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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.)

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 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.)

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.)

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.)