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Abstract Advances in organic materials manufacturing have enabled the creation of electronic devices using solution‐processing techniques by employing soluble materials with high conductivity grade. In this exploratory study, the use of micro‐contact for poly(3,4‐ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) polymer ink deposition as high‐quality structured electrodes for organic field‐effect transistors (OFETs) in top‐contact geometry is demonstrated. The optimized OFET's solution‐processed fabrication is a promising strategy to be realized in the simple, cost‐effective roll‐to‐roll manufacturing processes. The electrical performance of the fabricated devices is comparable to transistors with gold electrodes prepared via vacuum deposition, and even exceeding the values of the charge carriers’ mobilities and featuring lower contact resistance (Rc), due to lower charge‐carrier injection barrier for carbon‐based organic electrodes. An addition of multi‐walled carbon nanotubes to the PEDOT:PSS decreases Rc even further, changing the work function for better energy alignment with semiconductor materials.

This review explores the growing interest in 2D layered materials, such as graphene, h-BN, transition metal dichalcogenides (TMDs), and black phosphorus (BP), with a specific focus on recent advances in strain engineering. Both experimental and theoretical results are delved into, highlighting the potential of strain to modulate physical properties, thereby enhancing device performance. Various strain engineering methods are summarized, and the impact of strain on the electrical, optical, magnetic, thermal, and valleytronic properties of 2D materials is thoroughly examined. Finally, the review concludes by addressing potential applications and challenges in utilizing strain engineering for functional devices, offering valuable insights for further research and applications in optoelectronics, thermionics, and spintronics., (© 2024 Wiley‐VCH GmbH.)

The next-generation X-ray detectors require novel semiconductors with low material/fabrication cost, excellent X-ray response characteristics, and robust operational stability. The family of organic-inorganic hybrid perovskites (OIHPs) materials comprises a range of crystal configuration (i.e., films, wafers, and single crystals) with tunable chemical composition, structures, and electronic properties, which can perfectly meet the multiple-stringent requirements of high-energy radiation detection, making them emerging as the cutting-edge candidate for next-generation X-ray detectors. From the perspective of molecular dimensionality, the physicochemical and optoelectronic characteristics of OIHPs exhibit dimensionality-dependent behavior, and thus the structural dimensionality is recognized as the key factor that determines the device performance of OIHPs-based X-ray detectors. Nevertheless, the correlation between dimensionality of OIHPs and performance of their X-ray detectors is still short of theoretical guidance, which become a bottleneck that impedes the development of efficient X-ray detectors. In the review, the advanced studies on the dimensionality engineering of OIHPs are critically assessed in X-ray detection application, discussing the current understanding on the "dimensionality-property" relationship of OIHPs and the state-of-the-art progresses on the dimensionality-engineered OIHPs-based X-ray detector, and highlight the open challenges and future outlook of this field., (© 2023 Wiley‐VCH GmbH.)

The experimental replicability of highly efficient perovskite solar cells (PSCs) is a persistent challenge faced by laboratories worldwide. Although trace impurities in raw materials can impact the experimental reproducibility of high-performance PSCs, the in situ study of how trace impurities affect perovskite film growth is never investigated. Here, light is shed on the impact of inevitable water contamination in lead iodide (PbI 2 ) on the replicability of device performance, mainly depending on the synthesis methods of PbI 2 . Through synchrotron-based structure characterization, it is uncovered that even slight additions of water to PbI 2 accelerate the crystallization process in the perovskite layer during annealing. However, this accelerated crystallization also results in an imbalance of charge-carrier mobilities, leading to a degradation in device performance and reduced longevity of the solar cells. It is also found that anhydrous PbI 2 promotes a homogenous nucleation process and improves perovskite film growth. Finally, the PSCs achieve a remarkable certified power conversion efficiency of 24.3%. This breakthrough demonstrates the significance of understanding and precisely managing the water content in PbI 2 to ensure the experimental replicability of high-efficiency PSCs., (© 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

A novel donor-acceptor dyad, 4, in which the conjugated oligothiophene donor is covalently connected to fullerene PC 71 BM by a flexible alkyl ester linker, is synthesized and applied as photoactive layer in solution-processed single-material organic solar cells (SMOSCs). Excellent photovoltaic performance, including a high short-circuit current density (J SC ) of 13.56 mA cm -2 , is achieved, leading to a power conversion efficiency of 5.34% in an inverted cell architecture, which is substantially increased compared to other molecular single materials. Furthermore, dyad 4-based SMOSCs display excellent stability maintaining 96% of the initial performance after 750 h (one month) of continuous illumination and operation under simulated AM 1.5G irradiation. These results will strengthen the rational molecular design to further develop SMOSCs for potential industrial application., (© 2021 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

Understanding the conformation effect on molecular packing, miscibility, and photovoltaic performance is important to open a new avenue for small-molecule acceptor (SMA) design. Herein, two novel acceptor-(donor-acceptor1-donor)-acceptor (A-DA1D-A)-type asymmetric SMAs are developed, namely C-shaped BDTP-4F and S-shaped BTDTP-4F. The BDTP-4F-based polymer solar cells (PSCs) with PM6 as donor, yields a power conversion efficiency (PCE) of 15.24%, significantly higher than that of the BTDTP-4F-based device (13.12%). The better PCE for BDTP-4F-based device is mainly attributed to more balanced charge transport, weaker bimolecular recombination, and more favorable morphology. Additionally, two traditional A-D-A-type SMAs (IDTP-4F and IDTTP-4F) are also synthesized to investigate the conformation effect on morphology and device performance. Different from the device result above, here, IDTP-4F with S-shape conformation outperforms than IDTTP-4F with C-shape conformation. Importantly, it is found that for these two different types of SMA, the better performing binary blend has similar morphological characteristics. Specifically, both PM6:BDTP-4F and PM6:IDTP-4F blend exhibit perfect nanofibril network structure with proper domain size, obvious face-on orientation and enhance donor-acceptor interactions, thereby better device performance. This work indicates tuning molecular conformation plays pivotal role in morphology and device effciciency, shining a light on the molecular design of the SMAs., (© 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

In the field of all-polymer solar cells (all-PSCs), all efficient polymer acceptors that exhibit efficiencies beyond 8% are based on either imide or dicyanoethylene. To boost the development of this promising solar cell type, creating novel electron-deficient units to build high-performance polymer acceptors is critical. A novel electron-deficient unit containing B←N bonds, namely, BNIDT, is synthesized. Systematic investigation of BNIDT reveals desirable properties including good coplanarity, favorable single-crystal structure, narrowed bandgap and downshifted energy levels, and extended absorption profiles. By copolymerizing BNIDT with thiophene and 3,4-difluorothiophene, two novel conjugated polymers named BN-T and BN-2fT are developed, respectively. It is shown that these polymers possess wide absorption spectra covering 350-800 nm, low-lying energy levels, and ambipolar film-transistor characteristics. Using PBDB-T as the donor and BN-2fT as the acceptor, all-PSCs afford an encouraging efficiency of 8.78%, which is the highest for all-PSCs excluding the devices based on imide and dicyanoethylene-type acceptors. Considering that the structure of BNIDT is totally different from these classical units, this work opens up a new class of electron-deficient unit for constructing efficient polymer acceptors that can realize efficiencies beyond 8% for the first time., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A new class of subnaphthalocyanines bearing various peripheral and axial substituents have been synthesized for use as electron acceptors in solution-processed bulk-heterojunction polymer solar cells. The resulting solar cells exhibit modest photovoltaic performance with contributions from both the polymer donor and subnaphthalocyanine acceptor to the photocurrent., (© 2018 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.)

The photoactive layer of bulk-heterojunction organic solar cells, in a thickness range of tens to hundreds of nanometers, comprises phase-separated electron donors and acceptors after solution casting. The component distribution in the cross-section of these thin films is found to be heterogeneous, with electron donors or acceptors accumulated or depleted near the electrode interfaces. This vertical stratification of the photovoltaic blend influences device metrics through its impact on charge transport and recombination, and consequently plays an important role in determining the power conversion efficiency of photovoltaic devices. Here, different techniques, e.g., surface analysis and sputter-assisted depth-profiling, reflectivity modeling, and 3D imaging, that have been employed to characterize vertical stratification in bulk-heterojunction photovoltaic blends are reviewed. The origins of vertical stratification are summarized, including thermodynamics, kinetics, surface free energy, and selective dissolubility. The impact of correct and wrong vertical stratification to device metrics of solar cells are highlighted. Examples are then given to demonstrate how desired vertical stratification can be controlled with properly aligned device architecture to enable solar cells with high efficiency., (© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)