Abstract
Bottom-up approaches in solutions enable the low-temperature preparation of hybrid thin films suitable for printable transparent and flexible electronic devices. We report the obtainment of new transparent PMMA/ZrO2 nanostructured -building blocks (nBBs) hybrid thin films (61–75 nm) by a modified sol-gel method using zirconium ethoxide, Zr(OEt)4, and 3-methacryloxypropyl trimethoxysilane (MPS) as a coupling agent and methylmethacrylate monomer (MMA). The effect of low-temperature and UV irradiation on the nBBs gel films is discussed. The thermal behaviors of the hybrid sols and as-deposed gel films were investigated by modulated thermogravimetric (mTG) and differential scanning calorimetry (DSC) analysis. The chemical structure of the resulted films was elucidated by X-ray photoelectron (XPS), infrared (IR) and Raman spectroscopies. Their morphology and crystalline structure were observed by scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HR-TEM), and grazing incidence X-ray diffraction. The cured films show zirconia nanocrystallites of 2–4 nm in the hybrid matrix and different self-assembled structures for 160 °C or UV treatment; excellent dielectric behavior, with dielectric constant values within 6.7–17.9, depending on the Zr(OEt)4:MMA molar ratio, were obtained.
Highlights
The very small rate and weight loss over 120 ◦ C seems the beginning of a complex process, with overlapping steps, of structuration of the gel resulted in the previous steps
By aging the 1:1:1 and 6:1:1 sols for 24 h, more visible differences can be observed between the two sol compositions, namely the richest in zirconium ethoxide (6:1:1) sol underwent a bigger mass loss of 3.8%
In this work we report a modified sol-gel method by adding a vinyl-silane type (MPS)
Summary
Paving the way towards printability, solution processible metal oxides have to be integrated with complementary interfacing materials to deliver optimized contact performance [3] and channel control [1] For the latter, hybrid materials combining properties of the organic polymers (flexibility, elasticity, adhesion to substrate, facile processing, low leakage) with those of the inorganic compounds (high permittivity, optical and thermal properties) can simultaneously meet all the requirements of the gate dielectric for use in transparent and/or flexible electronics [1,2,3,4]. Vacuum and photolithographic techniques for production of high-quality transparent and flexible electronics have been replaced by the solution-base printed technique [11] The latter one implies adequate reagents selection for sol preparation [12], low processing temperature (
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