Dual-Function Ladder Polysilsesquioxanes for Precise Patterning and 3D Integration of High-Performance Flexible Organic Logic Circuits
Precise patterning of highly ordered organic semiconductor (OSC) thin-film arrays is critical for next-generation electronics. We report a ladder-like polysilsesquioxane (LPSQ) strategy to synthesize two functional analogs with tunable surface energies and robust dielectric properties. These LPSQ dielectrics, functionalized with alkyl or fluoroalkyl side chains, serve dual roles as gate insulators and patterning layers to guide blade-coating of 2,7-dioctyl[1]benzothieno[3,2-b][1]benzothiophene (C8-BTBT). This approach yields highly aligned arrays suitable for three-dimensional integration in flexible electronics. Synergistic combination of dense LPSQ dielectric packing and aligned semiconductor domains leads to excellent organic thin-film transistor (OTFT) performance, achieving approximately four-fold improvement in field-effect mobility compared to conventional silicon oxide dielectrics. Patterned LPSQ dielectrics enable high-resolution C8-BTBT patterning on plastic substrates, supporting 4-inch-scale 3D integration of flexible logic circuits, including inverters (voltage gain >100), NOR gates, and NAND gates. This work provides a scalable route to high-performance, large-area flexible organic circuits.