Research progress of tin oxide-based thin films and thin-film transistors prepared by sol-gel method

Liu Xian-Zhe; Zhang Xu; Tao Hong; Huang Jian-Lang; Huang Jiang-Xia; Chen Yi-Tao; Yuan Wei-Jian; Yao Ri-Hui; Ning Hong-Long; Peng Jun-Biao

doi:10.7498/aps.69.20200653

Abstract

Transparent conductive oxide (TCO) films and transparent oxide semiconductor (TOS) films have been widely adopted in solar cells, flat panel displays, smart windows, and transparent flexible electronic devices due to their advantages of high transparency and good conductivity and so on. Most of TCO and TOS films are mainly derived from indium oxide, zinc oxide and tin oxide. Among these materials, the In element is toxic, rare and expensive for indium oxide film, which will cause environmental pollution; zinc oxide film is sensitive to acid or alkali etchants, resulting in a poor formation of film patterning; tin oxide film is not only non-toxic, eco-friendly, and cheap but also has good electrical properties and strong chemical stability. Thus, tin oxide has a great potential for developing the TCO and TOS films. At present, the film is prepared mainly by the vacuum deposition technique. The drawbacks of this technique are complex and expensive equipment system, high energy consumption, complicated process and high-cost production. However, compared with the vacuum deposition technique, the sol-gel method has attracted extensive attention because of its virtues such as simple process and low cost. In this paper, we review the development status and trend of TCO and TOS films. First, the structural characteristics, conductive mechanism, element doping theory and carrier scattering mechanism of tin oxide thin films are introduced. Then the principle of sol-gel method and correlative film fabrication techniques are illustrated. Subsequently, the application and development of tin oxide-based thin films prepared by sol-gel method in n-type transparent conductive films, thin-film transistors and p-type semiconductor films in recent years are described. Finally, current problems and future research directions are also pointed out.

Keywords:

Authors and contacts

1.
Institute of Polymer Optoelectronic Materials and Devices, State Key Laboratory of Luminescence Materials and Devices, South China University of Technology, Guangzhou 510641, China
2.
New Vision Opto-Electronic Technology Co., Ltd, Guangzhou 510530, China

Corresponding author: Tao Hong, tao.h@scut.edu.cn ; Ning Hong-Long, ninghl@scut.edu.cn ;

Funds: Project supported by the Major project of Basic and Applied Basic Research in Guangdong Province, China(Grant No. 2019B030302007), the National Natural Science Foundation of China (Grant Nos. 51771074, 61574061), Major Integration Project of the National Natural Science Foundation of China (Grant No.U1601651), Guangzhou Science and Technology Project, China (Grant No. 201904010344), Special Funds for Basic Scientific Research Operating Expenses of Central Universities, China (Grant No. 2019MS012), Special Fund for "Climbing Plan" of Science and Technology Innovation Cultivation for Guangdong University Students in 2019 (Grant Nos. pdjh2019a0028, pdjh2019b0041), National Innovation and Entrepreneurship Training Program for College Students (Grant Nos. 201910561005, 201910561007), and the South China University of Technology BaiBu Ladder Climbing Program Research Project (Grant Nos. j2tw201902475, j2tw201902203).

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References

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Cited By

图 1 氧化锡　(a) 晶体结构; (b) XRD图谱^[22]; (c) 能带结构^[23]; (d) 能带结构示意图^[7]

Figure 1. SnO₂: (a) Crystalline structure; (b) XRD pattern^[22]; (c) band structure^[23]; (d) band structure schematic^[7].

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图 2 氧化锡内部不同本征点缺陷的形成能^[26]

Figure 2. Formation energy of intrinsic point defects in SnO₂^[26].

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图 3 不同半导体的能带图　(a)本征半导体; (b) n型掺杂半导体; (c) p型掺杂半导体

Figure 3. The energy band schematic of semiconductors: (a) intrinsic (b) n type; (c) p type.

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图 4 晶界散射和电离杂质散射机制示意图^[31]

Figure 4. The schematic of grain boundary scattering and ionized impurity scattering mechanism^[31].

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图 5 溶胶-凝胶技术原理^[33]

Figure 5. The overview of the sol-gel technologies^[33].

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图 6 (a) 旋涂法^[35]; (b) 喷雾热解法^[36]; (c) 浸涂法^[37]; (d) 喷墨打印法^[38]

Figure 6. The solution-processed fabrication techniques of thin film: (a) Spin coating^[35]; (b) spray pyrolysis^[36]; (c) dip coating^[37]; (d) inkjet print^[38].

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图 7 在不同SnF₂浓度下　(a) FTO薄膜 (110) 晶面衍射的半峰宽和晶粒尺寸的变化和 (b) FTO薄膜的电阻率、载流子浓度和迁移率的变化^[52]

Figure 7. (a) Variation of full-width-at-half-maximum and grain size estimated along (1 1 0) diffraction and (b) electrical resistivity, carrier concentration and Hall mobility of the FTO films as a function of SnF₂ concentration, 0–10 mol%^[52].

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图 8 不同Sb掺杂浓度下　(a) 方阻和电阻率的变化和 (b) 迁移率和载流子浓度的变化^[56]

Figure 8. The variation of (a) Sheet resistance and resistivity and (b) Hall mobility and carrier concentration for ATO film with different Sb concentrations^[56].

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图 9 在不同掺杂浓度下SnO₂基TCOs薄膜的电学性能变化　(a) Ta^[57]; (b) Nb^[58]; (c) Pr^[59]; (d) W^[60]

Figure 9. The variation of electrical properties for SnO₂-based TCOs films with different dopants concentrations: (a) Ta^[57]; (b) Nb^[58]; (c) Pr^[59]; (d) W^[60].

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图 10 (a) 不同浓度SnO₂薄膜的厚度和电学性能^[63]; (b) SnO₂薄膜的XRD图谱和TFT的转移特性曲线^[64]; (c) Ga掺杂SnO₂的TFT示意图及其转移特性曲线^[65]

Figure 10. (a) The thickness and electrical properties of SnO₂ films with different concentration^[63]; (b) the XRD pattern of SnO₂ film and the transfer characteristic curve of SnO₂ TFT^[64]; (c) the schematic cross-sectional diagram of Ga doped SnO₂ TFT and corresponding transfer characteristic curve^[65].

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图 11 (a) 不同锡前驱体溶液的热重分析曲线^[69]; (b) 不同原子的标准电极电位、带隙和电负性^[70]; (c) 不同氧化物介电材料的高介电常数和能带值^[71]; (d) 在标准条件下, 高介电常数的氧化物吸湿反应的吉布斯能量变化^[71]

Figure 11. (a) Thermogravimetric analyses curves of various Sn precursors^[69]; (b) standard electrode potential, bandgap, and electronegativity of In, Zn, Sn, and carrier suppressible atoms^[70]; (c) permittivity and band gap for different oxide dielectrics^[71]; (d) Gibbs energy changes for moisture absorption reactions in high permittivity oxides under standard conditions^[71].

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图 12 不同掺杂浓度SnO₂基薄膜的透过率图谱　(a) Ga掺杂SnO₂^[75]; (b) Co掺杂SnO₂^[81]; (c) Mn掺杂SnO₂^[80]; (d) 不同掺杂浓度下Mg掺杂SnO₂薄膜的光学吸收图谱^[79]

Figure 12. The transmittance spectra of SnO₂-based films with different dopant concentration: (a) Ga doped SnO₂^[75]; (b) Co doped SnO₂^[81]; (c) Mn doped SnO₂^[80]; (d) the optical absorption spectra of Mg-doped SnO₂ thin films with different concentration^[79].

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图 13 p-n结的电流-电压特性曲线　(a) SnO₂:Ga/ZnO:Al^[75]; (b) SnO₂:Ga/SnO₂:Si^[82]

Figure 13. The current–voltage characteristics curve of p-n heterojunction: (a) SnO₂:Ga/ZnO:Al^[75]; SnO₂:Ga/SnO₂:Si^[82].

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表 1 不同卤素元素的电负性、X—H和X—Sn键解离能和原子半径^[31,50]

Table 1. The electronegativity, BDE of X—H and X— Sn, atomic radius for halogen elements^[31,50].

Element	Electroneg- ativity	BDE of X-H/kJ·mol^–1	Atomic radius/nm	BDE of X-Sn/kJ·mol^–1
F	4.0	569.68	0.42	476
Cl	3.0	431.36	0.79	350
Br	2.8	366.16	1.2	337
BDE: Bond dissociation energy

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表 2 不同元素掺杂SnO₂薄膜的电学参数和透过率

Table 2. The electrical parameters and transmittance of SnO₂ thin films with different dopants.

Doping elements	Conductivity/Ω^–1·cm^–1	Carrier density /cm^–3	Hall Mobility /cm²·V^–1·s^–1	Transmittance/%	Technique	Ref.
F	0.33 × 10³	2.62 × 10²⁰	7.96	86	spray pyrolysis	[51]
F	1.43 × 10³	1.10 × 10²¹	8.1	90	dip-coating	[52]
Li, F	2.70 × 10³	5.62 × 10²⁰	29.1	70	spray pyrolysis	[53]
P, F	4.0 × 10⁵	8.30 × 10²⁶	0.0032	86	spray pyrolysis	[54]
Sb	0.36 × 10³	6.37 × 10²¹	0.347	61	spin-coating	[55]
Sb	3.50 × 10³	1.68 × 10²¹	12.03	—	spray pyrolysis	[56]
Ta	0.50 × 10³	1.30 × 10²⁰	29.26	80	spray pyrolysis	[57]
Pr	0.26 × 10³	8.70 × 10¹⁹	18.75	80	spray pyrolysis	[59]
W	0.17 × 10³	7.60 × 10¹⁹	14.2	90	dip-coating	[60]
Nb	0.23 × 10³	5.00 × 10¹⁹	25	70	spray pyrolysis	[61]

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表 3 溶液法制备SnO₂基TFTs的电学性能

Table 3. Electrical properties of solution-processed SnO₂-based TFTs.

Solute	Dopant	Concentration /mol·L^–1	Substrate	Channel thickness/nm	Annealing temperature /℃	Mobility /cm²·V^–1·s^–1	I_on/I_off	SS/V·dec^–1	Ref.
SnCl₂·2H₂O	—	0.02	SiO₂/Si	3.8	500	11.2	6.8 × 10⁶	0.78	[63]
SnCl₂·2H₂O	—	0.167	HfO₂/Mo	9.2	300	99.16	1.7 × 10⁸	0.114	[64]
SnCl₂·2H₂O	Ga(NO₃)₃ ·xH₂O	0.12	SiO₂/Si	—	400	4.1	6.6 × 10⁶	0.77	[65]
SnCl₂·2H₂O	—	0.03	SiO₂/Si	—	500	12.18	5 × 10⁷	1.17	[66]
SnCl₂·2H₂O	—	0.1	ZrO₂/ITO	22	400	103	10⁴—10⁵	0.3	[67]
C₁₆H₃₀O₄Sn	—	0.5	Al₂O₃/ITO	15	350	96.4	2.2 × 10⁶	0.26	[68]

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表 4 溶液法制备p型SnO₂基薄膜的电学性能

Table 4. Electrical properties of solution-processed p type SnO₂-based films.

Solute	Dopant	Resistivity /Ω·cm	Carrier density/cm^–3	Hall Mobility /cm²·V^–1·s^–1	Bandgap/eV	Technique	Ref.
SnCl₂·2H₂O	AlCl₃	3.6 × 10^–2	6.7 × 10¹⁸	25.90	4.11	spray pyrolysis	[74]
SnCl₂·2H₂O	Ga(NO₃)₃·H₂O	1.6	1.70 × 10¹⁸	6.34	3.83	spin-coating	[75]
SnCl₂·2H₂O	InCl₃·4H₂O	20.4	1.85 × 10¹⁷	1.57	3.8	dip-coating	[76]
SnCl₂·2H₂O	InCl₃·4H₂O, GaCl₃	0.17	9.5 × 10¹⁷	39.2	3.38	spray pyrolysis	[77]
SnCl₂·2H₂O	FeCl₃·6H₂O	660	1.4 × 10¹⁵	6.75	3.75	dip-coating	[78]
SnCl₂·2H₂O	MgCl₂·6H₂O	2.5 × 10⁴	10¹⁴	1.6	3.73	spin-coating	[79]
SnCl₂·2H₂O	MnCl₂	359.1	6.72 × 10¹⁴	6.14	3.85	dip-coating	[80]
SnCl₂·2H₂O	CoCl₂·6H₂O	140	1.47 × 10¹⁵	8.25	3.81	spin-coating	[81]

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[1]	Grundmann M, Frenzel H, Lajn A, Lorenz M, Schein F, von Wenckstern H 2010 Phys. Status Solidi Appl. Mater. Sci. 207 1437 Google Scholar
[2]	Yu X, Marks T J, Facchetti A 2016 Nat. Mater. 15 383 Google Scholar
[3]	Park J, Kim H, Kim I 2014 J. Electroceram. 32 117 Google Scholar
[4]	Hosono H 2007 Thin Solid Films 515 6000 Google Scholar
[5]	Park J S, Maeng W J, Kim H S, Park J S 2012 Thin Solid Films 520 1679 Google Scholar
[6]	Facchetti A, Marks T J 2010 Transparent Electron. From Synth. to Appl. 561 2002
[7]	Fortunato E, Barquinha P, Martins R 2012 Adv. Mater. 24 2945 Google Scholar
[8]	Chopra K L, Major S, Pandya D K 1983 Thin Solid Films. 102 1 Google Scholar
[9]	Nomura K, Ohta H, Takagi A, Kamiya T, Hirano M, Hosono H 2004 Nature 432 488 Google Scholar
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[11]	Fang F, Zhang Y, Wu X, ShaO Q, Xie Z 2015 Mater. Res. Bull. 68 240 Google Scholar
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