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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. Exciton diffusion length and graded vertical phase separation of the active layer play a critical role in the realization of high-performance thick-film organic solar cells (OSCs). Here, authors demonstrated OSCs with an efficiency of 17.31%, with an active layer thickness of around 300 nm.

Morphology control in laboratory and industry setting remains as a major challenge for organic solar cells (OSCs) due to the difference in film-drying kinetics between spin coating and the printing process. A two-step sequential deposition method is developed to control the active layer morphology. A conjugated polymer that self-assembles into a well-defined fibril structure is used as the first layer, and then a non-fullerene acceptor is introduced into the fibril mesh as the second layer to form an optimal morphology. A benefit of the combined fibril network morphology and non-fullerene acceptor properties was that a high efficiency of 16.5% (certified as 16.1%) was achieved. The preformed fibril network layer and the sequentially deposited non-fullerene acceptor form a robust morphology that is insensitive to the polymer batches, solving a notorious issue in OSCs. Such progress demonstrates that the utilization of polymer fibril networks in a sequential deposition process is a promising approach towards the fabrication of high-efficiency OSCs. Reliably controlling the morphology in organic solar cells is desired for up-scaling. Here Weng et al. combine the advantages of the fibril network donor and the state of the art Y6 acceptor in a two-step approach to deliver a high efficiency of 16% without batch-to-batch variation.

Developing active-layer systems with both high performance and mechanical robustness is a crucial step towards achieving future commercialization of flexible and stretchable organic solar cells (OSCs). Herein, we design and synthesize a series of acceptors BTA-C6, BTA-E3, BTA-E6, and BTA-E9, featuring the side chains of hexyl, and 3, 6, and 9 carbon-chain with ethyl ester end groups respectively. Benefiting from suitable phase separation and vertical phase distribution, the PM6:BTA-E3-based OSCs processed by o -xylene exhibit lower energy loss and improved charge transport characteristic and achieve a power conversion efficiency of 19.92% (certified 19.57%), which stands as the highest recorded value in binary OSCs processed by green solvents. Moreover, due to the additional hydrogen-bonding provided by ethyl ester side chain, the PM6:BTA-E3-based active-layer systems achieve enhanced stretchability and thermal stability. Our work reveals the significance of dynamic hydrogen-bonding in improving the photovoltaic performance, mechanical robustness, and morphological stability of OSCs. Developing high-performance and mechanically robust active-layer systems is crucial to commercializing flexible organic solar cells. Here, authors design small molecule acceptors with ethyl ester side chains and achieve certified efficiency of over 19% for mechanically robust devices.

Layer-by-layer (LbL) strategy has been developed to form bulk heterojunction (BHJ) structure for processing efficient organic solar cells (OSCs). Herein, LbL slot-die coating with twin boiling point solvents (TBPS) strategy was developed to fabricate highly efficient OSCs, which matches with large-scale, high throughput roll-to-roll (R2R) industrialized mass process. The TBPS strategy could produce high-quality thin film without any additive, leading to the optimized vertical phase separation with interpenetrating nanostructures, as well as the enhanced charge transport and extraction. Thus, the power conversion efficiency up to 14.42% was achieved for [(2,6-(4,8-bis(5-(2-ethylhexyl-3-fluoro)thiophen-2-yl)-benzo [1,2-b:4,5-b′]dithiophene))-alt-(5,5-(1′,3′-di-2-thienyl-5′,7′-bis(2-ethylhexyl)benzo[1′,2′-c:4′,5′-c′]dithiophene-4,8-dione)]:2,2′-((2Z,2′Z)-((12,13-bis(2-ethylhexyl)-3,9-diundecyl-12,13-dihydro-[1,2,5]thiadiazolo[3,4-e]thieno[2″,3″:4″,5″]thieno[2′,3′:4,5]pyrrolo[3,2-g]thieno[2′,3′:4,5]thieno[3,2-b]indole-2,10-diyl)bis(methanylylidene)) bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile (PM6:Y6) OSCs fabricated via sequentially LbL slot-die coating using the TBPS strategy under ambient condition. The research provides a potential route for industrialized production of high-efficiency and large-area OSC devices.

Polymer transistors are being intensively developed for next-generation flexible electronics. Blends comprising a small amount of semiconducting polymer mixed into an insulating polymer matrix have simultaneously shown superior performance and environmental stability in organic field-effect transistors compared with the neat semiconductor. Here we show that such blends actually perform very poorly in the undoped state, and that mobility and on/off ratio are improved dramatically upon moderate doping. Structural investigations show that these blend layers feature nanometre-scale semiconductor domains and a vertical composition gradient. This particular morphology enables a quasi three-dimensional spatial distribution of semiconductor pathways within the insulating matrix, in which charge accumulation and depletion via a gate bias is substantially different from neat semiconductor, and where high on-current and low off-current are simultaneously realized in the stable doped state. Adding only 5 wt% of a semiconducting polymer to a polystyrene matrix, we realized an environmentally stable inverter with gain up to 60. Blends of different polymer compounds are widely used for organic field-effect transistors. Here, Neher and colleagues show that moderate carrier doping is important to achieve maximum performance in blends of insulating and semiconducting polymers.

In organic solar cells (OSCs), which represent a quintessential application system for organic conjugated films, the intrinsic light reflection of these films significantly influences the optical performance of the devices through the Fabry–Pérot micro-cavity effect. However, this phenomenon has not been comprehensively investigated. This study demonstrates that the film’s intrinsic reflection arises from the light-matter interaction, which is mainly governed by the polarizability of delocalized electron cloud and the orientation of the conjugated backbone. Furthermore, the multi-level interference within the OSC micro-cavity leads to a dependence of both the reflection properties and the short-circuit current density ( J SC ) on the active layer thickness. Based on these insights, a strategy for synergistic optimization of device performance through precise tailoring of optical constants and the micro-cavity structure is proposed. By systematically analyzing the intrinsic reflection behavior of organic conjugated films, this study enhances the understanding of the role reflection plays in the performance of photovoltaic devices and provides theoretical support for further optical optimization of organic photovoltaics. The intrinsic light reflection of organic conjugated films significantly influences the optical performance of devices through Fabry–Pérot micro-cavity effect. Here, authors modulate cell micro cavity via tuning materials’ refractive index to improve photovoltaic performance of organic solar cells.

HighlightsAlkyl-tailored Y-SMAs named YR-SeNF series with near-infrared absorption, different molecular crystallinity and self-assembly abilities are developed.The related organic solar cells (OSCs) with an active layer processed from halogen-free solvents and spin-coating-free technologies achieve a ~ 19% efficiency.Ternary OSCs offer a robust operating stability under MPP tracking and well-keep > 80% of the initial efficiency for even over 400 h.Power-conversion-efficiencies (PCEs) of organic solar cells (OSCs) in laboratory, normally processed by spin-coating technology with toxic halogenated solvents, have reached over 19%. However, there is usually a marked PCE drop when the blade-coating and/or green-solvents toward large-scale printing are used instead, which hampers the practical development of OSCs. Here, a new series of N-alkyl-tailored small molecule acceptors named YR-SeNF with a same molecular main backbone are developed by combining selenium-fused central-core and naphthalene-fused end-group. Thanks to the N-alkyl engineering, NIR-absorbing YR-SeNF series show different crystallinity, packing patterns, and miscibility with polymeric donor. The studies exhibit that the molecular packing, crystallinity, and vertical distribution of active layer morphologies are well optimized by introducing newly designed guest acceptor associated with tailored N-alkyl chains, providing the improved charge transfer dynamics and stability for the PM6:L8-BO:YR-SeNF-based OSCs. As a result, a record-high PCE approaching 19% is achieved in the blade-coating OSCs fabricated from a green-solvent o-xylene with high-boiling point. Notably, ternary OSCs offer robust operating stability under maximum-power-point tracking and well-keep > 80% of the initial PCEs for even over 400 h. Our alkyl-tailored guest acceptor strategy provides a unique approach to develop green-solvent and blade-coating processed high-efficiency and operating stable OSCs, which paves a way for industrial development.

Organic solar cells (OSCs) have attracted extensive attention from both academia and industry in recent years due to their remarkable improvement in power conversion efficiency (PCE). However, the Golden Triangle (the balance of efficiency‐stability‐cost) required for large‐scale industrialization of OSCs still remains a great challenge. Here, a new nonfused‐ring electron acceptor (NFREA) BF and its polymerized counterpart PBF were designed and synthesized, and their photovoltaic performance, storage stability and material cost were systematically investigated. When blended with a widely‐used polymer donor PBDB‐T, the PBF ‐based all‐polymer solar cell (all‐PSC) displayed a record high PCE of 12.61% for polymerized NFREAs (PNFREAs) with an excellent stability (95.2% of initial PCE after 800 h storage), superior to the BF counterpart. Impressively, PBF ‐based all‐PSC possesses the highest industrial figure‐of‐merit (i‐FOM) value of 0.309 based on an efficiency‐stability‐cost evaluation, in comparison to several representative OSC systems (such as PM6:Y6 and PBDB‐T:PZ1). This work provides an insight into the balance of efficiency, stability, and cost, and also indicates that the PNFREAs are promising materials toward the commercial application of OSCs.

Halogenation of Y‐series small‐molecule acceptors (Y‐SMAs) is identified as an effective strategy to optimize photoelectric properties for achieving improved power‐conversion‐efficiencies (PCEs) in binary organic solar cells (OSCs). However, the effect of different halogenation in the 2D‐structured large π‐fused core of guest Y‐SMAs on ternary OSCs has not yet been systematically studied. Herein, four 2D‐conjugated Y‐SMAs (X‐QTP‐4F, including halogen‐free H‐QTP‐4F, chlorinated Cl‐QTP‐4F, brominated Br‐QTP‐4F, and iodinated I‐QTP‐4F) by attaching different halogens into 2D‐conjugation extended dibenzo[f,h]quinoxaline core are developed. Among these X‐QTP‐4F, Cl‐QTP‐4F has a higher absorption coefficient, optimized molecular crystallinity and packing, suitable cascade energy levels, and complementary absorption with PM6:L8‐BO host. Moreover, among ternary PM6:L8‐BO:X‐QTP‐4F blends, PM6:L8‐BO:Cl‐QTP‐4F obtains a more uniform and size‐suitable fibrillary network morphology, improved molecular crystallinity and packing, as well as optimized vertical phase distribution, thus boosting charge generation, transport, extraction, and suppressing energy loss of OSCs. Consequently, the PM6:L8‐BO:Cl‐QTP‐4F‐based OSCs achieve a 19.0% efficiency, which is among the state‐of‐the‐art OSCs based on 2D‐conjugated Y‐SMAs and superior to these devices based on PM6:L8‐BO host (17.70%) and with guests of H‐QTP‐4F (18.23%), Br‐QTP‐4F (18.39%), and I‐QTP‐4F (17.62%). The work indicates that halogenation in 2D‐structured dibenzo[f,h]quinoxaline core of Y‐SMAs guests is a promising strategy to gain efficient ternary OSCs. Four 2D‐conjugated guest acceptors (X‐QTP‐4F) are developed by attaching different halogens into the 2D‐structured dibenzo[f,h]quinoxaline core. Among X‐QTP‐4F, Cl‐QTP‐4F shows a higher absorption coefficient, optimized molecular packing, suitable cascade energy levels, and complementary absorption with PM6:L8‐BO host. Thus, ternary devices achieved 19% efficiency, which is among the state‐of‐the‐art devices with 2D‐structured acceptors.

Power equipment operates under high voltages, inducing space charge accumulation on the surface of key insulating structures, which increases the risk of discharge/breakdown and the possibility of maintenance workers experiencing electric shock accidents. Hence, a visualized non-equipment space charge detection method is of great demand in the power industry. Typical electrochromic phenomenon is based on redox of the material, triggered by a voltage smaller than 5 V with a continuous current in μA~mA level, which is not applicable to high electric fields above 106 V/m with pA~nA operation current in power equipment. Until now, no naked-eye observation technique has been realized for space charge detection to ensure the operation of power systems as well as the safety of maintenance workers. In this work, a viologen/poly(vinylidene fluoride-co-hexafluoropropylene)(P(VDF–HFP)) composite is investigated from gel to insulating bulk configurations to achieve high-voltage electrical-insulating electrochromism. The results show that viologen/P(VDF–HFP) composite bulk can withstand high electric fields at the 107 V/m level, and its electrochromism is triggered by space charges. This electrochromism phenomenon can be visually extended by increasing viologen content towards 5 wt.% and shows a positive response to voltage amplitude and application duration. As viologen/P(VDF–HFP) composite bulk exhibits a typical electrical insulating performance, it could be attached to the surface of insulating structures or clamped between metal and insulating materials as a space charge accumulation indicator in high-voltage power equipment.