ZnO@SnO_2包覆结构透明导电薄膜的制备及其发光性能研究
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摘要
氧化物透明导电薄膜被广泛应用于太阳能电池、液晶显示屏、等离子显示屏、抗静电涂层以及半导体／绝缘体／半导体(SIS)异质结、现代战机和巡航导弹的窗口等领域。研究表明,ZnO透明导电薄膜存在表面和晶粒间界氧吸附导致电学性能下降,SnO2透明导电薄膜存在难以刻蚀等问题,这极大的限制了ZnO、SnO2透明导电薄膜的应用范围。ZnO@SnO2薄膜兼备ZnO和SnO2的优点,这将有利于ZnO、SnO2透明导电薄膜的应用领域。
本论文采用以溶胶-凝胶法为基础的二步成胶工艺制备ZnO@SnO2包覆结构的粉体和透明导电薄膜。采用X射线衍射(XRD)、透射电子显微分析(TEM)、X射线光电子能谱(XPS)对粉体样品进行了结构分析和包覆性能表征,结果表明,ZnO@SnO2是以ZnO为核、SnO2为壳的核壳式包覆结构,是一种化学包覆结构,ZnO和SnO2之间以化学键Zn-O-Sn结合；并且当Zn／Sn摩尔比为8／12包覆效果较好。
利用NKD-8000e和四探针测试仪对ZnO@SnO2包覆结构的光学和电学性能进行表征,结果表明,可见光透过率均超过80%,当Sb掺杂浓度4at%,退火温度为600℃,Zn／Sn摩尔比为9／12时,电阻率最低可达1.1×10-3Ω.cm讨论了Zn／Sn摩尔比、退火温度、掺杂浓度、薄膜厚度等对可见光透过率和电阻率的影响。
研究了ZnO@SnO2包覆结构的光致发光特性,发现SnO2的包覆会使ZnO中的蓝光发射得到增强,原因是SnO2包覆结构增加了Zn空位缺陷密度,使Zn到Zn空位之间跃迁增强。
The transparent conductive oxide films are widely used in the fields of solar cells, liquid crystal displays, plasma displays, antistatic coatings, semiconductor/insulator/semiconductor (SIS) hetero-junction, the windows of modern warplanes and cruise missiles. Many investigation reveal that the electricity property of ZnO transparent conductive thin film is deteriorated by the adsorption of oxygen on the surface and crystal grain boundary. The SnO2 transparent conductive thin film is difficut to be corroded. This limits the application of the above two transparent conductive thin films greatly. ZnO@SnO2 have the advantages of both ZnO and SnO2, which will be more propitious to hasten the studies and application of the transparent conducting thin films.
In this thesis, the ZnO@SnO2 structure was prepared by the two steps gelation technique, which was based on the sol-gel method. The prepared samples were charicterized by the the X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS). The experimental results revealed that the ZnO@SnO2 was a chemical coating structure with cores of ZnO and shells of SnO2. The ZnO and SnO2 was bonded by the Zn-O-Sn net. The coating structure could in a better status when the Zn/Sn mol ratio was 8/12.
Moreover, the optical and electrical properties of the ZnO@SnO2 samples were characterized by the NKD-8000e and four-probe measurements, respectively. The results show that the optical transmittance is higher than 80% in the visible range, and the lowest resistivity is 1.1×10-3Ω·cm When the doping content of Sb is 4at%, the annealing temperature is 600℃, and the mol ratio of Zn/Sn is 9/12. The effect of molar ratio of Zn/Sn, annealing temperature, doping concentration, film thickness etc on the transmittance and resistivity of ZnO@SnO2 sample was discussed.
The photoluminescence of ZnO@SnO2 coating structure was investigated. It is found that the coating of SnO2 enhance the blue-ray emission of ZnO, because the coating structure of SnO2 increased the defect density of Zn vacanc, and increased the transition between the Zn to the Zn vacancy.
本论文采用以溶胶-凝胶法为基础的二步成胶工艺制备ZnO@SnO2包覆结构的粉体和透明导电薄膜。采用X射线衍射(XRD)、透射电子显微分析(TEM)、X射线光电子能谱(XPS)对粉体样品进行了结构分析和包覆性能表征,结果表明,ZnO@SnO2是以ZnO为核、SnO2为壳的核壳式包覆结构,是一种化学包覆结构,ZnO和SnO2之间以化学键Zn-O-Sn结合；并且当Zn／Sn摩尔比为8／12包覆效果较好。
利用NKD-8000e和四探针测试仪对ZnO@SnO2包覆结构的光学和电学性能进行表征,结果表明,可见光透过率均超过80%,当Sb掺杂浓度4at%,退火温度为600℃,Zn／Sn摩尔比为9／12时,电阻率最低可达1.1×10-3Ω.cm讨论了Zn／Sn摩尔比、退火温度、掺杂浓度、薄膜厚度等对可见光透过率和电阻率的影响。
研究了ZnO@SnO2包覆结构的光致发光特性,发现SnO2的包覆会使ZnO中的蓝光发射得到增强,原因是SnO2包覆结构增加了Zn空位缺陷密度,使Zn到Zn空位之间跃迁增强。
The transparent conductive oxide films are widely used in the fields of solar cells, liquid crystal displays, plasma displays, antistatic coatings, semiconductor/insulator/semiconductor (SIS) hetero-junction, the windows of modern warplanes and cruise missiles. Many investigation reveal that the electricity property of ZnO transparent conductive thin film is deteriorated by the adsorption of oxygen on the surface and crystal grain boundary. The SnO2 transparent conductive thin film is difficut to be corroded. This limits the application of the above two transparent conductive thin films greatly. ZnO@SnO2 have the advantages of both ZnO and SnO2, which will be more propitious to hasten the studies and application of the transparent conducting thin films.
In this thesis, the ZnO@SnO2 structure was prepared by the two steps gelation technique, which was based on the sol-gel method. The prepared samples were charicterized by the the X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS). The experimental results revealed that the ZnO@SnO2 was a chemical coating structure with cores of ZnO and shells of SnO2. The ZnO and SnO2 was bonded by the Zn-O-Sn net. The coating structure could in a better status when the Zn/Sn mol ratio was 8/12.
Moreover, the optical and electrical properties of the ZnO@SnO2 samples were characterized by the NKD-8000e and four-probe measurements, respectively. The results show that the optical transmittance is higher than 80% in the visible range, and the lowest resistivity is 1.1×10-3Ω·cm When the doping content of Sb is 4at%, the annealing temperature is 600℃, and the mol ratio of Zn/Sn is 9/12. The effect of molar ratio of Zn/Sn, annealing temperature, doping concentration, film thickness etc on the transmittance and resistivity of ZnO@SnO2 sample was discussed.
The photoluminescence of ZnO@SnO2 coating structure was investigated. It is found that the coating of SnO2 enhance the blue-ray emission of ZnO, because the coating structure of SnO2 increased the defect density of Zn vacanc, and increased the transition between the Zn to the Zn vacancy.
引文
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