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Herein, two emerging device optimization methods, solid additive and layer‐by‐layer (LBL) process, for organic solar cells (OSCs) are simultaneously studied. Through traditional blend cast and recently proposed identical solvent LBL cast, BDCB (2‐monobromo‐1,3‐dichloro‐bezene), a benzene derivative, is used to improve the device performance based on celebrity combination PM6:L8‐BO. The results reveal that finely optimized BDCB concentration in PM6 solution can push the efficiency of LBL to 19.03% compared to blend cast with only 18.12% while the power conversion efficiency (PCE) changing trend is determined by BDCB's ratio in L8‐BO's precursor. The morphology characterizations confirm there exists no significant stratification for LBL‐processed devices, supported by a previously reported swelling‐intercalation‐phase separation (SIPS) model. Thereby, the solid additive's 2D optimization is considered a smart strategy for finely tuning the SIPS process, which results in various final morphology states. This work not only reports a cutting‐edge efficiency for binary OSCs, but also new insight and deep understanding for LBL method‐based morphology optimization strategy development. [ABSTRACT FROM AUTHOR]

The challenge of continuous printing in high-efficiency large-area organic solar cells is a key limiting factor for their widespread adoption. A materials design concept for achieving large-area, solution-coated all-polymer bulk heterojunction solar cells with stable phase separation morphology between the donor and acceptor is presented. The key concept lies in inhibiting strong crystallization of donor and acceptor polymers, thus forming intermixed, low crystallinity, and mostly amorphous blends. Based on experiments using donors and acceptors with different degree of crystallinity, the results show that microphase separated donor and acceptor domain sizes are inversely proportional to the crystallinity of the conjugated polymers. This methodology of using low crystallinity donors and acceptors has the added benefit of forming a consistent and robust morphology that is insensitive to different processing conditions, allowing one to easily scale up the printing process from a small-scale solution shearing coater to a large-scale continuous roll-to-roll (R2R) printer. Large-area all-polymer solar cells are continuously roll-to-roll slot die printed with power conversion efficiencies of 5%, with combined cell area up to 10 cm2. This is among the highest efficiencies realized with R2R-coated active layer organic materials on flexible substrate.

Organic solar cell (OSC) development continues to demonstrate impressive device efficiency improvements. However, the materials synthetic simplicity essential to industrialization remains seriously lacking attention, imparting inferior performance records in low‐cost devices. Hence, low bandgap and completely non‐fused electron acceptors (CNFEAs) having simple molecular structures are investigated herein. In contrast to typically explored fused‐ring acceptors with smaller backbone conformational variations, minimizing the interface recombination sites through a greater extent of localized domains is identified as more critical in CNFEAs, leading to remarkable fill factors (FFs) approaching 75%, among the highest currently realized for low‐cost systems. However, this comes with diminishing charge generation efficiency. The general ternary blend optimization strategy modifying the morphology of host components is limited in preserving such remarkably high FFs. To suppress the trade‐off while keeping notable FFs, a new perspective of constructing functionally bridged components based on optical, electronic, and thermodynamic properties is introduced here. Specifically, charge generation is unrestrained from the host acceptor localized domains through the introduction of a "bridge" component while also taking advantage of the configuration to channel polarons toward the efficient transport moieties of the host components. Accordingly, this work incubates understanding‐guided optimizations toward the advancement of more practical devices. [ABSTRACT FROM AUTHOR]

Fluorination of end groups has been a great success in developing efficient small molecule acceptors. However, this strategy has not been applied to the development of polymer acceptors. Here, a dihalogenated end group modified by fluorine and bromine atoms simultaneously, namely IC‐FBr, is first developed, then employed to construct a new polymer acceptor (named PYF‐T) for all‐polymer solar cells (all‐PSCs). In comparison with its non‐fluorinated counterpart (PY‐T), PYF‐T exhibits stronger and red‐shifted absorption spectra, stronger molecular packing and higher electron mobility. Meanwhile, the fluorination on the end groups down‐shifts the energy levels of PYF‐T, which matches better with the donor polymer PM6, leading to efficient charge transfer and small voltage loss. As a result, an all‐PSC based on PM6:PYF‐T yields a higher power conversion efficiency (PCE) of 14.1% than that of PM6:PY‐T (11.1%), which is among the highest values for all‐PSCs reported to date. This work demonstrates the effectiveness of fluorination of end‐groups in designing high‐performance polymer acceptors, which paves the way toward developing more efficient and stable all‐PSCs. [ABSTRACT FROM AUTHOR]

In this paper, a strategy of asymmetric alkyl and alkoxy substitution is applied to state‐of‐the‐art Y‐series nonfullerene acceptors (NFAs), and it achieves great performance in organic solar cell (OSC) devices. Since alkoxy groups can have a significant influence on the material properties of NFAs, alkoxy substitution is applied to the Y6 molecule in a symmetric manner. The resulting molecule (named Y6‐2O), despite showing improved open‐circuit voltage (Voc), yields extremely poor performance due to low solubility and excessive aggregation properties, a change that is due to the conformational locking effect of alkoxy groups. In contrast, asymmetric alkyl and alkoxy substitution on Y6, yields a molecule named Y6‐1O that can maintain the positive effect of Voc improvement and obtain reasonably good solubility. The resulting molecule Y6‐1O enables highly efficient nonfullerene OSCs with 17.6% efficiency and the asymmetric side‐chain strategy has the potential to be applied to other NFA‐material systems to further improve their performance. [ABSTRACT FROM AUTHOR]

Abstract: Ternary organic solar cells (OSCs) have attracted much research attention, as they can maintain the simplicity of the single‐junction device architecture while broadening the absorption range of OSCs. However, one main challenge that limits the development of ternary OSCs is the difficulty in controlling the morphology of ternary OSCs. In this paper, an effective approach to control the morphology is presented that leads to multiple cases of efficient nonfullerene ternary OSCs with efficiencies of up to 11.2%. This approach is based on a donor polymer with strong temperature dependent aggregation properties processed from hot solutions without any solvent additives and a pair of small molecular acceptors (SMAs) that have similar surface tensions and thus low propensity to form discrete phases. Such a ternary blend exhibits a simplified bulk‐heterojunction morphology that is similar to the morphology of previously reported binary blends. As a result, an almost linear relationship between VOC and film composition is observed for all nonfullerene ternary devices. Meanwhile, by carefully designing a control system with a large interfacial tension, a different phase separation and VOC dependence is demonstrated. This morphology control approach can be applicable to more material systems and accelerates the development of the ternary OSC field. [ABSTRACT FROM AUTHOR]

Abstract: The device performance of polymer solar cells (PSCs) is strongly dependent on the blend morphology. One of the strategies for improving PSC performance is side‐chain engineering, which plays an important role in controlling the aggregation properties of the polymers and thus the domain crystallinity/purity of the donor–acceptor blends. In particular, for a family of high‐performance donor polymers with strong temperature‐dependent aggregation properties, the device performances are very sensitive to the size of alkyl chains, and the best device performance can only be achieved with an optimized odd‐numbered alkyl chain. However, the synthetic route of odd‐numbered alkyl chains is costly and complicated, which makes it difficult for large‐scale synthesis. Here, this study presents a facile method to optimize the aggregation properties and blend morphology by employing donor polymers with a mixture of two even‐numbered, randomly distributed alkyl chains. In a model polymer system, this study suggests that the structural and electronic properties of the random polymers comprising a mixture of 2‐octyldodecyl and 2‐decyltetradecyl alkyl chains can be systematically tuned by varying the mixing ratio, and a high power conversion efficiency (11.1%) can be achieved. This approach promotes the scalability of donor polymers and thus facilitates the commercialization of PSCs. [ABSTRACT FROM AUTHOR]

Abstract: Newly developed benzo[1,2‐b:4,5‐b′]dithiophene (BDT) block with 3,4‐ethylenedioxythiophene (EDOT) side chains is first employed to build efficient photovoltaic copolymers. The resulting copolymers, PBDTEDOT‐BT and PBDTEDOTFBT, have a large bandgap more than 1.80 eV, which is attributed to the increased steric hindrance between the BDT and EDOT skeletons. Both copolymers possess the satisfied absorptions, low‐lying highest occupied molecular orbital (HOMO) levels and high crystallinity. Using the fluorination strategy, PBDTEDOT‐FBT exhibits a wider and stronger absorption and a deeper HOMO level than those of PBDTEDOT‐BT. PBDTEDOT‐FBT:[6,6]‐Phenyl C71 butyric acid methyl ester (PC71BM) blend also shows the higher hole mobility and better surface morphology compared with the PBDTEDOTBT:PC71BM blend. Combination of above advantages, PBDTEDOT‐FBT devices exhibit much higher power conversion efficiency (PCE) of 10.11%, with an improved open circuit voltage (Voc) of 0.86 V, short circuit current densities (Jsc) of 16.01 mA cm−2, and fill factor (FF) of 72.6%. This work not only provides a newly efficient candidate of BDT donor block modified with EDOT conjugated side chains, but also achieves high‐performance large bandgap copolymers for polymer solar cells (PSCs) via the synergistic effect of fluorination and side chain engineering strategies. [ABSTRACT FROM AUTHOR]

Abstract: Nonfullerene polymer solar cells (PSCs) based on polymer donors and nonfullerene small molecular acceptors (SMAs) have recently attracted considerable attention. Although much of the progress is driven by the development of novel SMAs, the donor polymer also plays an important role in achieving efficient nonfullerene PSCs. However, it is far from clear how the polymer donor choice influences the morphology and performance of the SMAs and the nonfullerene blends. In addition, it is challenging to carry out quantitative analysis of the morphology of polymer:SMA blends, due to the low material contrast and overlapping scattering features of the π–π stacking between the two organic components. Here, a series of nonfullerene blends is studied based on ITIC‐Th blended with five different donor polymers. Through quantitative morphology analysis, the (010) coherence length of the SMA is characterized and a positive correlation between the coherence length of the SMA and the device fill factor (FF) is established. The study reveals that the donor polymer can significantly change the molecular ordering of the SMA and thus improve the electron mobility and domain purity of the blend, which has an overall positive effect that leads to the enhanced device FF for nonfullerene PSCs. [ABSTRACT FROM AUTHOR]

The influences of various processing parameters and polymer molecular weight on the morphology and properties of poly[(5,6-difluoro-2,1,3-benzothiadiazol-4,7-diyl)-alt-(3,3"-di(2-octyldodecyl) 2,2';5',2";5",2"-quaterthiophen-5,5"-diyl)] (PffBT4T-2OD)-based polymer solar cells (PSCs) are investigated. High spin rate/high temperature conditions are found to significantly reduce polymer crystallinity and change polymer backbone orientation from face-on to edge-on. Most surprisingly, it is found that the median domain sizes of PffBT4T-2OD:PC71BM blends processed at different temperatures/spin rates are nearly identical, while the average domain purity and the molecular orientation relative to polymer:fullerene interfaces can be significantly changed by the processing conditions. A systematic study is carried out to identify the roles of individual processing parameters including processing temperature, spin rate, concentration, and solvent mixtures. Furthermore, the effect of molecular weight on morphology control is also examined. These detailed studies provide important guidance to control and optimize various morphological parameters and thus electrical properties of PffBT4T-2OD-type materials for the application in PSC. [ABSTRACT FROM AUTHOR]

Although ternary solar cells (TSCs) offer a cost‐effective prospect to expand the absorption bandwidth of organic solar cells, only few TSCs have succeeded in surpassing the performance of binary solar cells (BSCs) primarily due to the complicated morphology of the ternary blends. Here, the key factors that create and limit the morphology and performance of the TSCs are elucidated. The origin of morphology formation is explored and the role of kinetic factors is investigated. The results reveal that the morphology of TSC blends considered in this study are characterized with either a single length‐scale or two length‐scale features depending on the composition of the photoactive polymers in the blend. This asymmetric morphology development reveals that TSC blend morphology critically depends on material compatibility and polymer solubility. Most interestingly, the fill factor (FF) of TSCs is found to linearly correlate with the relative standard deviation of the fullerene distribution at small lengths. This is the first time that such a correlation has been shown for ternary systems. The criteria that uniform sized and highly pure amorphous domains are accomplished through the correct kinetic path to obtain a high FF for TSCs are specifically elucidated. The findings provide a critical insight for the precise design and processing of TSCs. Linear correlation of fill factor and relative standard deviation of fullerene distribution reveals that a ternary blend morphology with a uniform and pure mixed amorphous domain is required to achieve efficient ternary solar cells. This is achieved by the right kinetic path, controlled by the material and process compatibility. [ABSTRACT FROM AUTHOR]

While the performance of laboratory‐scale organic solar cells (OSCs) continues to grow over 13%, the development of high‐efficiency large area OSCs still lags. One big challenge is that the formation of bulk heterojunction morphology is an extremely complicated process and the formed morphology is also a highly delicate balance involving many parameters such as domain size, purity, miscibility, etc. The morphology control becomes much more challenging when the device area is scaled up. In this work, a highly efficient (12.9%) nonfullerene organic solar cell processed using a sequential bilayer deposition method from nonhalogenated solvents, is reported. Using this bilayer processing method, the organic solar cells can be scaled up to a larger area (1 cm2) while maintaining a high performance of 11.4% using doctor‐blade‐coating technique. Moreover, as the acceptor is hidden behind the polymer donor, the possibility of degradation by sunlight is lessened. Thus, improved photostability is observed in the bilayer structure device when compared with the bulk heterojunction device. This method offers a truly compatible processing technique for printing large‐area OSC modules. A high‐performance (12.9%) non‐fullerene organic solar cell processed using a sequential bilayer deposition method from non‐halogenated solvents is reported. Using this method, the organic solar cell can be scaled up to a larger area (1 cm2) while maintaining a high performance of 11.4% by doctor‐blade coating. This method offers a truly compatible processing technique for printing large area organic solar cell modules. [ABSTRACT FROM AUTHOR]