Wide Bandgap Molecular Acceptors with a Truxene Core for Efficient Nonfullerene Polymer Solar Cells: Linkage Position on Molecular Configuration and Photovoltaic Properties

Two wide bandgap star‐shaped small molecular acceptors, para‐TrBRCN and meta‐TrBRCN , are synthesized for efficient nonfullerene polymer solar cells (PSCs). The tiny structural variation by just changing the linkage positions affects largely the inherent properties of the resulting molecules. Both molecules have a nonplanar 3D structure, which can prevent the excessively aggregation to realize the optimized morphology and ideal domain size in their active blends. Compared to para‐TrBRCN , meta‐TrBRCN exhibits the smaller distortions between the truxene skeleton and the benzothiadiazole units, which would also lead to the enhanced π–π stacking and charge transfer. When blending with PTB7‐Th, high power conversion efficiencies (PCEs) of 10.15% and 8.28% are obtained for meta‐TrBRCN and para‐TrBRCN devices, respectively. To make up the weak absorption of above binary active blend in the longer wavelength region and increase the whole device performance further, low bandgap 3,9‐bis(2‐methylene‐(3‐(1,1‐dicyanomethylene)‐indanone)‐5,5,11,11‐tetrakis(4‐hexylthienyl)‐dithieno[2,3‐d:2′,3′‐d′]‐s‐indaceno[1,2‐b:5,6‐b′]‐dithiophene (ITIC‐Th) is added as the second acceptor material to fabricate ternary blend PSCs. After adding 20 wt% of ITIC‐Th, the resulting devices exhibit the well‐balanced optical absorption and fine‐tuned morphology, giving rise to the significantly improved PCE of 11.40% with much higher J _sc of 18.25 mA cm^?2 and fill factor of 70.2%.     

Efficient Ternary Organic Solar Cells Enabled by the Integration of Nonfullerene and Fullerene Acceptors with a Broad Composition Tolerance

The ternary structure that combines fullerene and nonfullerene acceptors in a photoactive layer is demonstrated as an effective approach for boosting the power conversion efficiencies (PCEs) of organic solar cells (OSCs). Here, highly efficient ternary OSCs comprising a wide‐bandgap polymer donor (PBT1‐C), a narrow‐bandgap nonfullerene acceptor (IT‐2F), and a typical fullerene derivative (PC₇₁BM) are reported. It is found that the addition of PC₇₁BM into the PBT1‐C:IT‐2F blend not only increases the device efficiency up to 12.2%, but also improves the ambient stability of the OSCs. Detailed investigations indicate that the improvement in photovoltaic performance benefits from synergistic effects of increased photon‐harvesting, enhanced charge separation and transport, suppressed trap‐assisted recombination, and optimized film morphology. Moreover, it is noticed that such a ternary system exhibits excellent tolerance to the PC₇₁BM component, for which PCEs over 11.2% can be maintained throughout the whole blend ratios, higher than that (11.0%) of PBT1‐C:IT‐2F binary reference device.     

Near‐Infrared Small Molecule Acceptor Enabled High‐Performance Nonfullerene Polymer Solar Cells with Over 13% Efficiency

One of the most promising approaches to achieve high‐performance polymer solar cells (PSCs) is to develop nonfullerene small molecule acceptors (SMAs) with an absorption extending to the near‐infrared (NIR) region. In this work, two novel SMAs, namely, BTTIC and BTOIC, are designed and synthesized, with optical bandgaps (E_g^opt) of 1.47 and 1.39 eV, respectively. Desipte the narrow E_g^opt, the PBDB‐T:BTTIC‐ and PBDB‐T:BTOIC‐based PSCs can maintain high V_OCs of over 0.90 and 0.86 V, respectively, with low energy losses (E_loss) < 0.6 eV. Meanwhile, due to the favorable morphology of the PBDB‐T:BTTIC blend, balanced carrier mobilities are achieved. The high external quantum efficiencies enable a high power conversion efficiency (PCE) up to 13.18% for the PBDB‐T:BTTIC‐based PSCs. In comparison, BTOIC shows an excessive crystallization propensity owing to its oxyalkyl side groups, which eventually leads to a relatively low PCE for the PBDB‐T:BTOIC‐based PSCs. Overall, this work provides insights into the design of novel NIR‐absorbing SMAs for nonfullerene PSCs.     

Influence of Molecular Geometry of Perylene Diimide Dimers and Polymers on Bulk Heterojunction Morphology Toward High‐Performance Nonfullerene Polymer Solar Cells

In this study, we investigate the influence of molecular geometry of the donor polymers and the perylene diimide dimers (di‐PDIs) on the bulk heterojunction (BHJ) morphology in the nonfullerene polymer solar cells (PSCs). The results reveal that the pseudo 2D conjugated poly[4,8‐bis(5‐(2‐ethylhexyl)thiophen‐2‐yl)benzo[1,2‐b;4,5‐b′]dithiophene‐2,6‐diyl‐alt‐(4‐(2‐ethylhexyl)‐3‐fluorothieno[3,4‐b]thiophene‐)‐2‐carboxylate‐2‐6‐diyl)] (PTB7‐Th) has better miscibility with both bay‐linked di‐PDI (B‐di‐PDI) and hydrazine‐linked di‐PDI (H‐di‐PDI) compared to its 1D analog, poly[[4,8‐bis[(2‐ethylhexyl)oxy]benzo[1,2‐b:4,5‐b′]dithiophene‐2,6‐diyl][3‐fluoro‐2‐[(2‐ethylhexyl)carbonyl]thieno[3,4‐b]thiophenediyl]] (PTB7), to facilitate more efficient exciton dissociation in the BHJ films. However, the face‐on oriented π–π stacking of PTB7‐Th is severely disrupted by the B‐di‐PDI due to its more flexible structure. On the contrary, the face‐on oriented π–π stacking is only slightly disrupted by the H‐di‐PDI, which has a more rigid structure to provide suitable percolation pathways for charge transport. As a result, a very high power conversion efficiency (PCE) of 6.41% is achieved in the PTB7‐Th:H‐di‐PDI derived device. This study shows that it is critical to pair suitable polymer donor and di‐PDI‐based acceptor to obtain proper BHJ morphology for achieving high PCE in the nonfullerene PSCs.     

Influence of Blend Morphology and Energetics on Charge Separation and Recombination Dynamics in Organic Solar Cells Incorporating a Nonfullerene Acceptor

Nonfullerene acceptors (NFAs) in blends with highly crystalline donor polymers have been shown to yield particularly high device voltage outputs, but typically more modest quantum yields for photocurrent generation as well as often lower fill factors (FF). In this study, we employ transient optical and optoelectronic analysis to elucidate the factors determining device photocurrent and FF in blends of the highly crystalline donor polymer PffBT4T‐2OD with the promising NFA FBR or the more widely studied fullerene acceptor PC₇₁BM. Geminate recombination losses, as measured by ultrafast transient absorption spectroscopy, are observed to be significantly higher for PffBT4T‐2OD:FBR blends. This is assigned to the smaller LUMO‐LUMO offset of the PffBT4T‐2OD:FBR blends relative to PffBT4T‐2OD:PC₇₁BM, resulting in the lower photocurrent generation efficiency obtained with FBR. Employing time delayed charge extraction measurements, these geminate recombination losses are observed to be field dependent, resulting in the lower FF observed with PffBT4T‐2OD:FBR devices. These data therefore provide a detailed understanding of the impact of acceptor design, and particularly acceptor energetics, on organic solar cell performance. Our study concludes with a discussion of the implications of these results for the design of NFAs in organic solar cells.     

Effects of Fullerene Bisadduct Regioisomers on Photovoltaic Performance

Fullerene bisadducts have emerged as promising electron‐accepting materials because of their ability to increase the open‐circuit voltage (V_OC) of polymer solar cells (PSCs) due to their relatively high lowest unoccupied molecular orbital (LUMO) energy levels. It should be noted that the as‐prepared fullerene bisadducts are in fact a mixture of isomers. Here, the effects of fullerene bisadduct regioisomers on photovoltaic performance are examined. The trans‐2, trans‐3, trans‐4, and e isomers of dihydronaphthyl‐based [60]fullerene bisadduct (NCBA) are isolated and used as acceptors for P3HT‐based PSCs. The four NCBA isomers exhibit different absorption spectra, electrochemical properties, and electron mobilities, leading to varying PCE values of 5.8, 6.3, 5.6, and 5.5%, respectively, which are higher than that based on an NCBA mixture (5.3%), suggesting the necessity to use the individual fullerene bisadduct isomer for high‐performance PSCs.     

Molecular Consideration for Small Molecular Acceptors Based on Ladder‐Type Dipyran: Influences of O‐Functionalization and π‐Bridges

Molecular engineering of nonfullerene acceptors (NFAs) plays a vital role in the development of organic photovoltaics. Oxygen as an electron donating atom is incorporated into the NFA system as alkoxyl forms at central, terminal, or central conjugated moieties due to the tunability at structural conformation, solubility, electron donating ability, absorption, energy levels, etc. In this work, a novel dipyran‐based ladder‐type building block ( Ph‐DTDP ), which possesses two oxygen atoms in the conjugated skeleton, is designed and facilely synthesized. It is applied as the donor core for the acceptor–donor–acceptor‐type NFA design and such functionalized‐O efficiently enhances the electron donating ability, lowers the band gap, redshifts and extends the absorption spectra. In addition, the π‐bridge effects are considered as well. Photovoltaic performances are systematically investigated and a high power conversion efficiency of 9.21% can be afforded with an energy loss of 0.57 eV. Meanwhile, the morphologies as well as the carrier mobilities of the blend films are studied to assist further understanding of the structure–property relationships. Overall, the study in this work provides a new promising ladder‐type dipyran building block and brings in a novel way to use oxygen in NFA molecular structure design.     

Retarding the Crystallization of a Nonfullerene Electron Acceptor for High‐Performance Polymer Solar Cells

Developing a fundamental understanding of the molecular order within the photoactive layer, and the influence therein of solution casting conditions, is a key factor in obtaining high power conversation efficiency (PCE) polymer solar cells. Herein, the molecular order in PBDB‐T:INPIC‐4F nonfullerene solar cells is tuned by control of the molecular organization time during film casting, and the crucial role of retarding the crystallization of INPIC‐4F in achieving high performance is demonstrated. When PBDB‐T:INPIC‐4F is cast with the presence of solvent vapor to prolong the organization time, INPIC‐4F molecules form spherulites with a polycrystalline structure, resulting in large phase separation and device efficiency below 10%. On the contrary, casting the film on a hot substrate is effective in suppressing the formation of the polycrystalline structure, and encourages face‐on π?π stacking of INPIC‐4F. This molecular transformation of INPIC‐4F significantly enhances the absorption ability of INPIC‐4F at long wavelengths and facilitates a fine phase separation to support efficient exciton dissociation and balanced charge transport, leading to the achievement of a maximum PCE of 13.1%. This work provides a rational guide for optimizing nonfullerene polymer solar cells consisting of highly crystallizable small molecular electron acceptors.     

Molecular Engineering of Highly Efficient Small Molecule Nonfullerene Acceptor for Organic Solar Cells

A new molecularly engineered nonfullerene acceptor, 2,2′‐(5,5′‐(9,9‐didecyl‐9H‐fluorene‐2,7‐diyl)bis (benzo[c][1,2,5]thiadiazole‐7,4‐diyl)bis (methanylylidene))bis (3‐hexyl‐1,4‐oxothiazolidine‐5,2‐diylidene))dimalononitrile ( BAF‐4CN ), with fluorene as the core and arms of dicyano‐n‐hexylrhodanine terminated benzothiadiazole is synthesized and used as an electron acceptor in bulk heterojunction organic solar cells. BAF‐4CN shows a stronger and broader absorption with a high molar extinction coefficient of 7.8 × 10⁴m ^?1 cm^?1 at the peak position (498 nm). In the thin film, the molecule shows a redshift around 17 nm. The photoluminescence experiments confirm the excellent electron accepting nature of BAF‐4CN with a Stern–Volmer coefficient (K _sv) of 1.1 × 10⁵m ^?1. From the electrochemical studies, the highest occupied molecular orbital and lowest unoccupied molecular orbital energy levels of BAF‐4CN are estimated to be ?5.71 and ?3.55 eV, respectively, which is in good synchronization with low bandgap polymer donors. Using BAF‐4CN as an electron acceptor in a 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)] based bulk‐heterojunction solar cell, a maximum power conversion efficiency of 8.4% with short‐circuit current values of 15.52 mA cm^?2, a fill factor of 70.7%, and external quantum efficiency of about 84% covering a broad range of wavelength is achieved.     

Effects of Halogenation of Small-Molecule and Polymeric Acceptors for Efficient Organic Solar Cells

Tuning the properties of non-fullerene acceptors (NFAs) through halogenation, including fluorination and chlorination, represents one of the most promising strategies to boost the performance of organic solar cells (OSCs). However, it remains unclear how the F and Cl choice influences the molecular packing and performance between small-molecule and polymeric acceptors. Here, a series of small-molecule and polymeric acceptors with different amounts and types of halogenation is synthesized, and the effects of fluorination and chlorination between small-molecule and polymeric acceptors are investigated. It is found that chlorinated small-molecule acceptors lead to longer exciton diffusion length and better performance compared to the corresponding fluorinated ones, which attributes to their stronger intermolecular packing mode. For polymer acceptors, in contrast, the fluorinated polymers achieve a denser packing mode and better performance, because chlorinated polymers exhibit reduced intrachain conjugation between end group moieties and linker units. This study demonstrates different halogenation effects on the packing modes and performances for small-molecule and polymeric acceptors, which provides important guidance for the molecule design of high-performance acceptors for OSCs.     

Efficient and Scalable Large-Area Organic Solar Cells by Asymmetric Nonfullerene Acceptors Based on 9H-Indeno[1,2-b]pyrazine-2,3,8-Tricarbonitrile

It remains challenging to fabricate efficient, scalable large-area organic solar cells (OSCs) owing to the unfavorable morphology of photoactive blend films. To address this challenge, two asymmetric nonfullerene acceptors (NFAs) IPC1CN-BBO-IC2F and IPC1CN-BBO-IC2Cl are synthesized, where 12,13-bis(2-butyloctyl)-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 (BBO) is the molecular core, and two types of end groups are appended to its ends, namely the 9H-indeno[1,2-b]pyrazine-2,3,8-tricarbonitrile (IPC1CN) end group and one of 2-(5,6-dihalo-3-oxo-2,3-dihydro-1H-inden-1-ylidene)malononitrile end groups (IC2F or IC2Cl). These NFAs facilitate effective tuning of light absorption and energy levels, offer high carrier mobilities, and allow for the formation of appropriate morphologies. Note that these benefits apply even to large-area devices, unlike typical Y6-based NFAs. In addition, a random copolymer PM6-PBDBT(55) is synthesized and its energy levels are optimally matched with those of the asymmetric NFAs. The blade-coated 1 cm²-area OSCs based on PM6-PBDBT(55):IPC1CN-BBO-IC2Cl exhibit a PCE of 14.12%, which is higher than that of PM6-PBDBT(55)-IPC1CN-BBO-IC2F-based OSCs. More importantly, the PM6-PBDBT(55):IPC1CN-BBO-IC2Cl-based large-area (58.50 cm²) modules yield an impressive PCE of 11.28% with a small cell-to-module loss in fill factor. These results suggest that a combination of the asymmetric molecular design using the IPC1CN group and the terpolymer strategy will pave a new path for fabricating highly efficient and scalable large-area OSCs.     

Atomic Optimization on Pyran-Fused Nonfullerene Acceptor Enables Organic Solar Cells With an Efficiency Approaching 16% and Reduced Energy Loss

Atomic replacement on platforms of nonfullerene acceptor (NFA) with already excellent performance is expected to further optimize the energy levels, absorptions, and even charge transfer dynamics of NFAs effectively without greatly destroying their superior molecular conformations. On the basis of high-performance F-series NFAs, the structural optimization at atomic level is performed by replacing sulfur atoms in FO-2Cl with selenium atoms, thus affording a new NFA labeled as FOSe-2Cl. FOSe-2Cl not only inherits the good planar configuration of FO-2Cl, but also exhibits more suitable energy levels, redshifted absorption, enhanced molecular packing, and accelerative charge transfer/transport dynamics compared with those of FO-2Cl. With a widely used polymer PM6 as the donor, organic solar cell (OSC) based on FOSe-2Cl affords a significantly improved power conversion efficiency (PCE) of 15.94% with a reduced energy loss (E_loss) of 0.670 eV, with respect to that of FO-2Cl-based OSC with a PCE of 14.94% and E_loss of 0.706 eV. The result represents the best performance reported to date for pyran-fused NFAs and F-series NFAs-based binary OSCs, providing another promising platform to achieve the state-of-the-art OSCs in addition to the well-known Y-series NFAs.     

Perylene Diimide‐Based Nonfullerene Polymer Solar Cells with over 11% Efficiency Fabricated by Smart Molecular Design and Supramolecular Morphology Optimization

A series of perylene diimide (PDI) derivatives, TPP‐PDI , TPO‐PDI , and TPS‐PDI , are developed for nonfullerene polymer solar cells (NF‐PSCs) by flaking three PDI skeletons around 3D central cores with different configurations and electronic states, such as triphenylphosphine (TPP), triphenylphosphine monoxide (TPO), and triphenylphosphine sulfide (TPS). These small‐molecule acceptors have a “three‐wing propeller” structure due to their similar backbones. By changing the electron density of phosphorus atoms through oxidation and sulfuration, the “folding‐back” strength is decreased, resulting in a less twisted molecular conformation. The stronger electron‐withdrawing ability of the oxygen atom affords TPO‐PDI the least twisted conformation, which enhances the crystallinity of this complex. NF‐PSCs based on PTTEA : TPO‐PDI exhibit a high power conversion efficiency (PCE) of 8.65%. Ultimately, the joint “molecular lock” effect arising from O? H???F and O? H???O?P supramolecular interactions is achieved by introducing 4,4′‐biphenol as an additive, which successfully promotes fibril‐like phase separation and blend morphology optimization to generate the highest PCE of 11.01%, which is currently the highest value recorded for NF‐PSCs based on PDI acceptors.     

Effects of Short‐Axis Alkoxy Substituents on Molecular Self‐Assembly and Photovoltaic Performance of Indacenodithiophene‐Based Acceptors

The effects of central alkoxy side chain length of a series of narrow bandgap small molecule acceptors (SMAs) on their physicochemical properties and on the photovoltaic performance of the SMA‐based polymer solar cells (PSCs) are systematically investigated. It is found that the ordered aggregation of these SMAs in films is enhanced gradually with the increase of alkoxy chain length. The single‐crystal structures of these SMAs further reveal that small changes in the side chain length can have a dramatic impact on molecular self‐assembly. The short‐circuit current density and power conversion efficiency values of the corresponding PSCs increase with the increase of the side chain length of the SMAs. The π–π coherence length of the SMAs in the active layers is increased with the increase of the side chain length, which could be the reason for the increase of the J_sc in the PSCs. The results indicate that small changes in side chain length can have a dramatic impact on the molecular self‐assembly, morphology, and photovoltaic performance of the PSCs. The structure–performance relationship established in this study can provide important instructions for the side chain engineering and for the design of efficient SMAs materials.     

Side Group Engineering of Small Molecular Acceptors for High‐Performance Fullerene‐Free Polymer Solar Cells: Thiophene Being Superior to Selenophene

Side group of ITIC‐like small molecular acceptor (SMA) plays a critical role in crystallization property. In this article, two new SMAs with n‐hexylthienyl and n‐hexylselenophenyl as side chain, namely ITCPTC‐Th and ITCPTC‐Se, are designed and synthesized by employing newly developed thiophene‐fused ending group (CPTCN). And thiophene and selenophene side group substituted effects of SMA‐based fullerene‐free polymer solar cells (PSCs) are investigated. A stronger σ‐inductive effect between selenophene side group and electron‐donating backbone endows ITCPTC‐Se with better optical absorption and higher LUMO level, ITCPTC‐Th‐based PSCs deliver a higher power conversion efficiency of 10.61%. Charge transport and collection, recombination loss mechanism, and morphology of blend films are intensively studied. These results confirm that side group substituted effects of SMAs are multiple and thiophene is a superior option to selenophene as aromatic side group of ITIC‐like SMAs.     

Nonfullerene Polymer Solar Cells based on a Perylene Monoimide Acceptor with a High Open‐Circuit Voltage of 1.3 V

Nonfullerene polymer solar cells (PSCs) are fabricated with a perylene monoimide‐based n‐type wide‐bandgap organic semiconductor PMI‐F‐PMI as an acceptor and a bithienyl‐benzodithiophene‐based wide‐bandgap copolymer PTZ1 as a donor. The PSCs based on PTZ1:PMI‐F‐PMI (2:1, w/w) with the treatment of a mixed solvent additive of 0.5% N ‐methyl pyrrolidone and 0.5% diphenyl ether demonstrate a very high open‐circuit voltage (V _oc) of 1.3 V with a higher power conversion efficiency (PCE) of 6%. The high V _oc of the PSCs is a result of the high‐lying lowest unoccupied molecular orbital (LUMO) of ?3.42 eV of the PMI‐F‐PMI acceptor and the low‐lying highest occupied molecular orbital (HOMO) of ?5.31 eV of the polymer donor. Very interestingly, the exciton dissociation efficiency in the active layer is quite high, even though the LUMO and HOMO energy differences between the donor and acceptor materials are as small as ≈0.08 and 0.19 eV, respectively. The PCE of 6% is the highest for the PSCs with a V _oc as high as 1.3 V. The results indicate that the active layer based on PTZ1/PMI‐F‐PMI can be used as the front layer in tandem PSCs for achieving high V _oc over 2 V.     

Over 15% Efficiency Polymer Solar Cells Enabled by Conformation Tuning of Newly Designed Asymmetric Small‐Molecule Acceptors

The prosperous period of polymer solar cells (PSCs) has witnessed great progress in molecule design methods to promote power conversion efficiency (PCE). Designing asymmetric structures has been proved effective in tuning energy level and morphology, which has drawn strong attention from the PSC community. Two hepta‐ring and octa‐ring asymmetric small molecular acceptors (SMAs) (IDTP‐4F and IDTTP‐4F) with S‐shape and C‐shape confirmations are developed to study the relationship between conformation shapes and PSC efficiencies. The similarity of absorption and energy levels between two SMAs makes the conformation a single variable. Additionally, three wide‐bandgap polymer donors (PM6, S1, and PM7) are chosen to prove the universality of the relationship between conformation and photovoltaic performance. Consequently, the champion PCE afforded by PM7: IDTP‐4F is as high as 15.2% while that of PM7: IDTTP‐4F is 13.8%. Moreover, the S‐shape IDTP‐4F performs obviously better than their IDTTP‐4F counterparts in PSCs regardless of the polymer donors, which confirms that S‐shape conformation performs better than the C‐shape one. This work provides an insight into how conformations of asymmetric SMAs affect PCEs, specific functions of utilizing different polymer donors to finely tune the active‐layer morphology and another possibility to reach an excellent PCE over 15%.     

Easily Available High-Performance Organic Solar Cells by Regulating Phenylalkyl Side Groups of Non-Fused Ring Electron Acceptors

Although non-fused ring electron acceptors (NFREAs) have received increasing attention due to their relatively low synthetic costs, the achievement of high efficiencies strongly depends on tedious pre- or/and post-treatments to refine the active layers, which in turn greatly increase fabrication complexity and expense of organic solar cells (OSCs). Nowadays most of the available as-cast devices based on NFREAs are below 12% efficiencies. Herein, phenylalkyl category side groups (CnPh) are employed to construct new NFREAs named BOR-CnPh (n = 3, 4, and 6), which exhibit inherently decent molecular aggregation and thus exclude additional treatments from device fabrication. The modified alkyl spacers of CnPh side groups not only trigger different aggregation of the acceptors, but also regulate the interaction conformations of donor (D) and acceptor (A), and thus D/A interactions. Encouragingly, the pristine PBDB-T:BOR-C4Ph blend delivers intrinsic fibrous networks with dominating face-on orientation, which yields an optimal efficiency up to 13.12%, and ranks as the highest value among as-cast OSCs based on NFREAs. This research provides a practical strategy to control molecular aggregations, interactions, and pristine heterojunction morphologies for easily available and high-performance organic photovoltaics.     

Emerging Chemistry in Enhancing the Chemical and Photochemical Stabilities of Fused-Ring Electron Acceptors in Organic Solar Cells

The power conversion efficiency of organic solar cells (OSCs) has made exceptionally rapid progress in the past five years owing to the emergence of fused-ring electron acceptors (FREAs). To achieve the commercialization, it is urgent to resolve the stability issues of OCSs from materials to devices. In particular, the state-of-the-art FREAs, often synthesized by Knoevenagel condensation, generally contain two exocyclic vinyl groups (CC bond) as the conjugated bridges, which inevitably exhibit an obvious electron-deficient characteristic due to the strong push-pull electronic effect. As a result, these vinyl bridges are vulnerable to nucleophile attacking and/or photooxidation, leading to poor chemical and photochemical stabilities of FREAs that easily cause the degradation of device performance. In this perspective, an in-depth understanding of the degradation mechanism of FREAs is provided, and then effective strategies reported recently are reviewed for improving the chemical and photochemical stabilities of FREAs from interfacial engineering to molecular engineering to additive engineering. Finally, a conclusion and outlook for the future design of highly efficient and stable FREAs are also presented.     

Ternary Polymer Solar Cells with High Efficiency of 14.24% by Integrating Two Well‐Complementary Nonfullerene Acceptors

Ternary polymer solar cells (PSCs) are one of the most promising device architectures that maintains the simplicity of single‐junction devices and provides an important platform to better tailor the multiple performance parameters of PSCs. Herein, a ternary PSC system is reported employing a wide bandgap polymeric donor (PBTA‐PS) and two small molecular nonfullerene acceptors (labeled as LA1 and 6TIC). LA1 and 6TIC keep not only well‐matched absorption profiles but also the rational crystallization properties. As a result, the optimal ternary PSC delivers a state of the art power conversion efficiency (PCE) of 14.24%, over 40% higher than the two binary devices, resulting from the prominently increased short‐circuit current density (J_sc) of 22.33 mA cm^?2, moderate open‐circuit voltage (V_oc) of 0.84 V, and a superior fill factor approaching 76%. Notably, the outstanding PCE of the ternary PSC ranks one of the best among the reported ternary solar cells. The greatly improved performance of ternary PSCs mainly derives from combining the complementary properties such as absorption and crystallinity. This work highlights the great importance of the rational design of matched acceptors toward highly efficient ternary PSCs.