Leveraging Bio-Inspired and Dynamic Chemistry to Develop Soft and Degradable Thin-Film Transistors

π-Conjugated semiconducting polymers possess remarkable properties such as excellent charge transport, low elastic moduli, and high biocompatibility/low toxicity. As the use of semiconducting polymers continues to expand across various fields, there has been limited focus on their environmental impact. From manufacturing and processing with toxic, high-boiling-point solvents to their accumulation in electronic waste, the environmental footprint of organic semiconducting materials is a growing concern. While efforts to develop more eco-friendly manufacturing processes are essential, equally critical is the need to design materials and electronics with controllable lifespans and functionalities. This dual approach is crucial for advancing sustainable technologies, particularly in applications that integrate with the human body. To address the environmental and biointegration challenges posed by semiconducting materials in organic electronics, our team has explored new materials-driven strategies for creating degradable polymers and thin-film transistors. These strategies draw inspiration from nature, utilizing functional groups and moieties that degrade under specific conditions. By leveraging dynamic disulfide bonds that spontaneously break and reform, or incorporating carbohydrates and proteins that can be enzymatically decomposed, bio-inspired materials provide a rich structural toolbox for the development of organic electronics that seamlessly combine sustainability, softness, and high performance.

This presentation will focus on our recent efforts to achieve controllable degradation in semiconducting polymers and thin film transistors. Toward this goal, we designed diketopyrrolopyrrole-based semiconducting polymers that incorporate dynamic disulfide bonds, which can break and reform under light exposure. This behavior, driven by the formation of organic radicals, allows the materials to be processed into thin films while exhibiting notable solid-state reversibility and degradation properties, which we explore further in the context of organic electronics. We will also introduce recent work on enzyme-degradable oligosaccharides and their incorporation into the backbone of isoindigo-based polymers, expanding the scope of degradable materials. Additionally, we will discuss recent advancements in our group on fabricating thin-film electronics using degradable polyesters derived from environmentally benign precursors. Throughout the presentation, we will introduce results from a comprehensive characterization of the solid-state morphology of these new materials in thin films, highlighting the structure-property relationships revealed through our investigations. We will also emphasize the findings from a multimodal characterization strategy applied to both the materials and thin-film transistors.