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Frequency-Agile Low-temperature Solution-Processed Alumina Dielectrics for Inorganic and Organic Electronics Enhanced by Fluoride Doping
Journal of the American Chemical Society ( IF 15.0 ) Pub Date : 2020-06-15 , DOI: 10.1021/jacs.0c05161
Xinming Zhuang 1, 2 , Sawankumar Patel 3 , Chi Zhang 4 , Binghao Wang 2 , Yao Chen 2 , Haoyu Liu 3 , Vinayak P Dravid 4 , Junsheng Yu 1 , Yan-Yan Hu 3, 5 , Wei Huang 2 , Antonio Facchetti 2, 6 , Tobin J Marks 2
Affiliation  

The frequency-dependent capacitance of low-temperature solution-processed metal oxide (MO) dielectrics typically yields unrelia-ble and unstable thin-film transistor (TFT) performance metrics, which hinders the development of next-generation roll-to-roll MO electronics, and obscures inter-comparisons between processing methodologies. Here, capacitance values stable over a wide fre-quency range are achieved in low-temperature combustion-synthesized aluminum oxide (AlOx) dielectric films by fluoride doping. For an optimal F incorporation of ~ 3.7 atomic % F, the F:AlOx film capacitance of 166±11 nF/cm2 is stable over a 10-1 - 104 Hz frequency range, far more stable than that of neat AlOx films (capacitance = 336±201 nF/cm2) which falls from 781±85 nF/cm2 to 104±4 nF/cm2 over this frequency range. Importantly, both n-type/inorganic and p-type/organic TFTs exhibit reliable electrical characteris-tics with minimum hysteresis when employing the F:AlOx dielectric with ~ 3.7 atomic % F. Systematic characterization of film microstructural/compositional and electronic/dielectric properties by X-ray photoelectron spectroscopy, time-of-fight secondary ion mass spectrometry, cross-section transmission electron microscopy, solid-state nuclear magnetic resonance, and UV-vis absorption spectroscopy reveal that fluoride doping generates AlOF, which strongly suppresses the mobile hydrogen content, suppressing polarization mechanisms at low frequencies. Thus, this work provides a broadly applicable anion doping strategy for the realization of high-performance solution-processed metal oxide dielectrics for both organic and inorganic electronics applications.

中文翻译:

氟化物掺杂增强的用于无机和有机电子设备的频率捷变低温固溶氧化铝电介质

低温溶液处理的金属氧化物 (MO) 电介质的频率相关电容通常会产生不可靠且不稳定的薄膜晶体管 (TFT) 性能指标,这阻碍了下一代卷对卷 MO 电子设备的发展,并掩盖了处理方法之间的相互比较。在这里,通过氟化物掺杂在低温燃烧合成氧化铝 (AlOx) 介电膜中实现了在宽频率范围内稳定的电容值。对于约 3.7 原子 % F 的最佳 F 掺入,166±11 nF/cm2 的 F:AlOx 薄膜电容在 10-1 - 104 Hz 频率范围内稳定,远比纯 AlOx 薄膜(电容 = 336±201 nF/cm2),在这个频率范围内从 781±85 nF/cm2 下降到 104±4 nF/cm2。重要的,当采用 F:AlOx 电介质时,n 型/无机和 p 型/有机 TFT 均表现出可靠的电气特性,具有最小的滞后。 X 对薄膜微观结构/组成和电子/介电特性的系统表征射线光电子能谱、战斗时间二次离子质谱、横截面透射电子显微镜、固态核磁共振和紫外可见吸收光谱表明,氟化物掺杂会产生 AlOF,强烈抑制移动氢含量,抑制低频的极化机制。因此,这项工作为实现用于有机和无机电子应用的高性能溶液处理金属氧化物电介质提供了一种广泛适用的阴离子掺杂策略。
更新日期:2020-06-15
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