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图 6 利用改进的Swanepoel方法获得的具有上下切线包络的透射曲线　(a) Ge₂₀Sb₁₅Se₆₅薄膜; (b) Ge₂₈Sb₁₂Se₆₀薄膜

Figure 6. Transmission curve with upper and lower tangent envelopes obtained by using the improved Swanepoel method: (a) Ge₂₀Sb₁₅Se₆₅ film; (b) Ge₂₈Sb₁₂Se₆₀ film.

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图 7 Ge-Sb-Se薄膜的折射率和色散　(a)折射率与波长的关系; (b) 色散与波长的关系

Figure 7. Refractive index and dispersion of Ge-Sb-Se films: (a) Refractive index vs. wavelength; (b) dispersion vs. wavelength.

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图 8 Ge-Sb-Se薄膜的吸收特性　(a) 吸收系数与波长的关系; (b) 强吸收区域中吸收系数与光子能量乘积的平方根与光子能量之间的关系

Figure 8. Absorption characteristics of Ge-Sb-Se films: (a) Absorption coefficient vs. wavelength; (b) square root of the product of the absorption coefficient and photon energy vs. the photon energy in the strong absorption region.

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图 9 Ge-Sb-Se薄膜的拉曼光谱

Figure 9. Raman spectrum of Ge-Sb-Se film.

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表 1 六种折射率模型

Table 1. Six models of refractive index.

名称	模型
Cauchy	$n = A + \dfrac{B}{{{\lambda ^2}}} + \dfrac{C}{{{\lambda ^4}}}$
二阶归一化标准Sellmeier	$n = \sqrt {1 + \dfrac{{A \cdot {\lambda ^2}}}{{{\lambda ^2} - B}} + \dfrac{{C \cdot {\lambda ^2}}}{{{\lambda ^2} - D}}} $
三阶归一化标准Sellmeier	$n = \sqrt {1 + \dfrac{{A \cdot {\lambda ^2}}}{{{\lambda ^2} - B}} + \dfrac{{C \cdot {\lambda ^2}}}{{{\lambda ^2} - D}} + \dfrac{{E \cdot {\lambda ^2}}}{{{\lambda ^2} - F}}} $
二阶非标准形式的Sellmeier	$n = \sqrt {A + \dfrac{{B \cdot {\lambda ^2}}}{{{\lambda ^2} - C}} + D \cdot {\lambda ^2}} $
Conrady	$n = A + \dfrac{B}{\lambda } + \dfrac{C}{{{\lambda ^{3.5}}}}$
Herzberger	$n = A + B \cdot {\lambda ^2} + C \cdot {\lambda ^2} + \dfrac{D}{{\left( {{\lambda ^2} - 0.028} \right)}} + \dfrac{E}{{{{\left( {{\lambda ^2} - 0.028} \right)}^2}}}$

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表 2 由图2中数据获得的λ, T_M和T_m的值以及通过改进后的Swanepoel方法计算的n和d值

Table 2. Values of λ, T_M, and T_m obtained in Fig. 2 and the values of n and d calculated by the improved Swanepoel method

λ	T_M	T_m	n	d	m₀	m	n₀	d₀
972.4	0.9202	0.5007	2.9173		6.001	6.0	2.9169	1000.0
911.2	0.9199	0.4904	2.9613		6.501	6.5	2.9611	1000.0
859.0	0.9193	0.4801	3.0066	1000.0	7.002	7.0	3.0062	1000.0
814.1	0.9183	0.4697	3.0527	1000.4	7.501	7.5	3.0526	1000.1
774.9	0.9165	0.4591	3.0996	1000.1	8.002	8.0	3.0993	1000.0
740.5	0.9134	0.4485	3.1471	999.5	8.502	8.5	3.1468	1000.0
710.0	0.9080	0.4376	3.1951	999.7	9.002	9.0	3.1947	1000.0
682.8	0.8984	0.4260	3.2435	999.4	9.502	9.5	3.2430	999.9
658.4	0.8818	0.4132	3.2921	1000.2	10.002	10.0	3.2917	1000.0
636.3	0.8530	0.3982	3.3410	999.3	10.503	10.5	3.3402	999.9
616.3	0.8050	0.3796	3.3898	999.6	11.003	11.0	3.3893	999.9
598.1	0.7252	0.3546	3.4335	1020.4	11.483	11.5	3.4387	1001.6
581.3	0.6127	0.3191	3.4878	1000.6	12.002	12.0	3.4874	1000.0
565.9	0.4595	0.2678	3.5368	981.9	12.502	12.5	3.5365	1000.0
551.7	0.2879	0.1965	3.5856	1001.6	13.001	13.0	3.5857	1000.1
注: $ \qquad \quad \overline d = 1000.2;{\sigma _1} = 7.58;\overline {{d_0}} = 1000.1;{\sigma _0} = 0.40$.

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表 A1 六种模型的系数

Table A1. Coefficients of six models.

	A	B	C	D	E	F
Cauchy	2.6006	2.9900 × 10⁵	2.4107 × 10⁸
二阶归一化标准Sellmeier	6.0592	1.3837 × 10⁵	0.5371	1.3837 × 10⁵
三阶归一化标准Sellmeier	11.1212	6.4542 × 10⁴	5.9297	6.4455 × 10⁴	–11.3546	–4.9139 × 10⁴
二阶非标准形式的Sellmeier	–30.1052	36.8509	4.3322 × 10⁴	–0.0079
Conrady	2.3534	502.8603	1.2718 × 10⁹
Herzberger	4.3450	–3.1408 × 10^–8	1.7525 × 10^–12	3.0038 × 10⁵	9.0228 × 10¹⁰

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表 A2 利用六种模型和多点柯西法得到的折射率与真实值的差

Table A2. Difference between refractive index obtained by using six models, MFM, and real value.

λ	Δn_cauchy	Δn_Sel2	Δn_Sel3	Δn_sel2非	Δn_Conrady	Δn_Herzberger	Δn_MCM
580	–0.0002	0.0018	–0.0005	–0.0003	–0.0007	–0.0050	–0.0001
600	–0.0003	–0.0107	–0.0007	–0.0005	–0.0014	0.0081	–0.0002
620	–0.0004	–0.0180	–0.0008	–0.0006	–0.0016	0.0162	–0.0002
640	–0.0004	–0.0216	–0.0007	–0.0006	–0.0015	0.0201	–0.0003
660	–0.0004	–0.0226	–0.0006	–0.0005	–0.0012	0.0207	–0.0003
680	–0.0004	–0.0218	–0.0005	–0.0005	–0.0008	0.0186	–0.0003
700	–0.0004	–0.0197	–0.0003	–0.0004	–0.0003	0.0146	–0.0003
720	–0.0004	–0.0167	–0.0002	–0.0003	0.0001	0.0091	–0.0003
740	–0.0004	–0.0131	–0.0001	–0.0003	0.0005	0.0028	–0.0003
760	–0.0004	–0.0090	0.0000	–0.0002	0.0008	–0.0038	–0.0003
780	–0.0004	–0.0047	0.0000	–0.0002	0.0010	–0.0103	–0.0003
800	–0.0004	–0.0002	0.0000	–0.0002	0.0011	–0.0160	–0.0003
820	–0.0004	0.0043	0.0000	–0.0002	0.0011	–0.0207	–0.0003
840	–0.0003	0.0089	0.0000	–0.0002	0.0009	–0.0238	–0.0003
860	–0.0003	0.0134	–0.0001	–0.0002	0.0007	–0.0249	–0.0003
880	–0.0003	0.0178	–0.0002	–0.0002	0.0004	–0.0236	–0.0003
900	–0.0003	0.0222	–0.0003	–0.0002	–0.0001	–0.0196	–0.0003
920	–0.0002	0.0264	–0.0004	–0.0003	–0.0006	–0.0123	–0.0003
940	–0.0002	0.0305	–0.0006	–0.0004	–0.0012	–0.0014	–0.0003
960	–0.0002	0.0345	–0.0007	–0.0004	–0.0019	0.0134	–0.0003
$\begin{aligned}{\text{注}}:\; & \Delta {n_{{\rm{Cauchy}}}} = 0.0003;\sigma {n_{{\rm{Cauchy}}}} = 0.0002;\Delta {n_{{\rm{Sel2}}}} = 0.0253;\sigma {n_{{\rm{Sel2}}}} = 0.0273;\\ &\Delta {n_{{\rm{Sel3}}}} = 0.0006;\sigma {n_{{\rm{Sel3}}}} = 0.0010;\Delta {n_{{\rm{Sel}}2{\simfont\text{非}}}} = 0.0005;\sigma {n_{{\rm{Sel}}2{\simfont\text{非}}}} = 0.0005;\\ & \Delta {n_{{\rm{Conrady}}}} = 0.0016;\sigma {n_{{\rm{Conrady}}}} = 0.0022;\Delta {n_{{\rm{Herzberger}}}} = 0.0226;\sigma {n_{{\rm{Herzberger}}}} = 0.0225;\\ & \Delta {n_{{\rm{MCM}}}} = 0.0002;\sigma {n_{{\rm{MCM}}}} = 0.0001 .\end{aligned}$

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表 3 多点柯西法获得的两种薄膜多个波长处的折射率

Table 3. Refractive index at multiple wavelengths of two thin films obtained by MCM.

波长/nm	Ge₂₀Sb₁₅Se₆₅薄膜				Ge₂₈Sb₁₂Se₆₀薄膜
波长/nm	T_exp	T_M	m	n	T_exp	T_M	m	n
600	0.2449	0.2682	8.7331	2.6902	0.0009	0.0253	13.3793	2.8670
620	0.3463	0.4036	8.0131	2.6530	0.0417	0.0726	12.7620	2.8259
640	0.4987	0.5496	7.4160	2.6208	0.1107	0.0957	12.2073	2.7902
660	0.4749	0.6845	6.9106	2.5929	0.2449	0.2519	11.7057	2.7592
680	0.7724	0.7891	6.4760	2.5685	0.2914	0.3957	11.2495	2.7320
700	0.6566	0.8552	6.0972	2.5472	0.5222	0.5266	11.0259	2.7081
750	0.9088	0.9096	5.7634	2.5041	0.7469	0.7853	10.1068	2.6597
800	0.6160	0.9219	5.4665	2.4720	0.6155	0.9123	9.3455	2.6233
900	0.6199	0.9321	4.9602	2.4285	0.8667	0.9681	8.1494	2.5735
1000	0.7666	0.9388	4.5433	2.4014	0.7547	0.9735	7.2448	2.5420
1100	0.8085	0.9429	4.1932	2.3835	0.6124	0.9773	6.5316	2.5210
1200	0.7580	0.9455	3.8945	2.3711	0.9678	0.9805	5.9523	2.5062
1300	0.6850	0.9472	3.6364	2.3622	0.6186	0.9813	5.4709	2.4955
1400	0.9418	0.9480	3.4109	2.3556	0.9556	0.9806	5.0638	2.4875
1500	0.7814	0.9482	3.2121	2.3506	0.7282	0.9801	4.7145	2.4813
1600	0.6521	0.9479	3.0356	2.3466	0.6430	0.9800	4.4112	2.4765
1700	0.7244	0.9474	2.8776	2.3435	0.8853	0.9800	4.1452	2.4726
1800	0.8914	0.9470	3.1213	2.3410	0.9383	0.9801	3.9099	2.4694
1900	0.9384	0.9470	2.9544	2.3389	0.7164	0.9801	3.7002	2.4668
2000	0.8249	0.9476	2.8046	2.3372	0.6282	0.9800	3.5121	2.4647
2100	0.7121	0.9491	2.6694	2.3358	0.6868	0.9800	3.2838	2.4628
2200	0.6614	0.9518	2.5468	2.3345	0.8411	0.9801	3.1325	2.4613
2300	0.6679	0.9559	2.4349	2.3335	0.9705	0.9804	2.9947	2.4599
2400	0.7188	0.9617	2.3326	2.3326	0.9441	0.9809	2.8686	2.4588

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表 4 Ge-Sb-Se薄膜拉曼光谱中对应的振动模式

Table 4. Vibration modes in the Raman spectrum of Ge-Sb-Se system.

拉曼峰位/cm^–1	振动模式
160	Se₂Sb-SbSe₂结构中的Sb—Sb同极键的振动
170	Ge₂Se_6/2结构中的Ge—Ge同极键的伸缩振动
197	SbSe_3/2三角锥结构中的Sb—Se键的E₁模式振动
203	共顶角GeSe_4/2四面体中的Ge—Se键的V₁模式振动
215	共边GeSe_4/2四面体中的Ge—Se键振动
235	Se_n环结构中的Se—Se键振动
256	Se_n链结构中的Se—Se键振动
270	Ge-Ge_mSe_4-m结构中的Ge—Ge同极键的振动
303	GeSe₄四面体的F₂型不对称振动

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[1]	Rode A V, Zakery A, Samoc M 2002 Appl. Surf. Sci. 197 481
[2]	Yamada N, Ohno E, Akahira N 1987 Jpn. J. Appl. Phys. 26 61
[3]	Afonso C N, Solis J, Catalina F 1992 Appl. Phys. Lett. 60 3123 Google Scholar
[4]	Yang Z, Wilhelm A A, Lucas P 2010 J. Am. Ceram. Soc. 93 1941
[5]	Hilfiker J N, Singh N, Tiwald T 2008 Thin Solid Films 516 7979 Google Scholar
[6]	Alias M S, Dursun I, Saidaminov M I 2016 Opt. Express 24 16586 Google Scholar
[7]	Rodenhausen K B, Schmidt D, Kasputis T 2012 Opt. Express 20 5419 Google Scholar
[8]	Onodera H, Awai I, Ikenoue J 1983 Appl. Opt. 22 1194 Google Scholar
[9]	Zhang G, Sasaki K 1988 Appl. Opt. 27 1358 Google Scholar
[10]	Wang H 1994 Fiber Integr. Opt. 13 293 Google Scholar
[11]	顾晓明, 贾宏志, 王铿 2009 光学仪器 31 89 Google Scholar Gu X M, Jia H Z, Wang K 2009 Optical Instruments 31 89 Google Scholar
[12]	Aqili A K S, Maqsood A 2002 Appl. Opt. 41 218 Google Scholar
[13]	Chambouleyron I, Martinez J M, Moretti A C 1997 Appl. Opt. 36 8238 Google Scholar
[14]	宗双飞, 沈祥, 徐铁峰, 陈昱, 王国祥, 陈芬, 李军, 林常规, 聂秋华 2013 物理学报 62 096801 Google Scholar Zong S F, Shen X, Xu T F, Chen Y, Wang G X, Chen F, Li J, Lin C G, Nie Q H 2013 Acta Phys. Sin. 62 096801 Google Scholar
[15]	Verma K C, Sharma P, Negi N S 2008 Appl. Phys. B 93 859 Google Scholar
[16]	Song S, Dua J, Arnold C B 2010 Opt. Express 18 5472 Google Scholar
[17]	Sharma N, Sharda S, Sharma V 2012 Mater. Chem. Phys. 136 967 Google Scholar
[18]	Yahia I S, Shapaan M, Ismail Y A M 2015 J. Alloys Compd. 636 317 Google Scholar
[19]	Xiao C, Song B, Jin Y 2019 Opt. Laser Technol. 120 105708 Google Scholar
[20]	Jin Y, Song B, Jia Z 2017 Opt. Express 25 440 Google Scholar
[21]	Jin Y, Song B, Lin C 2017 Opt. Express 25 31273 Google Scholar
[22]	高静, 于峰, 葛廷武 2014 红外与激光工程 43 3368 Google Scholar Gao J, Yu F, Ge Y W 2014 Infrared and Laser Engineering 43 3368 Google Scholar
[23]	Pernick B J 1983 Appl. Opt. 22 1133 Google Scholar
[24]	王申浩, 陶宗明, 杨蕾, 张辉 2017 大学物理实验 30 58 Wang S H, Tao Z M, Yang L, Zhang H 2017 College Physics Experiment 30 58
[25]	Tatian B 1984 Appl. Opt. 23 4477 Google Scholar
[26]	Swanepoel R 1983 J. Phys. E: Sci. Instrum. 16 1214 Google Scholar
[27]	Fu Y Z, Cheng G G, Wang Q 2012 Mater. Sci. Technol. 20 145
[28]	张巍, 陈昱, 付晶, 陈飞飞, 沈祥, 戴世勋, 林常规, 徐铁峰 2012 物理学报 61 056801 Google Scholar Zhang W, Chen Y, Fu J, Chen F F, Shen X, Dai S X, Lin C G, Xu T F 2012 Acta Phys. Sin. 61 056801 Google Scholar
[29]	Afzal M Z, Krämer M, Bukhari S S 2013 International Workshop on Camera-Based Document Analysis and Recognition (Cham: Springer) pp139−149
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Vol. 69, Issue 11 - 2020-06-05

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