We propose a highly efficient crosslinking strategy for organic-inorganic hybrid dielectric layers using azide-functionalized acetylacetonate, which covalently connect inorganic particles to polymers, enabling highly efficient inter- and intra-crosslinking of organic and inorganic inclusions, resulting in a dense and defect-free thin-film morphology. From the optimized processing conditions, we obtained an excellent dielectric strength of over 4.0 MV cm-1, a high dielectric constant of ~14, and a low surface energy of 38 mN m-1. We demonstrated the fabrication of exceptionally high-performance, hysteresis-free n-type solution-processed oxide transistors comprising an In2O3/ZnO double layer as an active channel with an electron mobility of over 50 cm2 V-1 s-1, on/off ratio of ~107, subthreshold swing of 108 mV dec-1, and high bias-stress stability. From temperature-dependent I-V analyses combined with charge transport mechanism analyses, we demonstrated that the proposed hybrid dielectric layer provides percolation-limited charge transport for the In2O3/ZnO double layer under field-effect conditions.
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