Perovskites have been intensively investigated for their use in solar cells and light‐emitting diodes. However, research on their applications in thin‐film transistors (TFTs) has drawn less attention despite their high intrinsic charge carrier mobility. In this study, the universal approaches for high‐performance and reliable p‐channel lead‐free phenethylammonium tin iodide TFTs are reported. These include self‐passivation for grain boundary by excess phenethylammonium iodide, grain crystallization control by adduct, and iodide vacancy passivation through oxygen treatment. It is found that the grain boundary passivation can increase TFT reproducibility and reliability, and the grain size enlargement can hike the TFT performance, thus, enabling the first perovskite‐based complementary inverter demonstration with n‐channel indium gallium zinc oxide TFTs. The inverter exhibits a high gain over 30 with an excellent noise margin. This work aims to provide widely applicable and repeatable methods to make the gate more open for intensive efforts toward high‐performance printed perovskite TFTs.
MIL-101 and MIL-101-NH 2 were partially modified to incorporate various functional groups that are capable of forming hydrogen bonds with water. Specifically, MIL-101-NH 2 was partially functionalized with -NHCONHCH 2 CH 3 (-UR2), -NHCOCHCHCOOH (-Mal), or -NH(CH 2 ) 3 SO 3 H (-3SO 3 H) and MIL-101 was partially functionalized with -COOH in order to investigate the effect of these groups on the water sorption properties when compared to the pristine versions. The MIL-101 derivatives were synthesized by either post-synthetic modification of MIL-101-NH 2 or through direct synthesis using a mixed linker strategy. The ratios of the incorporated functional groups were determined by 1 H-NMR analyses and the porosity changes were revealed by N 2 gas adsorption measurements at 77 K. Water sorption isotherms at 298 K conclude that the incorporation of -3SO 3 H enhances the water vapour uptake capacity at a low relative pressure (P/P 0 ¼ 0.30), whereas -UR2 and -Mal retard water adsorption in MIL-101-NH 2 . The partial incorporation of -COOH in MIL-101 exhibits a steeper water uptake at lower pressure (P/P 0 ¼ 0.40) than MIL-101-NH 2 . Interestingly, a greater -COOH content within the MIL-101 framework reduces the water uptake capacity. These results indicate that even partial functionalization of MIL-101 induces noticeably large changes in the water adsorption properties.
The functionalization of UiO-67 with -NH2 groups enhances CO2 and CH4 adsorption at 1 bar and 298 K and positively influences the framework's interaction with water as evidenced by the significant enhancement of water vapour adsorption at 0.1 < P/P0 < 0.3 and 298 K.
Energy-efficient solution-processed organic field-effect transistors (OFETs) are highly sought after in the low-cost printing industry as well as for the manufacture of flexible and other next-generation devices. The fabrication of such electronic devices requires high-functioning insulating materials that are chemically and mechanically robust to avoid lowering insulating properties during the device fabrication process or utilization of devices. In this study, we report a facile, fluorinated, UV-assisted cross-linker series using a fluorophenyl azide (FPA), which reacts with the C–H groups of a conventional polymer. This demonstrates the application of the cross-linked films in OFET gate dielectrics. The effects of the cross-linkable chemical structure of the FPA series on the cross-linking chemistry, photopatternability, and dielectric properties of the resulting films are investigated for low/high-k or amorphous/crystalline polymeric gate dielectric materials. The characteristics of insulating layers and behavior of OFETs containing these cross-linked gate dielectrics (for example, leakage current density (J), hysteresis, and charge trap density) depend on the polymer type. Furthermore, an organic-based complementary inverter and various printable OFETs with excellent electrical characteristics are successfully fabricated. Thus, these reported cross-linkers that enable the solution process and patterning of well-developed conventional polymer dielectric materials are promising for the realization of a more sustainable next-generation industrial technology for flexible and printable devices.
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.
Printed electronics will be essential in the implementation of next-generation electronic devices, because printing facilitates fabrication of devices on various rigid, thin, or flexible substrates. Inkjet printing enables precise placement...
Non-fullerene acceptors (NFAs) for organic solar cells (OSCs) have significantly developed over the past five years with continuous improvements in efficiency now over 18%. However, a key challenge still remains in order to fully realize their commercialization potential: the need to extend device lifetime and to control degradation mechanisms. Herein, we investigate the effect of two different molecular engineering routes on the widely utilized ITIC NFA, to tune its optoelectronic properties and interactions with the donor polymer in photoactive blends. Heavier selenium (Se) atoms substitute sulfur (S) atoms in the NFA core in either outer or inner positions, and methyl chains are attached to the end groups. By investigating the effects of these structural modifications on the long-term operational stability of bulk-heterojunction OSC devices, we identify outer selenation as a powerful strategy to significantly increase device lifetime compared to ITIC. Combining outer selenation and methylation results in an impressive 95% of the initial OSC efficiency being retained after 450 h under operating conditions, with an exceptionally long projected half-lifetime of 5600 h compared to 400 h for ITIC. We find that the heavier and larger Se atoms at outer-core positions rigidify the molecular structure to form highly crystalline films with low conformational energetic disorder. It further enhances charge delocalization over the molecule, promoting strong intermolecular interactions among acceptor molecules. Upon methylation, this strong intermolecular interaction stabilizes acceptor domains in blends to be resilient to light-induced morphological changes, thereby leading to superior device stability. Our results highlight the crucial role of NFA molecular structure for OSC operational stability and provide important NFA design rules via heteroatom position and end-group control.
Perovskite materials have displayed remarkable performance when used in photovoltaic devices. In comparison, research on their application in thin-film transistors (TFTs) has been developing slowly. We report reliable high-performance p-channel lead-free layered perovskite phenethylammonium tin iodide TFTs using simple and easily repeatable one-step spin-coating with premixed binary solvents of N,N-dimethylformamide (DMF) and chlorobenzene (CB)/ethyl acetate (EA). CB/EA antisolvent addition facilitates nucleation and formation of films with oriented grain ripening and full coverage. The champion perovskite TFT shows a fivefold increase in the mobility (3.8 cm 2 V −1 s −1 ) and a twofold magnitude increase in the current on/off ratio (∼10 6 ) with improved bias stress stability. Using well-developed n-channel indium gallium zinc oxide TFTs, a complementary inverter with a high gain of ∼30 is demonstrated. Moreover, with efficient charge transport, transistor amplification function, and pronounced photogating properties, the optimized perovskite phototransistors show a remarkably high photodetectivity of up to 3.2 × 10 17 Jones. This simple and highly repeatable method has attracted more attention for fabricating printed high-performance perovskite TFTs and phototransistors beyond energy sector applications.
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