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The optoelectronic properties of semiconducting polymers and device performance rely on a delicate interplay of design and processing conditions. However, screening and optimizing the relationships between these parameters for reliably fabricating organic electronics can be an arduous task requiring significant time and resources. To overcome this challenge, Polybot is developed—a robotic platform within a self‐driving lab that can efficiently produce organic field‐effect transistors (OFETs) from various semiconducting polymers via high‐throughput blade coating deposition. Polybot not only handles the fabrication process but also can conduct characterization tests on the devices and autonomously analyze the data gathered, thus facilitating the rapid acquisition of data on a large scale. This work leverages the capabilities of this platform to investigate the fabrication of OFETs using hydrogen bonding‐containing semiconducting polymers. Through high‐throughput fabrication and characterization, various data trends are analyzed, and large extents of anisotropic charge mobility are observed in devices. The materials are thoroughly characterized to understand the role of processing conditions in solid state and electronic properties of these organic semiconductors. The findings demonstrate the effectiveness of automated fabrication and characterization platforms in uncovering novel structure–property relationships, facilitating refinement of rational chemical design, and processing conditions, ultimately leading to new semiconducting materials. [ABSTRACT FROM AUTHOR]

Organic electroactive materials, particularly semiconducting polymers, are at the forefront of emerging organic electronics. Among the plethora of unique features, the possibility to formulate inks out of these materials is particularly promising for the large‐scale manufacturing of electronics at lower cost on a variety of soft substrates. While solution deposition of semiconducting materials is promising for developing printed electronics, the environmental footprint of the materials and related devices needs to be considered to achieve sustainable manufacturing. Towards the development of greener printed electronics, this work investigates the utilization of a non‐toxic, environmentally‐friendly solvent, namely branched polyethylene (BPE), to formulate semiconducting inks. Focusing on a diketopyrrolopyrrole‐based (DPP) semiconducting polymer, shellac as dielectric, and BPE as the solvent, solutions were prepared in different concentrations and their rheological properties were characterized. Then, printing on polyethylene terephthalate (PET) substrates using two different techniques was performed to fabricate organic field‐effect transistors (OFETs). Both printing techniques yielded OFETs with good performance and device characteristics, averaging approximately 10−2 and 10−4 cm2 V−1 s−1, respectively, for slot‐die coating and direct‐ink writing deposition. Notably, despite some difference in threshold voltages, OFETs produced via slot‐die coating and direct‐ink writing showed comparable charge mobilities to previously reported OFETs prepared from similar materials, particularly those prepared on silicon dioxide wafers. Overall, this work confirms the suitability of BPE to formulate semiconducting inks to develop printed electronics in a greener manner. The printing methodology developed in this work also open new avenues for the design of functional printed electronics and related technologies. [ABSTRACT FROM AUTHOR]