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Hybrid photoanodes for water-splitting photoelectrochemical cells (WS-PECs) consist of a visible-light-absorbing semiconductor (VLASC) with a molecular water-oxidation catalyst (mWOC) attached and ...

The extension of reticular chemistry concepts to electrically conductive three-dimensional metal–organic frameworks (MOFs) has been challenging, particularly for cases in which strong interactions between electroactive linkers create the charge transport pathways. Here, we report the successful replacement of tetrathiafulvalene (TTF) with a nickel glyoximate core in a family of isostructural conductive MOFs with Mn2+, Zn2+, and Cd2+. Different coordination environments of the framework metals lead to variations in the linker stacking geometries and optical properties. Single-crystal conductivity data are consistent with charge transport along the linker stacking direction, with conductivity values only slightly lower than those reported for the analogous TTF materials. These results serve as a case study demonstrating how reticular chemistry design principles can be extended to conductive frameworks with significant intermolecular contacts., U.S. Department of Energy, Basic Energy Sciences (Grant DE-SC0018235)

The joint of the donor and acceptor moieties allows a facile and effective strategy to develop novel organic conjugated materials. However, few pieces of work report the understanding of the donor-acceptor interactions at the molecular level. Herein, we developed three small molecules containing one acceptor motif with different amounts of the donor unit. By combining theoretical calculations and energy level characterization, the lowest unoccupied molecular orbital (LUMO) levels of the three molecules were proven to be almost identical. The molecular packing modes were evaluated from crystal structure prediction. Owing to the donor-acceptor interactions, the packing mode can be tuned from a 1D slipped stacking to a 2D brick layer. The 2D molecular packing and charge transport channel endowed the materials a higher electron mobility of 3.29 cm2 V-1 s-1 in the single-crystal field-effect transistors after such modulation.

The detailed relationship between film morphology and the performance of solution processed n-type organic thermoelectric (TE) devices is investigated. It is interesting to find that the better ordered molecular packing of n-type polymer can be achieved by adding a small fraction of dopant molecules, which is not observed before. The better ordered structure will be favorable for the charge carrier mobility. Meanwhile, dopant molecules improve free carrier concentration via doping reaction. As a result, a significantly enhanced electrical conductivity (12 S cm(-1)) and power factor (25.5 μW m(-1) K(-2)) of TE devices are obtained. Furthermore, the phase separation of conjugated polymer/dopants is observed for the first time with resonant soft X-ray scattering. Our results indicate that the miscibility of conjugated polymers and dopants plays an important role on controlling the morphology and doping efficiency of TE devices.

Wafer-scale fabrication of high-performance uniform organic electronic materials is of great challenge and has rarely been realized before. Previous large-scale fabrication methods always lead to different layer thickness and thereby poor film and device uniformity. Herein, the first demonstration of 4 in. wafer-scale, uniform, and high-performance n-type polymer monolayer films is reported, enabled by controlling the multi-level self-assembly process of conjugated polymers in solution. Since the self-assembly process happened in solution, the uniform 2D polymer monolayers can be facilely deposited on various substrates, and theoretically without size limitations. Polymer monolayer transistors exhibit high electron mobilities of up to 1.88 cm2 V-1 s-1 , which is among the highest in n-type monolayer organic transistors. This method allows to easily fabricate n-type conjugated polymers with wafer-scale, high uniformity, low contact resistance, and excellent transistor performance (better than the traditional spin-coating method). This work provides an effective strategy to prepare large-scale and uniform 2D polymer monolayers, which could enable the application of conjugated polymers for wafer-scale sophisticated electronics.

p- or n-Dopants have played significant roles in the improvement of organic electronic devices through the controllable doping of organic semiconductors. However, there has been little study of air-stable n-dopants under ambient conditions with strong doping capability due to the low electron affinities of organic semiconductors. Herein, a 1,4-dihydropyridine-based derivative is designed and facilely synthesized as an efficient n-dopant. The doping process is systematically investigated by UV–vis–NIR spectroscopy in solution and ultraviolet photoelectron spectroscopy in the solid state. Excellent conductivities are obtained for a variety of doped n-type semiconductors via a simple solution process without further treatment, suggesting a broad class of 1,4-dihydropyridine derivatives could be used as n-dopants in future organic electronic devices.