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Publication date: 21 April 2021

Source: Joule, Volume 5, Issue 4

Author(s): Di Wang, Haoran Liu, Yuhao Li, Guanqing Zhou, Lingling Zhan, Haiming Zhu, Xinhui Lu, Hongzheng Chen, Chang-Zhi Li

The intermolecular interaction in an all-polymer system is well modulated through incorporating a third component, resulting simultaneous enhancement of efficiency, deformability, and mechanical stability. Better mechanical stability against multiple forces in optimized ternary system is achieved through strengthening intermolecular interaction between two donors to inhibit the morphology evolution under strain.

Abstract

Promoting efficiency, deformability, and life expectancy of stretchable organic solar cells (OSCs) have always been key concerns that researchers are committed to solving. However, how to improve them simultaneously remains challenging, as morphology parameters, such as ordered molecular arrangement, beneficial for highly efficient devices actually limits mechanical stability and deformability. In this study, the unfavorable trade-off among these properties has been reconciled in an all-polymer model system utilizing a mechanically deformable guest component. The success of this strategy stems from introducing a highly ductile component without compromising the pristine optimized morphology. Preferable interaction between two donors can maintain the fiber-like structure while enhancing the photocurrent to improve efficiency. Morphology evolution detected via grazing incidence X-ray scattering and in situ UV–vis absorption spectra during stretching have verified the critical role of strengthened interaction on stabilizing morphology against external forces. The strengthened interaction also benefits thermal stability, enabling the ternary films with small efficiency degradation after heating 1500 h under 80 °C. This work highlights the effect of morphology evolution on mechanical stability and provides new insights from the view of intermolecular interaction to fabricate highly efficient, stable, and stretchable/wearable OSCs.

The operational lifetimes of UV‐absorbing organic solar cells based on contorted hexabenzocoronene (cHBC) and its derivatives are systematically investigated. In contrast to highly stable reference cells, devices based on halogenated cHBCs as acceptors show rapid degradation with development of S‐shaped J–V curves. The introduction of halogenation on cHBC can affect thin‐film morphological stability and thus device lifetime.

Abstract

Transparent photovoltaics that harvest ultraviolet photons are promising point‐of‐use power sources for lower power applications, such as electrochromic windows that regulate the flow of visible and infrared photons for lighting and temperature regulation. Organic photovoltaic cells employing contorted hexabenzocoronene (cHBC) and its derivatives as chromophores have shown promise for transparent solar cells due to their high open‐circuit voltages, large‐area scalability, and high photoactive layer transparency. Here, the operational stability of such devices is investigated and it is found that the solar cell active layers that include peripherally halogenated chromophores undergo rapid morphological degradation during operation, while control cells employing cHBC and other non‐halogenated derivatives as donors with archetype C₇₀ as an acceptor are highly stable. This study suggests halogenation of chromophores can play an outsized role in determining the operational stability of devices comprising them, which should be considered during the molecular design process.

A record efficiency of 15.24% is achieved for organic solar cells with an area of ≥1 cm² with D18:Y6 as absorber material. The optimized cell design minimizes resistive losses due to the indium tin oxide (ITO) electrode. The cell is very homogeneous and is hardly affected by shunts, as revealed by light beam‐induced current, electroluminescence, and dark lock‐in thermography imaging.

In organic photovoltaics, high power conversion efficiencies (PCE) are mostly achieved on device areas well below 0.1 cm². Herein, organic solar cells based on a D18:Y6 absorber layer on an active area of ≥ 1 cm² with a certified PCE of 15.24% are reported. The impacts of the sheet resistance of the transparent electrode and the cell design are quantified by means of full optical device simulations and an analytical electrical model. Three imaging methods (light beam‐induced current, dark lock‐in thermography, and electroluminescence [EL]) are applied and reveal a strong homogeneity of the record cell. Nevertheless, it is found that there is substantial room for improvement mostly in current but also in fill factor and that a PCE of 18.6% on ≥1 cm² is feasible with this absorber material. Further, photoluminescence (PL) and EL spectroscopy reveal that both emissions occur at the same wavelength(s) and are very similar to the PL spectrum of a pure Y6 acceptor film. The latter points strongly toward electronic coupling between the S1 states of the acceptor and the charge transfer states at the donor/acceptor interface.

Combining the layer‐by‐layer processing method and a ternary strategy, 18.16% efficiency, which is among the highest values reported to date, is achieved in single‐junction organic photovoltaics (OPVs) based on the PM6:BO‐4Cl:BTP‐S2 blend, superior to that (18.03%) of bulk‐heterojunction OPVs, proving that layer‐by‐layer processed ternary OPVs could be a promising approach to high efficiencies.

Abstract

Obtaining a finely tuned morphology of the active layer to facilitate both charge generation and charge extraction has long been the goal in the field of organic photovoltaics (OPVs). Here, a solution to resolve the above challenge via synergistically combining the layer‐by‐layer (LbL) procedure and the ternary strategy is proposed and demonstrated. By adding an asymmetric electron acceptor, BTP‐S2, with lower miscibility to the binary donor:acceptor host of PM6:BO‐4Cl, vertical phase distribution can be formed with donor‐enrichment at the anode and acceptor‐enrichment at the cathode in OPV devices during the LbL processing. In contrast, LbL‐type binary OPVs based on PM6:BO‐4Cl still show bulk‐heterojunction like morphology. The formation of the vertical phase distribution can not only reduce charge recombination but also promote charge collection, thus enhancing the photocurrent and fill factor in LbL‐type ternary OPVs. Consequently, LbL‐type ternary OPVs exhibit the best efficiency of 18.16% (certified: 17.8%), which is among the highest values reported to date for OPVs. The work provides a facile and effective approach for achieving high‐efficiency OPVs with expected morphologies, and demonstrates the LbL‐type ternary strategy as being a promising procedure in fabricating OPV devices from the present laboratory study to future industrial production.

The effect of Pd cross‐coupling catalyst traces on the physical processes in a non‐fullerene bulk‐heterojunction solar cell is investigated. The drop of the solar cell performance upon addition of systematically added amounts of tetrakis(triphenylphosphine)palladium(0) is explained by alteration of the morphology, charge carrier generation, recombination, and charge extraction.

Abstract

The effect of the cross‐coupling catalyst tetrakis(triphenylphosphine)palladium(0) (Pd(PPh₃)₄) on the performance of a model organic bulk‐heterojunction solar cell composed of a blend of poly([2,6′‐4,8‐di(5‐ethylhexylthienyl)benzo[1,2‐b;3,3‐b]dithiophene]{3‐fluoro‐2[(2‐ethylhexyl)carbonyl]thieno[3,4‐b]thiophenediyl}) (PTB7‐Th) donor and 3,9‐bis(2‐methylene‐((3‐(1,1‐dicyanomethylene)‐6,7‐difluoro)‐indanone))‐5,5,11,11‐tetrakis(4‐hexylphenyl)‐dithieno[2,3‐d:2′,3′‐d′]‐s‐indaceno[1,2‐b:5,6‐b′]dithiophene (IOTIC‐4F) non‐fullerene acceptor is investigated. The effect of intentional addition of different amounts of Pd(PPh₃)₄ on morphology, free charge carrier generation, non‐geminate bulk trap‐ and surface trap‐assisted recombination as well as bimolecular recombination and charge extraction is quantified. This work shows that free charge carrier generation is affected significantly, while the impact of Pd(PPh₃)₄ on non‐geminate recombination processes is limited because the catalyst does not facilitate efficient trap‐assisted recombination. The studied system shows substantial robustness towards the addition of Pd(PPh₃)₄ in small amounts.

Using newly developed high‐quality FlexAgNEs, flexible OPV devices are fabricated and studied with the newly emerging star acceptor Y6 and its derivatives. Comparable performance with rigid counterparts is achieved for all the tested materials. The flexible devices display superior and robust mechanical stability under extreme bending or even folding conditions. Furthermore, the mechanism underlying the super mechanical robustness of these flexible devices is thoroughly investigated.

Abstract

Among the various advantages of organic photovoltaics (OPVs), the key one is their ability to be a highly flexible renewable energy source. However, the power conversion efficiencies for flexible OPV devices still lag behind those of their rigid counterparts, and their mechanical stability cannot meet the requirements for practical applications at present. These, in particular, depend on flexible transparent electrodes (FTEs). Here, a high‐quality FTE (called FlexAgNE), with the simultaneously combined excellent characteristics, has been tested with a series of efficient active materials for flexible OPV devices, and high performance comparable with rigid counterparts has been achieved. In addition, due to the synergistic effect of FlexAgNE and the upper ZnO transport layer, including strong binding between the polyethylene terephthalate substrate and a hydrophilic polyelectrolyte (the key component of FlexAgNE), together with the capillary force effect of crossed silver nanowires and tight filling of ZnO, the flexible devices demonstrate robust mechanical stability even under extreme bending or folding conditions.

An organic photovoltaic (OPV) formulation is developed, which suggests a low synthetic complexity and a competitive figure of merit. The prepared module exhibits a maximum power conversion efficiency (PCE) of 10% when using solution‐processed material as the hole‐transporting layer and simultaneously exhibits outstanding stability, which will benefit the commercialization of highly efficient OPV products.

A scalable and accessible photoactive formulation with a low synthetic complexity (SC) index is utilized in organic photovoltaic (OPV) fabrication. The formulation readily dissolves in nonchlorinated solvents, and the corresponding photoactive films can be processed by various coating methods to fabricate devices with power conversion efficiencies (PCEs) of 16.1% and 15.2% when using vacuum‐based molybdenum oxide and solution‐processable conducting polymer as the hole transporting layer in the inverted structure, respectively. This prepared device shows superior stability under light exposure. The PCE is maintained 94% of the initial values after 1080 h of light soaking at 100 mW cm⁻². Furthermore, the figure of merit based on the ratio of the SC index and PCE indicates the benefit of this formulation for OPV manufacturing, showing the feasibility of commercialization. Eventually, a PCE of 10.3% is demonstrated for a mini‐module fabricated under ambient conditions, with an active area of 32.6 cm². To our knowledge, this PCE is one of the largest values reported to date for a green solvent and an all‐solution‐processed OPV module with an inverted architecture.

Organic solar cells (OSCs) outperform other technologies at low‐light intensities providing an exciting opportunity for commercialization. Previous OSC low‐light studies utilize non‐scalable materials or methods unsuitable for commercialization. Scalable materials are used to highlight the current performance of commercially relevant low‐light OSCs. The effect of parasitic resistance and a light‐soaking effect that is critical for low‐light performance are also investigated.

Abstract

Low‐light applications provide an exciting market opportunity for organic solar cells (OSCs). However, so far, studies have only considered OSCs of limited commercial viability. Herein, the applicability of a fully‐scalable, flexible, inverted non‐fullerene acceptor (NFA) containing OSC is demonstrated by showing its superior performance to silicon under low‐light, achieving 40 µW cm⁻² maximum power output at 1300 lx illumination. The effect of parasitic resistance and dark current on low‐light performance are identified. Furthermore, an atmosphere sensitive light‐soaking (LS) effect, critical for low‐light performance and resulting in undesirable S‐shaped current‐voltage characteristics, is analyzed. By employing different interlayers and photoactive layers (PALs) the origin of this LS effect is identified as poor electron extraction at the electron transport layer (ETL)/PAL interface when the common ETL ZnO is used. Two strategies are implemented to overcome the LS effect: replacement of ZnO with SnO₂ nanoparticles to reduce ETL sub‐gap electron trap states or tuning the NFA energy levels to optimize interfacial energetics. Finally, the commercial viability of these LS‐free devices is demonstrated by fabricating fully printed large‐area modules (21.6 cm²) achieving a maximum power output of 17.2 µW cm⁻², providing the most relevant example of the currently obtainable performance in commercial low‐light OSCs.

A dissymmetric fused‐ring acceptor BTIC‐2Cl‐γCF₃ with chlorine and trifluoromethyl end groups give a power conversion efficiency (PCE) of over 17 % which is the highest among polymer solar cells processed by halogen‐free solvents. Dissymmetric chlorination and trifluoromethylation is a practical approach towards a low band‐gap acceptor for eco‐compatible processed photovoltaic applications.

Abstract

To elevate the performance of polymer solar cells (PSC) processed by non‐halogenated solvents, a dissymmetric fused‐ring acceptor BTIC‐2Cl‐γCF₃ with chlorine and trifluoromethyl end groups has been designed and synthesized. X‐ray crystallographic data suggests that BTIC‐2Cl‐γCF₃ has a 3D network packing structure as a result of H‐ and J‐aggregations between adjacent molecules, which will strengthen its charge transport as an acceptor material. When PBDB‐TF was used as a donor, the toluene‐processed binary device realized a high power conversion efficiency (PCE) of 16.31 %, which improved to 17.12 % when PC71ThBM was added as the third component. Its efficiency of over 17 % is currently the highest among polymer solar cells processed by non‐halogenated solvents. Compared to its symmetric counterparts BTIC‐4Cl and BTIC‐CF₃‐γ, the dissymmetric BTIC‐2Cl‐γCF₃ integrates their merits, and has optimized the molecular aggregations with excellent storage and photo‐stability, and also extending the maximum absorption peak in film to 852 nm. The devices exhibit good transparency indicating a potential utilization in semi‐transparent building integrated photovoltaics (ST‐BIPV).

Publication date: 20 January 2021

Source: Joule, Volume 5, Issue 1

Author(s): Yunlong Ma, Ming Zhang, Shuo Wan, Pan Yin, Pengsong Wang, Dongdong Cai, Feng Liu, Qingdong Zheng

The photoinitiator bifunctional bis‐benzophenone is introduced into non‐fullerene solar cells as a multifunctional solid additive for the first time. The doping of this solid additive could not only modify the polymer order and firm morphology of active layer to improve device performance, but also to achieve better reproducibility, thickness insensitivity, and thermal stability for the non‐fullerene solar cells.

Abstract

Simultaneously improving efficiency and stability is critical for the commercial application of non‐fullerene acceptor polymer solar cells (NFA‐PSCs). Multifunctional solid additives have been considered as a potential route to tune the morphology of the active layer and optimize performance. In this work, photoinitiator bifunctional bis‐benzophenone (BP‐BP) is used as a solid additive, replacing solvent additives, in the PBDB‐T:ITIC NFA system. With the addition of BP‐BP, the intermolecular π–π stacking of PBDB‐T and morphology is improved, leading to more balanced carrier transport and more effective exciton dissociation. Devices fabricated with BP‐BP show a power conversion efficiency (PCE) of 11.89%, with enhanced short‐circuit current (J _sc), and fill factor (FF). Devices optimized with BP‐BP show excellent reproducibility, insensitivity to thickness, and an improved thermal stability under atmospheric conditions without encapsulation. This work provides a new strategy for the application of solid additives in NFA‐PSCs.

Herein, a comparison among all candidates to replace indium tin oxide electrodes to fabricate flexible organic solar cells (FOSCs) is discussed, while focusing on the benefits and problems of silver nanowires (AgNWs) electrodes. All progress in addressing the issues that AgNWs present, along with publications regarding the fabrication of highly efficient FOSCs based on AgNWs, are summarized.

Abstract

In this review, silver nanowires (AgNWs) are introduced, as the primary material to replace indium tin oxide for fabricating cost‐effective flexible organic solar cells (FOSCs), because of their remarkable solution‐processing, flexibility, transparency, and conductivity, along with their enhanced properties in terms of light‐scattering, plasmonic effects, and transmittance in the near infrared region. The drawbacks of AgNWs, particularly their high roughness, low adhesion to substrates, atmospheric corrosion, degradation under UV and visible light, and poor contact at wire‐wire junctions, must be resolved prior to their use in commercial FOSCs applications. Herein, comparisons among all candidates (e.g., graphene, carbon nanotubes, metal grids, and conducting polymers), along with a report of all recent progress in addressing these issues for using AgNWs as flexible transparent conductive electrodes (TCEs), are discussed. In addition, recent publications on the fabrication of highly efficient FOSCs based on AgNWs are summarized. The discussed issues regarding AgNWs‐TCEs apply not only to FOSCs, but can be generalized for other third‐generation solar cells, such as perovskite solar cells and dye‐sensitized solar cells; additionally, they provide insight for other optoelectronic applications, such as organic light‐emitting diodes, liquid crystal displays, smart windows, touch panels, and heaters.

To fine‐tune the energy levels of polymer donors, a family of random polymers is synthesized, which shows favorable properties of aggregation and morphology. The performance of these polymers is less sensitive to their molecular weights compared with PM7. Thus, multiple cases of highly efficient nonfullerene organic solar cells are achieved with efficiencies between 16.0% and 17.1%.

Abstract

Developing high‐performance donor polymers is important for nonfullerene organic solar cells (NF‐OSCs), as state‐of‐the‐art nonfullerene acceptors can only perform well if they are coupled with a matching donor with suitable energy levels. However, there are very limited choices of donor polymers for NF‐OSCs, and the most commonly used ones are polymers named PM6 and PM7, which suffer from several problems. First, the performance of these polymers (particularly PM7) relies on precise control of their molecular weights. Also, their optimal morphology is extremely sensitive to any structural modification. In this work, a family of donor polymers is developed based on a random polymerization strategy. These polymers can achieve well‐controlled morphology and high‐performance with a variety of chemical structures and molecular weights. The polymer donors are D–A1–D–A2‐type random copolymers in which the D and A1 units are monomers originating from PM6 or PM7, while the A2 unit comprises an electron‐deficient core flanked by two thiophene rings with branched alkyl chains. Consequently, multiple cases of highly efficient NF‐OSCs are achieved with efficiencies between 16.0% and 17.1%. As the electron‐deficient cores can be changed to many other structural units, the strategy can easily expand the choices of high‐performance donor polymers for NF‐OSCs.

Layer‐by‐layer solution‐processed organic solar cells optimize the donor layer and acceptor layer separately to make the two components ideally distribute in the vertical direction, which facilitates charge transport and collection. This bilayer structure has less dependence on donor/acceptor ratio, solvent concentration, and so on. It is easy to prepare high‐performance devices with good stability and a high repetition rate.

Organic solar cells (OSCs) have attracted wide attention due to their economy, environmental protection, and potential for large‐scale commercial production. The layer‐by‐layer (LbL) solution processing method, where donor solution and acceptor solution are coated sequentially, is a simple and effective way to fabricate OSCs, achieving a high power conversion efficiency (PCE) of up to 17%. Compared with bulk‐heterojunction (BHJ) OSCs, LbL solution‐processed OSCs separately adjust different layers, making the components distribute ideally in the vertical direction that is beneficial for exciton dissociation, charge transport, and charge collection. Moreover, the LbL approach has better potential in the preparation of large‐area devices, which is a key link in the commercialization of OSCs. Herein, the basic principles and the latest research progress of LbL solution‐processed OSCs are summarized, and the existing challenges and prospects of the LbL solution processing method in industrial production are discussed.

9‐Fluorenone‐1‐carboxylic acid (FCA) is utilized to prolong the lifetime of photogenerated excitons in a nonfullerene acceptor (IT‐M) approximately twofold, ensuring longer exciton diffusion length and efficiency enhancement in organic photovoltaic devices. The prolongation arises from the discovered intermolecular vibrational coupling between the electronic excited state of IT‐M and the electronic ground state of FCA, thus suppressing the nonradiative decay.

Abstract

Exciton lifetime (τ) is crucial for the migration of excitons to donor/acceptor interfaces for subsequent charge separation in organic solar cells (OSCs); however, obvious prolongation of τ has rarely been achieved. Here, by introducing a solid additive 9‐fluorenone‐1‐carboxylic acid (FCA) into the active layer, which comprises a nonfullerene acceptor, 3,9‐bis(2‐methylene‐((3‐(1,1‐dicyanomethylene)‐6/7‐methyl)‐indanone))‐5,5,11,11‐tetrakis(4‐hexylphenyl)‐dithieno[2,3‐d:2′,3′‐d′]‐s‐indaceno[1,2‐b:5,6‐b′]dithiophene (IT‐M), τ is substantially prolonged from 491 to 928 ps, together with obvious increases in fluorescence intensity and quantum yield. Time‐resolved transient infrared spectra indicate the presence of an intermolecular vibrational coupling between the electronic excited state of IT‐M and the electronic ground state of FCA, which is first observed here and which can suppress the internal conversion process. IT‐M‐based OSCs display an improved short‐circuit current and fill factor after the addition of FCA. Thus, the power conversion efficiency is increased, particularly for devices with a large donor/acceptor ratio of 1:4, whose efficiency is increased by 56%. This study describes a novel method, which is also applicable to other nonfullerene acceptors, for further improving the performance of OSCs without affecting their morphology and light absorption properties.

With synergistic optimization of the active layer morphology, flexible substrate properties, and processing temperature, large‐area flexible organic solar cells with high performance are achieved by the slot‐die coating process. The 1 cm² flexible devices produce an excellent power conversion efficiency (PCE) of 12.16%, and, for modules with an area of 25 cm², an extraordinary PCE of 10.09% is observed.

Abstract

Slot‐die coating is generally regarded as the most effective large‐scale methodology for the fabrication of organic solar cells (OSCs). However, the corresponding device performance significantly lags behind spin‐coated devices. Herein, the active layer morphology, flexible substrate properties, and the processing temperature are optimized synergistically to obtain high power conversion efficiency (PCE) for both the flexible single cells and the modules. As a result, the 1 cm² flexible devices produce an excellent PCE of 12.16% as compared to 12.37% for the spin‐coated small‐area (0.04 cm²) rigid devices. Likewise, for modules with an area of 25 cm², an extraordinary PCE of 10.09% is observed. Hence, efficiency losses associated with the upscaling are significantly reduced by the synergistic optimization. Moreover, after 1000 bending cycles at a bending radius of 10 mm, the flexible devices still produce over 99% of their initial PCE, whereas after being stored for over 6000 h in a glove box, the PCE reaches 103% of its initial value, indicating excellent device flexibility as well as superior shelf stability. These results, thus, are a promising confirmation the great potential for upscaling of large‐area OSCs in the near future.

Through investigation of the underlying thermodynamic and kinetic aspects of non‐fullerene acceptor crystallization, the importance of diffusion coefficients and melting enthalpies in controlling the crystal growth rates is demonstrated, and it is revealed and that differences in halogenation can drastically change crystallization kinetics and device stability.

Abstract

With power conversion efficiency now over 17%, a long operational lifetime is essential for the successful application of organic solar cells. However, most non‐fullerene acceptors can crystallize and destroy devices, yet the fundamental underlying thermodynamic and kinetic aspects of acceptor crystallization have received limited attention. Here, room‐temperature (RT) diffusion coefficients of 3.4 × 10⁻²³ and 2.0 × 10⁻²² are measured for ITIC‐2Cl and ITIC‐2F, two state‐of‐the‐art non‐fullerene acceptors. The low coefficients are enough to provide for kinetic stabilization of the morphology against demixing at RT. Additionally profound differences in crystallization characteristics are discovered between ITIC‐2F and ITIC‐2Cl. The differences as observed by secondary‐ion mass spectrometry, differential scanning calorimetry (DSC), grazing‐incidence wide‐angle X‐ray scattering, and microscopy can be related directly to device degradation and are attributed to the significantly different nucleation and growth rates, with a difference in the growth rate of a factor of 12 at RT. ITIC‐4F and ITIC‐4Cl exhibit similar characteristics. The results reveal the importance of diffusion coefficients and melting enthalpies in controlling the growth rates, and that differences in halogenation can drastically change crystallization kinetics and device stability. It is furthermore delineated how low nucleation density and large growth rates can be inferred from DSC and microscopy experiments which could be used to guide molecular design for stability.

Herein the morphology and exciton/charge carrier dynamics in bulk heterojunctions of the donor polymer PTQ10 and molecular acceptor IDIC are investigated. The results emphasize the potential for high material crystallinity to enhance charge separation and collection in organic solar cells, but also that long exciton diffusion lengths are likely to be essential for efficient exciton separation in such high crystallinity devices.

Abstract

Herein the morphology and exciton/charge carrier dynamics in bulk heterojunctions (BHJs) of the donor polymer PTQ10 and molecular acceptor IDIC are investigated. PTQ10:IDIC BHJs are shown to be particularly promising for low cost organic solar cells (OSCs). It is found that both PTQ10 and IDIC show remarkably high crystallinity in optimized BHJs, with GIWAXS data indicating pi‐pi stacking coherence lengths of up to 8 nm. Exciton‐exciton annihilation studies indicate long exciton diffusion lengths for both neat materials (19 nm for PTQ10 and 9.5 nm for IDIC), enabling efficient exciton separation with half lives of 1 and 3 ps, despite the high degree of phase segregation in this blend. Transient absorption data indicate exciton separation leads to the formation of two spectrally distinct species, assigned to interfacial charge transfer (CT) states and separated charges. CT state decay is correlated with the appearance of additional separate charges, indicating relatively efficient CT state dissociation, attributed to the high crystallinity of this blend. The results emphasize the potential for high material crystallinity to enhance charge separation and collection in OSCs, but also that long exciton diffusion lengths are likely to be essential for efficient exciton separation in such high crystallinity devices.

The two non‐fullerene acceptors 3,9‐bis(2‐methylene‐(3‐(1,1‐dicyanomethylene)‐indanone))‐5,5,11,11‐tetrakis(4‐hexylphenyl)‐dithieno[2,3‐d:2',3'‐d']‐s‐indaceno[1,2‐b:5,6‐b']dithiophene (ITIC)‐4F and ITIC‐4Cl co‐crystallize, a process that is suppressed when blended with the donor polymer PTB7‐Th. As a result, the corresponding ternary devices display stable photovoltaic performance up to 170 °C, in contrast to the binary devices that suffer acceptor crystallization. This indicates that acceptor mixtures allow to fabricate devices with excellent thermal stability.

Abstract

While photovoltaic blends based on non‐fullerene acceptors are touted for their thermal stability, this type of acceptor tends to crystallize, which can result in a gradual decrease in photovoltaic performance and affects the reproducibility of the devices. Two halogenated indacenodithienothiophene‐based acceptors that readily co‐crystallize upon mixing are studied, which indicates that the use of an acceptor mixture alone does not guarantee the formation of a disordered mixture. The addition of the donor polymer to the acceptor mixture readily suppresses the crystallization, which results in a fine‐grained ternary blend with nanometer‐sized domains that do not coarsen due to a high T _g ≈ 200 °C. As a result, annealing at temperatures of up to 170 °C does not markedly affect the photovoltaic performance of ternary devices, in contrast to binary devices that suffer from acceptor crystallization in the active layer. The results indicate that the ternary approach enables the use of high‐temperature processing protocols, which are needed for upscaling and high‐throughput fabrication of organic solar cells. Further, ternary devices display a stable photovoltaic performance at 130 °C for at least 205 h, which indicates that the use of acceptor mixtures allows to fabricate devices with excellent thermal stability.

Large‐area prepatterned silver nanowire electrodes are prepared via gravure printing, which show high uniformity and balanced conductivity (10.8 Ω sq⁻¹) and transparency (95.4%). High power conversion efficiencies of 15.28% and 13.61% are achieved for 0.04 and 1 cm² cells, respectively.

Abstract

With the aim of developing high‐performance flexible polymer solar cells, the preparation of flexible transparent electrodes (FTEs) via a high‐throughput gravure printing process is reported. By varying the blend ratio of the mixture solvent and the concentration of the silver nanowire (AgNW) inks, the surface tension, volatilization rate, and viscosity of the AgNW ink can be tuned to meet the requirements of gravure printing process. Following this method, uniformly printed AgNW films are prepared. Highly conductive FTEs with a sheet resistance of 10.8 Ω sq⁻¹ and a high transparency of 95.4% (excluded substrate) are achieved, which are comparable to those of indium tin oxide electrode. In comparison with the spin‐coating process, the gravure printing process exhibits advantages of the ease of large‐area fabrication and improved uniformity, which are attributed to better ink droplet distribution over the substrate. 0.04 cm² polymer solar cells based on gravure‐printed AgNW electrodes with PM6:Y6 as the photoactive layer show the highest power conversion efficiency (PCE) of 15.28% with an average PCE of 14.75 ± 0.35%. Owing to the good uniformity of the gravure‐printed AgNW electrode, the highest PCE of 13.61% is achieved for 1 cm² polymer solar cells based on the gravure‐printed FTEs.