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Pimpisut Worakajit Pinit Kidkhunthod Thanasee Thanasarnsurapong Saran Waiprasoet Hideki Nakajima Taweesak Sudyoadsuk Vinich Promarak Adisak Boonchun Pichaya Pattanasattayavong 《Advanced functional materials》2023,33(25):2209504
Solution-processed copper(I) thiocyanate (CuSCN) typically exhibits low crystallinity with short-range order; the defects result in a high density of trap states that limit the device's performance. Despite the extensive electronic applications of CuSCN, its defect properties are not understood in detail. Through X-ray absorption spectroscopy, pristine CuSCN prepared from the standard diethyl sulfide-based recipe is found to contain under-coordinated Cu atoms, pointing to the presence of SCN− vacancies. A defect passivation strategy is introduced by adding solid I2 to the processing solution. At small concentrations, the iodine is found to exist as I− which can substitute for the missing SCN− ligand, effectively healing the defective sites and restoring the coordination around Cu. Computational study results also verify this point. Applying I2-doped CuSCN as a p-channel in thin-film transistors shows that the hole mobility increases by more than five times at the optimal doping concentration of 0.5 mol.%. Importantly, the on/off current ratio and the subthreshold characteristics also improve as the I2 doping method leads to the defect-healing effect while avoiding the creation of detrimental impurity states. An analysis of the capacitance-voltage characteristics corroborates that the trap state density is reduced upon I2 addition. 相似文献
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Pimpisut Worakajit Fumiya Hamada Debashis Sahu Pinit Kidkhunthod Taweesak Sudyoadsuk Vinich Promarak David J. Harding Daniel M. Packwood Akinori Saeki Pichaya Pattanasattayavong 《Advanced functional materials》2020,30(36)
Copper(I) thiocyanate (CuSCN) is rising to prominence as a hole‐transporting semiconductor in various opto/electronic applications. Its unique combination of good hole mobility, high optical transparency, and solution‐processability renders it a promising hole‐transport layer for solar cells and p‐type channel in thin‐film transistors. CuSCN is typically deposited from sulfide‐based solutions with diethyl sulfide (DES) being the most widely used. However, little is known regarding the effects of DES on CuSCN films despite the fact that DES can coordinate with Cu(I) and result in a different coordination polymer having a distinct crystal structure when fully coordinated. Herein, the coordination of DES in CuSCN films is thoroughly investigated with a suite of characterization techniques as well as density functional theory. This study reveals that DES directly affects the microstructure of CuSCN by stabilizing the polar crystalline surfaces via the formation of strong coordination bonds. Furthermore, a simple antisolvent treatment is demonstrated to be effective at modifying the microstructure and morphology of CuSCN films. The treatment with tetrahydrofuran or acetone leads to uniform films consisting of CuSCN crystallites with high crystallinity and their surfaces passivated by DES molecules, resulting in an increase in the hole mobility from 0.01 to 0.05 cm2 V?1 s?1. 相似文献
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