Here we present and discuss our recent investigations into the understanding of microscopic charge transport, novel film processing technologies, and a development of layered-crystalline organic semiconductors for high performance OTFTs. We first discuss the microscopic charge transport in the OTFTs, as investigated by field-induced electron spin resonance spectroscopy. The technique can detect signals due to tiny amount of field-induced carriers, accumulated at the semiconductor-insulator interfaces. Following aspects are presented and discussed; 1) Carrier motion within the crystalline domains can be understood in terms of the trap-and-release transport, 2) charge trap states are spatially extended over several sites depending on the trap levels, and 3) the intra- and inter-domain transport can be discriminated by anisotropic electron spin resonance measurements. Next we discuss novel print production technologies for organic semiconductors showing high layered crystallinity. The concept of “printed electronics” is now regarded as a realistic paradigm to manufacture light-weight, thin, and impact-resistant electronics devices, although production of highly crystalline semiconductor films may be incompatible with conventional printing process. We here present printing techniques for manufacturing high performance OTFTs; 1) double-shot inkjet printing for small-molecule-based semiconductors, and 2) push-coating for semiconducting polymers. We demonstrate that both processes are useful to manufacture high quality semiconductor layers with the high layered crystallinity.
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