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The structure of molecular aggregates is crucial for charge transport and photovoltaic performance in organic solar cells (OSCs). Herein, the intermolecular interactions and aggregated structures of nonfused-ring electron acceptors (NFREAs) are precisely regulated through a halogen transposition strategy, resulting in a noteworthy transformation from a 2D-layered structure to a 3D-interconnected packing network. Based on the 3D electron transport pathway, the binary and ternary devices deliver outstanding power conversion efficiencies (PCEs) of 17.46 % and 18.24 %, respectively, marking the highest value for NFREA-based OSCs., (© 2024 Wiley-VCH GmbH.)

High performance organic solar cells (OSCs) are usually realized by using post-treatment and/or additive, which can induce the formation of metastable morphology, leading to unfavorable device stability. In terms of the industrial production, the development of high efficiency as-cast OSCs is crucially important, but it remains a great challenge to obtain appropriate active layer morphology and high power conversion efficiency (PCE). Here, efficient as-cast OSCs are constructed via introducing a new polymer acceptor PY-TPT with a high dielectric constant into the D18:L8-BO blend to form a double-fibril network morphology. Besides, the incorporation of PY-TPT enables an enhanced dielectric constant and lower exciton binding energy of active layer. Therefore, efficient exciton dissociation and charge transport are realized in D18:L8-BO:PY-TPT-based device, affording a record-high PCE of 18.60% and excellent photostability in absence of post-treatment. Moreover, green solvent-processed devices, thick-film (300 nm) devices, and module (16.60 cm 2 ) are fabricated, which show PCEs of 17.45%, 17.54%, and 13.84%, respectively. This work brings new insight into the construction of efficient as-cast devices, pushing forward the practical application of OSCs., (© 2024 Wiley‐VCH GmbH.)

Achieving desirable charge-transport highway is of vital importance for high-performance organic solar cells (OSCs). Here, it is shown how molecular packing arrangements can be regulated via tuning the alkyl-chain topology, thus resulting in a 3D network stacking and highly interconnected pathway for electron transport in a simple-structured nonfused-ring electron acceptor (NFREA) with branched alkyl side-chains. As a result, a record-breaking power conversion efficiency of 17.38% (certificated 16.59%) is achieved for NFREA-based devices, thus providing an opportunity for constructing low-cost and high-efficiency OSCs., (© 2024 Wiley‐VCH GmbH.)

In the development of high-performance organic solar cells (OSCs), the self-organization of organic semiconductors plays a crucial role. This study focuses on the precisely manipulation of molecular assemble via tuning alkyl side-chain topology in a series of low-cost nonfused-ring electron acceptors (NFREAs). Among the three NFREAs investigated, DPA-4, which possesses an asymmetric alkyl side-chain length, exhibits a tight packing in the crystal and high crystallinity in the film, contributing to improved electron mobility and favorable film morphology for DPA-4. As a result, the OSC device based on DPA-4 achieves an excellent power conversion efficiency of 16.67 %, ranking among the highest efficiencies for NFREA-based OSCs., (© 2024 Wiley-VCH GmbH.)

Developing an artificial visual sensory system requires optoelectronic materials and devices that can mimic the behavior of biological synapses. Organic/polymeric semiconductors have emerged as promising candidates for optoelectronic synapses due to their tunable optoelectronic properties, mechanic flexibility, and biological compatibility. In this review, we discuss the recent progress in organic optoelectronic synaptic materials and devices, including their design principles, working mechanisms, and applications. We also highlight the challenges and opportunities in this field and provide insights into potential applications of these materials and devices in next-generation artificial visual systems. By leveraging the advances in organic optoelectronic materials and devices, we can envision its future development in artificial intelligence., (© 2023 Wiley-VCH GmbH.)

The development of high-efficiency thickness-insensitive organic solar cells (OSCs) is crucially important for the mass production of solar panels. However, increasing the active layer thickness usually induces a substantial loss in efficiency. Herein, a ternary strategy in which an oligomer DY-TF is incorporated into PM6:L8-BO system as a guest component is adopted to break this dilemma. The S···F intramolecular noncovalent interactions in the backbone endow DY-TF with a high planarity. Upon the addition of DY-TF, the crystallinity of the blend is effectively improved, leading to increased charge carrier mobility, which is highly desirable in the fabrication of thick-film devices. As a result, thin-film PM6:L8-BO:DY-TF-based device (110 nm) shows a power conversion efficiency (PCE) of 19.13%. Impressively, when the active layer thickness increases to 300 nm, an efficiency of 18.23% (certified as 17.8%) is achieved, representing the highest efficiency reported for 300 nm thick OSCs thus far. Additionally, blade-coated thick device (300 nm) delivers a promising PCE of 17.38%. This work brings new insights into the construction of efficient OSCs with high thickness tolerance, showing great potential for roll-to-roll printing of large-area solar cells., (© 2023 Wiley-VCH GmbH.)

Semi-transparent organic solar cells (ST-OSCs) have great potential for application in vehicle- or building-integrated solar energy harvesting. Ultrathin active layers and electrodes are typically utilized to guarantee high power conversion efficiency (PCE) and high average visible transmittance (AVT) simultaneously; however, such ultrathin parts are unsuitable for industrial high-throughput manufacturing. In this study, ST-OSCs are fabricated using a longitudinal through-hole architecture to achieve functional region division and to eliminate the dependence on ultrathin films. A complete circuit that vertically corresponds to the silver grid is responsible for obtaining high PCE, and the longitudinal through-holes embedded in it allow most of the light to pass through,where the overall transparency is associated with the through-hole specification rather than the thicknesses of active layer and electrode. Excellent photovoltaic performance over a wide range of transparency (9.80-60.03%), with PCEs ranging from 6.04% to 15.34% is achieved. More critically, this architecture allows printable 300-nm-thick devices to achieve a record-breaking light utilization efficiency (LUE) of 3.25%, and enables flexible ST-OSCs to exhibit better flexural endurance by dispersing the extrusion stress into the through-holes. This study paves the way for fabricating high-performance ST-OSCs and shows great promise for the commercialization of organic photovoltaics., (© 2023 Wiley-VCH GmbH.)

Although all-polymer solar cells (all-PSCs) show great commercialization prospects, their power conversion efficiencies (PCEs) still fall behind their small molecule acceptor-based counterparts. In all-polymer blends, the optimized morphology and high molecular ordering are difficult to achieve since there is troublesome competition between the crystallinity of the polymer donor and acceptor during the film-formation process. Therefore, it is challenging to improve the performance of all-PSCs. Herein, a ternary strategy is adopted to modulate the morphology and the molecular crystallinity of an all-polymer blend, in which PM6:PY-82 is selected as the host blend and PY-DT is employed as a guest component. Benefiting from the favorable miscibility of the two acceptors and the higher regularity of PY-DT, the ternary matrix features a well-defined fibrillar morphology and improved molecular ordering. Consequently, the champion PM6:PY-82:PY-DT device produces a record-high PCE of 18.03%, with simultaneously improved open-circuit voltage, short-circuit current and fill factor in comparison with the binary devices. High-performance large-area (1 cm 2 ) and thick-film (300 nm) all-PSCs are also successfully fabricated with PCEs of 16.35% and 15.70%, respectively.Moreover, 16.5 cm 2 organic solar module affords an encouraging PCE of 13.84% when using the non-halogenated solvent , showing the great potential of "Lab-to-Fab" transition of all-PSCs., (© 2022 Wiley-VCH GmbH.)

The development of organic solar cells (OSCs) with thick active layers is of crucial importance for the roll-to-roll printing of large-area solar panels. Unfortunately, increasing the active layer thickness usually results in a significant reduction in efficiency. Herein, we fabricated efficient thick-film OSCs with an active layer consisting of one polymer donor and two non-fullerene acceptors. The two acceptors were found to possess enlarged exciton diffusion length in the mixed phase, which is beneficial to exciton generation and dissociation. Additionally, layer by layer approach was employed to optimize the vertical phase separation. Benefiting from the synergetic effects of enlarged exciton diffusion length and graded vertical phase separation, an efficiency of 17.31% (certified value of 16.9%) is obtained for the 300 nm-thick OSC, with a short-circuit current density of 28.36 mA cm -2 , and a high fill factor of 73.0%. Moreover, the device with an active layer thickness of 500 nm also shows an efficiency of 15.21%. This work provides valuable insights into the fabrication of OSCs with thick active layers., (© 2022. The Author(s).)

The power conversion efficiencies (PCEs) of small molecule acceptor (SMA)-based organic solar cells have already exceeded 18%. However, the development of polymer acceptors still lags far behind their SMA counterparts mainly due to the lack of efficient polymer acceptors. Herein, a series of polymer acceptors named PY-X (with X being the branched alkyl chain) are designed and synthesized by employing the same central core with the SMA L8-BO but with different branched alkyl chains on the pyrrole motif. It is found that the molecular packing of SMA-HD featuring 2-hexyldecyl side chain used in the synthesis of PY-HD is similar to L8-BO, in which the branched alkyl chains lead to condensed and high-order molecular assembly in SMA-HD molecules. When combined with PM6, PY-HD-based all polymer solar cell (all-PSC) exhibits a high PCE of 16.41%, representing the highest efficiency for the binary all-PSCs. Moreover, the side-chain modification on the pyrrole site position further improves the performance of the all-PSCs, and the PY-DT-based device delivers a new record high efficiency of 16.76% (certified as 16.3%). The work provides new insights for understanding the structure-property relationship of polymer acceptors and paves a feasible avenue to develop efficient conjugated polymer acceptors., (© 2022 Wiley-VCH GmbH.)

The ternary strategy, introducing a third component into a binary blend, opens a simple and promising avenue to improve the power conversion efficiency (PCE) of organic solar cells (OSCs). The judicious selection of an appropriate third component, without sacrificing the photocurrent and voltage output of the OSC, is of significant importance in ternary devices. Herein, highly efficient OSCs fabricated using a ternary approach are demonstrated, wherein a novel non-fullerene acceptor L8-BO-F is designed and incorporated into the PM6:BTP-eC9 blend. The three components show complementary absorption spectra and cascade energy alignment. L8-BO-F and BTP-eC9 are found to form a homogeneous mixed phase, which improves the molecular packing of both the donor and acceptor materials, and optimizes the ternary blend morphology. Moreover, the addition of L8-BO-F into the binary blend suppresses the non-radiative recombination, thus leading to a reduced voltage loss. Consequently, concurrent increases in open-circuit voltage, short-circuit current, and fill factor are realized, resulting in an unprecedented PCE of 18.66% (certified value of 18.2%), which represents the highest efficiency values reported for both single-junction and tandem OSCs so far., (© 2021 Wiley-VCH GmbH.)

Compared with inorganic or perovskite solar cells, the relatively large non-radiative recombination voltage losses (ΔV non-rad ) in organic solar cells (OSCs) limit the improvement of the open-circuit voltage (V oc ). Herein, OSCs are fabricated by adopting two pairs of D-π-A polymers (PBT1-C/PBT1-C-2Cl and PBDB-T/PBDB-T-2Cl) as electron donors and a wide-bandgap molecule BTA3 as the electron acceptor. In these blends, a charge-transfer state energy (E CT ) as high as 1.70-1.76 eV is achieved, leading to small energetic differences between the singlet excited states and charge-transfer states (ΔE CT ≈ 0.1 eV). In addition, after introducing chlorine atoms into the π-bridge or the side chain of benzodithiophene (BDT) unit, electroluminescence external quantum efficiencies as high as 1.9 × 10 -3 and 1.0 × 10 -3 are realized in OSCs based on PBTI-C-2Cl and PBDB-T-2Cl, respectively. Their corresponding ΔV non-rad are 0.16 and 0.17 V, which are lower than those of OSCs based on the analog polymers without a chlorine atom (0.21 and 0.24 V for PBT1-C and PBDB-T, respectively), resulting in high V oc of 1.3 V. The ΔV non-rad of 0.16 V and V oc of 1.3 V achieved in PBT1-C-2Cl:BTA3 OSCs are thought to represent the best values for solution-processed OSCs reported in the literature so far., (© 2020 Wiley-VCH GmbH.)

The energy offset, considered as the driving force for charge transfer between organic molecules, has significant effects on both charge separation and charge recombination in organic solar cells. Herein, we designed material systems with gradually shifting energy offsets, including both positive and negative values. Time-resolved spectroscopy was used to monitor the charge dynamics within the bulk heterojunction. It is striking to find that there is still charge transfer and charge generation when the energy offset reached -0.10 eV (ultraviolet photoelectron spectroscopy data). This work not only indicates the feasibility of the free carrier generation and the following charge separation under the condition of a negative offset but also elucidates the relationship between the charge transfer and the energy offset in the case of polymer chlorination.

Morphological stability is crucially important for the long-term stability of polymer solar cells (PSCs). Many high-efficiency PSCs suffer from metastable morphology, resulting in severe device degradation. Here, a series of copolymers is developed by manipulating the content of chlorinated benzodithiophene-4,8-dione (T1-Cl) via a random copolymerization approach. It is found that all the copolymers can self-assemble into a fibril nanostructure in films. By altering the T1-Cl content, the polymer crystallinity and fibril width can be effectively controlled. When blended with several nonfullerene acceptors, such as TTPTT-4F, O-INIC3, EH-INIC3, and Y6, the optimized fibril interpenetrating morphology can not only favor charge transport, but also inhibit the unfavorable molecular diffusion and aggregation in active layers, leading to excellent morphological stability. The work demonstrates the importance of optimization of fibril network morphology in realizing high-efficiency and ambient-stable PSCs, and also provides new insights into the effect of chemical structure on the fibril network morphology and photovoltaic performance of PSCs., Competing Interests: The authors declare no conflict of interest., (© 2020 The Authors. Published by WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim.)

Ternary organic solar cells are promising alternatives to the binary counterpart due to their potential in achieving high performance. Although a growing number of ternary organic solar cells are recently reported, less effort is devoted to morphology control. Here, ternary organic solar cells are fabricated using a wide-bandgap polymer PBT1-C as the donor, a crystalline fused-ring electron acceptor ITIC-2Cl, and an amorphous fullerene derivative indene-C 60 bisadduct (ICBA) as the acceptor. It is found that ICBA can disturb π-π interactions of the crystalline ITIC-2Cl molecules in ternary blends and then help to form more uniform morphology. As a result, incorporation of 20% ICBA in the PBT1-C:ITIC-2Cl blend enables efficient charge dissociation, negligible bimolecular recombination, and balanced charge carrier mobilities. An impressive power conversion efficiency (PCE) of 13.4%, with a high fill factor (FF) of 76.8%, is eventually achieved, which represents one of the highest PCEs reported so far for organic solar cells. The results manifest that the adoption of amorphous fullerene acceptor is an effective approach to optimizing the ternary blend morphology and thereby increases the solar cell performance., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A novel nonconjugated polymer named poly(2-acrylamido-2-methyl-1-propanesulfonic acid sodium salt) (PAMPS-Na) was designed and synthesized. The PAMPS-Na has good solubility in polar solvents, such as water, methanol, and ethanol, which can be used as the cathode buffer layer in organic solar cells (OSCs) through solution processing without damaging the underlying active layer. Moreover, it was found that PAMPS-Na can significantly decrease the Al work function when it was modified with Al. To reveal its universal application in organic photovoltaic devices, a variety of photovoltaic donor materials, including two medium-band gap polymers, a wide-band gap polymer, and a small molecule donor were employed to fabricate OSCs. Compared with OSCs with Ca/Al electrode, the devices based on PAMPS-Na/Al exhibited higher photovoltaic performance, mainly because of the increased short-circuit current. Additionally, OSCs with PAMPS-Na/Al displayed better ambient stability than devices with Ca/Al. It is also interesting to find that the performance of the devices can tolerate a wide change of PAMPS-Na's thickness, enabling the potential for large-scale fabrication of OSCs. The results suggest that PAMPS-Na is a promising candidate as the cathode buffer layer to improve the efficiency and stability of OSCs.

The past decade has witnessed significant advances in the field of organic solar cells (OSCs). Ongoing improvements in the power conversion efficiency of OSCs have been achieved, which were mainly attributed to the design and synthesis of novel conjugated polymers with different architectures and functional moieties. Among various conjugated polymers, the development of wide-bandgap (WBG) polymers has received less attention than that of low-bandgap and medium-bandgap polymers. Here, we briefly summarize recent advances in WBG polymers and their applications in organic photovoltaic (PV) devices, such as tandem, ternary, and non-fullerene solar cells. Addtionally, we also dissuss the application of high open-circuit voltage tandem solar cells in PV-driven electrochemical water dissociation. We mainly focus on the molecular design strategies, the structure-property correlations, and the photovoltaic performance of these WBG polymers. Finally, we extract empirical regularities and provide invigorating perspectives on the future development of WBG photovoltaic materials., (© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Tungsten oxide as an alternative to conventional acidic PEDOT:PSS has attracted much attention in organic solar cells (OSCs). However, the vacuum-processed WO 3 layer and high-temperature sol-gel hydrolyzed WO X are incompatible with large-scale manufacturing of OSCs. Here, we report for the first time that a specific tungsten oxide WO 2.72 (W 18 O 49 ) nanowire can function well as the anode buffer layer. The nw-WO 2.72 film exhibits a high optical transparency. The power conversion efficiency (PCE) of OSCs based on three typical polymer active layers PTB7:PC 71 BM, PTB7-Th:PC 71 BM, and PDBT-T1:PC 71 BM with nw-WO 2.72 layer were improved significantly from 7.27 to 8.23%, from 8.44 to 9.30%, and from 8.45 to 9.09%, respectively compared to devices with PEDOT:PSS. Moreover, the photovoltaic performance of OSCs based on small molecule p-DTS(FBTTh 2 ) 2 :PC 71 BM active layer was also enhanced with the incorporation of nw-WO 2.72 . The enhanced performance is mainly attributed to the improved short-circuit current density (J sc ), which benefits from the oxygen vacancies and the surface apophyses for better charge extraction. Furthermore, OSCs based on nw-WO 2.72 show obviously improved ambient stability compared to devices with PEDOT:PSS layer. The results suggest that nw-WO 2.72 is a promising candidate for the anode buffer layer materials in organic solar cells.

A novel polymer donor (PBDTS-Se) is designed to match with a non-fullerene acceptor (SdiPBI-S). The corresponding solar cells show a high efficiency of 8.22%, which result from synergetic improvements of light harvesting, charge carrier transport and collection, and morphology. The results indicate that rational design of novel donor materials is important for non-fullerene organic solar cells.

A novel perylene bisimide (PBI) dimer-based acceptor material, SdiPBI-S, was developed. Conventional bulk-heterojunction (BHJ) solar cells based on SdiPBI-S and the wide-band-gap polymer PDBT-T1 show a high power conversion efficiency (PCE) of 7.16% with a high open-circuit voltage of 0.90 V, a high short-circuit current density of 11.98 mA/cm(2), and an impressive fill factor of 66.1%. Favorable phase separation and balanced carrier mobilites in the BHJ films account for the high photovoltaic performance. The results demonstrate that fine-tuning of PBI-based materials is a promising way to improve the PCEs of non-fullerene BHJ organic solar cells.