Frequency-Agile Low-Temperature Solution-Processed Alumina Dielectrics for Inorganic and Organic Electronics Enhanced by Fluoride Doping

Xinming Zhuang, Sawankumar Patel, Chi Zhang, Binghao Wang, Yao Chen, Haoyu Liu, Vinayak P. Dravid, Junsheng Yu, Yan Yan Hu, Wei Huang, Antonio Facchetti, Tobin J. Marks

Research output: Contribution to journalArticle

Abstract

The frequency-dependent capacitance of low-temperature solution-processed metal oxide (MO) dielectrics typically yields unreliable and unstable thin-film transistor (TFT) performance metrics, which hinders the development of next-generation roll-to-roll MO electronics and obscures intercomparisons between processing methodologies. Here, capacitance values stable over a wide frequency 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 characteristics 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 reduces 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.

Original languageEnglish
Pages (from-to)12440-12452
Number of pages13
JournalJournal of the American Chemical Society
Volume142
Issue number28
DOIs
Publication statusPublished - Jul 15 2020

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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    Zhuang, X., Patel, S., Zhang, C., Wang, B., Chen, Y., Liu, H., Dravid, V. P., Yu, J., Hu, Y. Y., Huang, W., Facchetti, A., & Marks, T. J. (2020). Frequency-Agile Low-Temperature Solution-Processed Alumina Dielectrics for Inorganic and Organic Electronics Enhanced by Fluoride Doping. Journal of the American Chemical Society, 142(28), 12440-12452. https://doi.org/10.1021/jacs.0c05161