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Experimental and theoretical evidence for hydrogen doping in polymer solution-processed indium gallium oxide.
Proceedings of the National Academy of Sciences of the United States of America ( IF 11.1 ) Pub Date : 2020-08-04 , DOI: 10.1073/pnas.2007897117
Wei Huang 1, 2 , Po-Hsiu Chien 3, 4 , Kyle McMillen 5 , Sawankumar Patel 3 , Joshua Tedesco 6 , Li Zeng 7, 8 , Subhrangsu Mukherjee 9 , Binghao Wang 1, 2 , Yao Chen 1, 2 , Gang Wang 1, 2 , Yang Wang 1, 2 , Yanshan Gao 1, 2 , Michael J Bedzyk 8, 10 , Dean M DeLongchamp 11 , Yan-Yan Hu 4, 12 , Julia E Medvedeva 13 , Tobin J Marks 2, 14 , Antonio Facchetti 2, 14, 15
Affiliation  

The field-effect electron mobility of aqueous solution-processed indium gallium oxide (IGO) thin-film transistors (TFTs) is significantly enhanced by polyvinyl alcohol (PVA) addition to the precursor solution, a >70-fold increase to 7.9 cm2/Vs. To understand the origin of this remarkable phenomenon, microstructure, electronic structure, and charge transport of IGO:PVA film are investigated by a battery of experimental and theoretical techniques, including In K-edge and Ga K-edge extended X-ray absorption fine structure (EXAFS); resonant soft X-ray scattering (R-SoXS); ultraviolet photoelectron spectroscopy (UPS); Fourier transform-infrared (FT-IR) spectroscopy; time-of-flight secondary-ion mass spectrometry (ToF-SIMS); composition-/processing-dependent TFT properties; high-resolution solid-state 1H, 71Ga, and 115In NMR spectroscopy; and discrete Fourier transform (DFT) analysis with ab initio molecular dynamics (MD) liquid-quench simulations. The 71Ga{1H} rotational-echo double-resonance (REDOR) NMR and other data indicate that PVA achieves optimal H doping with a Ga···H distance of ∼3.4 Å and conversion from six- to four-coordinate Ga, which together suppress deep trap defect localization. This reduces metal-oxide polyhedral distortion, thereby increasing the electron mobility. Hydroxyl polymer doping thus offers a pathway for efficient H doping in green solvent-processed metal oxide films and the promise of high-performance, ultra-stable metal oxide semiconductor electronics with simple binary compositions.



中文翻译:

在聚合物溶液处理的氧化铟镓中氢掺杂的实验和理论证据。

通过将聚乙烯醇(PVA)添加到前体溶液中,水溶液处理的铟镓氧化物(IGO)薄膜晶体管(TFT)的场效应电子迁移率显着提高,增加了70倍,达到7.9 cm 2 / VS. 为了了解这种现象的起源,通过一系列实验和理论技术研究了IGO:PVA薄膜的微观结构,电子结构和电荷传输,包括In K-edge和Ga K-edge扩展X射线吸收精细结构(EXAFS);共振软X射线散射(R-SoXS); 紫外光电子能谱(UPS); 傅立叶变换红外(FT-IR)光谱;飞行时间二次离子质谱(ToF-SIMS)与成分/工艺有关的TFT特性;高分辨率固态1H,71 Ga和115 In NMR光谱;以及从头算分子动力学(MD)液体猝灭模拟的离散傅里叶变换(DFT)分析。在71嘎{ 1个H}旋转回波双共振(REDOR)NMR和其他数据表明,PVA达到最佳ħ掺杂与~3.4埃的嘎...ħ距离和转换从六到四个坐标镓,它们一起抑制了深陷阱缺陷的定位。这减少了金属氧化物多面体畸变,从而增加了电子迁移率。因此,羟基聚合物掺杂为绿色溶剂加工的金属氧化物膜中的有效H掺杂提供了途径,并有望以简单的二元组成提供高性能,超稳定的金属氧化物半导体电子产品。

更新日期:2020-08-05
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