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氧流量比和热退火对反应直流磁控溅射法制备的铝掺杂氧化锌薄膜缺陷演变的影响

Effects of oxygen flow ratio and thermal annealing on defect evolution of aluminum doped zinc oxide thin films by reactive DC magnetron sputtering.

作者信息

Liu Chao Ping, Li Zhan Hua, Egbo Kingsley O, Kwok Cheuk Kai, Lv Xiao Hu, Ho Chun Yuen, Wang Ying, Yu Kin Man

机构信息

Research Center for Advanced Optics and Photoelectronics, Department of Physics, College of Science, Shantou University, Shantou, Guangdong 515063, People's Republic of China.

Department of Physics, City University of Hong Kong, 83 Tat Chee Ave., Kowloon, Hong Kong Special Administrative Region of China.

出版信息

J Phys Condens Matter. 2021 Sep 3;33(46). doi: 10.1088/1361-648X/ac1f50.

Abstract

Al doped ZnO (AZO) is a promising transparent conducting oxide to replace the expensive Sn doped InO(ITO). Understanding the formation and evolution of defects in AZO is essential for its further improvement. Here, we synthesize transparent conducting AZO thin films by reactive DC magnetron sputtering. The effects of oxygen flow ratio as well as the rapid thermal annealing (RTA) in different conditions on their structural and optoelectrical properties were investigated by a variety of analytical techniques. We find that AZO thin films grown in O-rich conditions exhibit inferior optoelectrical performance as compared with those grown in Zn-rich conditions, possibly due to the formation of excessive native acceptor defects and/or secondary phases (e.g. AlO). Temperature-dependent Hall measurements indicate that mobilities of these highly degenerate AZO films with> 10 cmare primarily limited by ionized and neutral impurities, while films with relatively low∼ 10 cmexhibit a temperature-activated mobility owing to the grain-barrier scattering. Asincreases, the optical band gap of AZO thin film increases as a result of Burstein-Moss shift and band gap narrowing. RTA treatments under appropriate conditions (i.e. at 500 °C for 60 s in Ar) can further improve the electrical properties of AZO thin film, with low resistivity of ∼6.2 × 10Ω cm achieved, while RTA at high temperature with longer time can lead to the formation of substantial sub-gap defect states and thus lowers the electron mobility. X-ray photoelectron spectroscopy provides further evidence on the variation of Al (Zn) content at the surface of AZO thin films with different processing conditions.

摘要

铝掺杂氧化锌(AZO)是一种很有前景的透明导电氧化物,有望取代昂贵的锡掺杂氧化铟(ITO)。了解AZO中缺陷的形成和演变对于其进一步改进至关重要。在此,我们通过反应性直流磁控溅射合成了透明导电的AZO薄膜。利用多种分析技术研究了氧流量比以及不同条件下的快速热退火(RTA)对其结构和光电性能的影响。我们发现,与在富锌条件下生长的AZO薄膜相比,在富氧条件下生长的AZO薄膜表现出较差的光电性能,这可能是由于形成了过多的本征受主缺陷和/或第二相(如AlO)。变温霍尔测量表明,这些高简并度(载流子浓度>10¹⁹ cm⁻³)的AZO薄膜的迁移率主要受电离杂质和中性杂质限制,而载流子浓度相对较低(10¹⁸ cm⁻³)的薄膜由于晶粒间界散射表现出温度激活的迁移率。随着载流子浓度增加,由于Burstein-Moss位移和带隙变窄,AZO薄膜的光学带隙增大。在适当条件下(即在500℃的氩气中退火60秒)进行RTA处理可以进一步改善AZO薄膜的电学性能,实现低至6.2×10⁻⁴Ω·cm的电阻率,而高温长时间的RTA会导致形成大量的亚带隙缺陷态,从而降低电子迁移率。X射线光电子能谱为不同处理条件下AZO薄膜表面Al(Zn)含量的变化提供了进一步的证据。

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