'Ideal' transparent p-type semiconductors are required for the integration of high-performance thin-film transistors (TFTs) and circuits. Although CuI has recently attracted attention owing to its excellent opto-electrical properties, solution processability, and low-temperature synthesis, the uncontrolled copper vacancy generation and subsequent excessive hole doping hinder its use as a semiconductor material in TFT devices. In this study, we propose a doping approach through soft chemical solution process and transparent p-type Zn-doped CuI semiconductor for high-performance TFTs and circuits. The optimised TFTs annealed at 80°C exhibit a high hole mobility of over 5 cm 2 V −1 s −1 and high on/off current ratio of~10 7 with good operational stability and reproducibility. The CuI:Zn semiconductors show intrinsic advantages for next-generation TFT applications and wider applications in optoelectronics and energy conversion/storage devices. This study paves the way for the realisation of transparent, flexible, and large-area integrated circuits combined with n-type metal-oxide semiconductor.
Understanding the sensing mechanism in organic chemical sensors is essential for improving the sensing performance such as detection limit, sensitivity, and other response/recovery time, selectivity, and reversibility for real applications. Here, we report a highly sensitive printed ammonia (NH) gas sensor based on organic thin film transistors (OTFTs) with fluorinated difluorobenzothiadiazole-dithienosilole polymer (PDFDT). These sensors detected NH down to 1 ppm with high sensitivity (up to 56%) using bar-coated ultrathin (<4 nm) PDFDT layers without using any receptor additives. The sensing mechanism was confirmed by cyclic voltammetry, hydrogen/fluorine nuclear magnetic resonance, and UV/visible absorption spectroscopy. PDFDT-NH interactions comprise hydrogen bonds and electrostatic interactions between the PDFDT polymer backbone and NH gas molecules, thus lowering the highest occupied molecular orbital levels, leading to hole trapping in the OTFT sensors. Additionally, density functional theory calculations show that gaseous NH molecules are captured via cooperation of fluorine atoms and dithienosilole units in PDFDT. We verified that incorporation of functional groups that interact with a specific gas molecule in a conjugated polymer is a promising strategy for producing high-performance printed OTFT gas sensors.
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Many advanced materials have been developed for organic field-effect transistors (OFETs) or thin-film transistors (TFTs) based on organic and organic hybrid materials. However, although many new OFETs exhibit superior characteristic parameters (such as high mobility), most of them show nonideal performances that have strongly limited progress in the design of molecules, the understanding of transport mechanisms, and the circuit applications of OFETs. In this review, the device physics of ideal and nonideal OFETs is discussed first to understand the factors that limit effective mobility in semiconducting channels, distort the potential distribution, or reduce the drift electric field. Then, recent advances in optimizing the material combinations, device structures, and fabrications of OFETs toward ideal transistors are discussed. Based on the good control of materials and interfaces, some new and novel concepts to utilize the nonideal properties of OFETs to build low-power circuits and integrated sensors are also discussed.
The application of organic–inorganic perovskites has recently attracted increasing interest due to their excellent optoelectronic properties. As an emerging semiconductor, the doping capability and efficiency of these materials require further clarification but have rarely been studied previously. In this study, diverse monovalent cations, Cu+, Na+, and Ag+, are incorporated into phenethylammonium tin iodide ((PEA)2SnI4) perovskite, and the resultant lattice structural variation, film properties, and thin-film transistor performance are systematically investigated by combining theoretical and experimental methods. Owing to their unique composition and octahedral unit, perovskite semiconductors possess strong ‘substitution doping tolerance’ with the aliovalent cation dopants. Theoretical studies claim that the hypothetical monovalent cation substitution on the Sn2+ B-site creates undesired vacancies and destabilizes the perovskite lattice structure. The experimental results show that the incorporated foreign aliovalent cations are not doped inside the perovskite lattice but segregated along the grain boundaries. Benefiting from the excellent hole transport property and passivation effect of copper iodide (CuI), the CuI–(PEA)2SnI4 heterostructure composite channel layers exhibit much improved film properties and device performance, including doubled field effect mobility, compared with the pristine ones.
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