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.
Keywords: PMMA; high-k dielectric thin film; hybrid gel film; modified sol-gel; nBB-based hybrid; transparent flexible electronics; zirconia.