Yuyun Yao, Mustafeez Bashir Shah, Wanpeng Lu, Xian’e Li, Rushil Vasant, Zeinab Hamid, Keren Ai, Junfu Tian, Maryam Alsufyani, Jonathan Rawle, Malina Gaşpar, Qingpei Wan, Rachael Found, Wesley Chen, Tomaž Kotnik, Thuc-Quyen Nguyen, Achilleas Savva, James R. Durrant, Iain McCulloch
High Resolution Image Download MS PowerPoint Slide The development of organic electrochemical transistors (OECTs) critically depends on the design and characterization of mixed-conducting, high-performance conjugated polymers (CPs) as channel materials, particularly for n-type OECTs. In this study, we present a novel strategy to enhance the OECT performance of a semiconducting polymer film via a postdeposition ester pyrolysis of thermally cleavable side chains, thus facilitating ion incorporation and transport within the bulk. Our approach relies on the synthesis of a high glass-transition, rigid-rod polymer, able to withstand the pyrolysis temperature without deformation and maintain the voids formed from the pyrolysis reaction which removes the thermally cleavable ester side chains. After side-chain cleavage, the resulting film exhibits increased porosity, hydrophilicity, and crystallinity. By creating bulk porosity in thin films via this approach, ion diffusion is enhanced, resulting in a superior μ C* figure of merit up to 158.85 F cm –1 V –1 s –1, and a corresponding increase in normalized transconductance (31.67 S cm –1 ). In addition, the device switching speed and long-term stability are also observed to increase, further demonstrating the benefit of nanoscale porosity for mixed conductivity semiconductors.