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透明导电氧化物 (transparent conductive oxides, TCOs)薄膜和透明氧化物半导体 (transparent oxide semiconductors, TOSs) 薄膜具有高透明度和良好的导电率等特点, 广泛应用于太阳能电池、平板显示、智能窗以及透明柔性电子器件等领域. 大多数TCOs和TSOs薄膜主要是以氧化铟、氧化锌和氧化锡三种材料为基础衍生来的, 其中, 氧化铟薄膜中In元素有毒、含量稀少且价格昂贵, 会造成环境污染; 氧化锌薄膜对酸或碱刻蚀液敏感, 薄膜图形化困难; 氧化锡薄膜不仅无毒、无污染、价格低廉, 还具有良好的电学性能和化学稳定性, 具有巨大的发展潜力. 目前, 薄膜的制备主要依赖于真空镀膜技术. 此类技术的缺点在于设备结构复杂且价格昂贵、能耗高、工艺复杂、生产成本高等. 相比传统真空镀膜技术, 溶胶-凝胶法具有工艺简单、成本低等优点, 受到了人们的广泛关注. 本文从TCOs和TSOs薄膜的发展现状和发展趋势出发, 先介绍了氧化锡薄膜的结构特性、导电机制、元素掺杂理论以及载流子散射机理, 然后介绍了溶胶-凝胶法原理和制备方法, 接着介绍了近些年来溶胶-凝胶法制备氧化锡基薄膜在n型透明导电薄膜、薄膜晶体管以及p型半导体薄膜中的应用和发展, 最后总结了当前存在的问题以及今后研究的方向.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.
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Keywords:
- tin oxide/
- sol-gel method/
- transparent conductive oxide films/
- transparent semiconductor oxide films/
- thin film transistor/
- p-type semiconductor films
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Element Electroneg-
ativityBDE 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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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] 下载:
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Solute Dopant Concentration /mol·L–1 Substrate Channel thickness/nm Annealing temperature /℃ Mobility /cm2·V–1·s–1 Ion/Ioff 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
·xH2O0.12 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] 下载:
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Solute Dopant Resistivity
/Ω·cmCarrier
density/cm–3Hall Mobility
/cm2·V–1·s–1Bandgap/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] 下载:
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