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1.
    
Currently, high-performance polymerized small-molecule acceptors (PSMAs) based on ADA-type SMAs are still rare and greatly demanded for polymer solar cells (PSCs). Herein, two novel regioregular PSMAs (PW-Se and PS-Se) are designed and synthesized by using centrosymmetric (linear-shaped) and axisymmetric (banana-shaped) ADA-type SMAs as the main building blocks, respectively. It is demonstrated that photovoltaic performance of the PSMAs can be significantly improved by optimizing the configuration of ADA-type SMAs. Compared to the axisymmetric SMA-based polymer (PS-Se), PW-Se using a centrosymmetric SMA as the main building block exhibits better backbone coplanarity thereby resulting in bathochromically shifted absorption with a higher absorption coefficient, tighter interchain π–π stacking, and more favorable blend film morphology. As a result, enhanced and more-balanced charge transport, better exciton dissociation, and reduced charge recombination are achieved for PW-Se-based devices with PM6 as polymer donor. Benefiting from these positive factors, the optimal PM6:PW-Se-based device exhibits a higher power conversion efficiency (PCE) of 15.65% compared to the PM6:PS-Se-based device (8.90%). Furthermore, incorporation of PW-Se as a third component in the binary active layer of PM6:M36 yields ternary devices with an outstanding PCE of 18.0%, which is the highest value for PSCs based on ADA-type SMAs, to the best of the knowledge.  相似文献   

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Improving the fill factor (FF) is known as a challenging issue in organic solar cells (OSCs). Herein, a strategy of extending the conjugated area of end‐group is proposed for the molecular design of acceptor–donor–acceptor (A–D–A)‐type small molecule acceptor (SMA), and an indaceno[1,2‐b:5,6‐b′]dithiophene‐based SMA, namely IDTN, by end‐capping with the naphthyl fused 2‐(3‐oxocyclopentylidene)malononitrile is synthesized. Benefiting from the π‐conjugation extension by fusing two phenyls, IDTN shows stronger molecular aggregation, more ordered packing structure, thus over one order of magnitude higher electron mobility relative to its counterpart. By utilizing the fluorinated polymer (PBDB‐TF) as the electron donor, the corresponding device exhibits a high efficiency of 12.2% with a record‐high FF of 0.78, which is approaching the theoretical limit of OSCs. Compared with the reference molecule, such a high FF in the IDTN system can be mainly attributed to the more ordered π–π packing of acceptor aggregates, higher domain purity and symmetric carrier transport in the blend. Hence, enlarging the conjugated area of the terminal‐group in these A–D–A‐type SMAs is a promising approach not only for enhancing the electron mobility, but also for improving the blend morphology, and both of them are conducive to the fill‐factor breakthrough.  相似文献   

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A new polymer acceptor, naphthodiperylenetetraimide‐vinylene (NDP‐V), featuring a backbone of altenating naphthodiperylenetetraimide and vinylene units is designed and applied in all‐polymer solar cells (all‐PSCs). With this polymer acceptor, a new record power‐conversion efficiencies (PCE) of 8.59% has been achieved for all‐PSCs. The design principle of NDP‐V is to reduce the conformational disorder in the backbone of a previously developed high‐performance acceptor, PDI‐V, a perylenediimide‐vinylene polymer. The chemical modifications result in favorable changes to the molecular packing behaviors of the acceptor and improved morphology of the donor–acceptor (PTB7‐Th:NDP‐V) blend, which is evidenced by the enhanced hole and electron transport abilities of the active layer. Moreover, the stronger absorption of NDP‐V in the shorter‐wavelength range offers a better complement to the donor. All these factors contribute to a short‐circuit current density (J sc) of 17.07 mA cm?2. With a fill factor (FF) of 0.67, an average PCE of 8.48% is obtained, representing the highest value thus far reported for all‐PSCs.  相似文献   

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Recent advances in the development of polymerized A–D–A-type small-molecule acceptors (SMAs) have promoted the power conversion efficiency (PCE) of all-polymer solar cells (all-PSCs) over 13%. However, the monomer of an SMA typically consists of a mixture of three isomers due to the regio-isomeric brominated end groups (IC-Br(in) and IC-Br(out)). In this work, the two isomeric end groups are successfully separated, the regioisomeric issue is solved, and three polymer acceptors, named PY-IT, PY-OT, and PY-IOT, are developed, where PY-IOT is a random terpolymer with the same ratio of the two acceptors. Interestingly, from PY-OT, PY-IOT to PY-IT, the absorption edge gradually redshifts and electron mobility progressively increases. Theory calculation indicates that the LUMOs are distributed on the entire molecular backbone of PY-IT, contributing to the enhanced electron transport. Consequently, the PM6:PY-IT system achieves an excellent PCE of 15.05%, significantly higher than those for PY-OT (10.04%) and PY-IOT (12.12%). Morphological and device characterization reveals that the highest PCE for the PY-IT-based device is the fruit of enhanced absorption, more balanced charge transport, and favorable morphology. This work demonstrates that the site of polymerization on SMAs strongly affects device performance, offering insights into the development of efficient polymer acceptors for all-PSCs.  相似文献   

6.
    
A cross-linking strategy can result in a three-dimensional network of interconnected chains for the copolymers, thereby improving their mechanical performance. In this work, a series of cross-linked conjugated copolymers, named PC2, PC5, and PC8, constructed with different ratios of monomers are designed and synthesized. For comparison, a random linear copolymer, PR2 is also synthesized based on the similar monomers. When blended with Y6 acceptor, the cross-linked polymers PC2, PC5, and PC8-based polymer solar cells (PSCs) achieve superior power conversion efficiencies (PCEs) of 17.58%, 17.02%, and 16.12%, respectively, which are higher than that (15.84%) of the random copolymer PR2-based devices. Moreover, the PCE of PC2:Y6-based flexible PSC retains ≈88% of the initial efficiency value after 2000 bending cycles, overwhelming the PR2:Y6-based device with the remaining 12.8% of the initial PCE. These results demonstrate that the cross-linking strategy is a feasible and facile approach to developing high-performance polymer donors for the fabrication of flexible PSCs.  相似文献   

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Here, a pair of A1–D–A2–D–A1 unfused ring core‐based nonfullerene small molecule acceptors (NF‐SMAs), BO2FIDT‐4Cl and BT2FIDT‐4Cl is synthesized, which possess the same terminals (A1) and indacenodithiophene unit (D), coupling with different fluorinated electron‐deficient central unit (difluorobenzoxadiazole or difluorobenzothiadiazole) (A2). BT2FIDT‐4Cl exhibits a slightly smaller optical bandgap of 1.56 eV, upshifted highest occupied molecular orbital energy levels, much higher electron mobility, and slightly enhanced molecular packing order in neat thin films than that of BO2FIDT‐4Cl . The polymer solar cells (PSCs) based on BT2FIDT‐4Cl:PM7 yield the best power conversion efficiency (PCE) of 12.5% with a Voc of 0.97 V, which is higher than that of BO2FIDT‐4Cl ‐based devices (PCE of 10.4%). The results demonstrate that the subtle modification of A2 unit would result in lower trap‐assisted recombination, more favorable morphology features, and more balanced electron and hole mobility in the PM7:BT2FIDT‐4Cl blend films. It is worth mentioning that the PCE of 12.5% is the highest value in nonfused ring NF‐SMA‐based binary PSCs with high Voc over 0.90 V. These results suggest that appropriate modulation of the quinoid electron‐deficient central unit is an effective approach to construct highly efficient unfused ring NF‐SMAs to boost PCE and Voc simultaneously.  相似文献   

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Compared with the quick development of polymer solar cells, achieving high‐efficiency small‐molecule solar cells (SMSCs) remains highly challenging, as they are limited by the lack of matched materials and morphology control to a great extent. Herein, two small molecules, BSFTR and Y6, which possess broad as well as matched absorption and energy levels, are applied in SMSCs. Morphology optimization with sequential solvent vapor and thermal annealing makes their blend films show proper crystallinity, balanced and high mobilities, and favorable phase separation, which is conducive for exciton dissociation, charge transport, and extraction. These contribute to a remarkable power conversion efficiency up to 13.69% with an open‐circuit voltage of 0.85 V, a high short‐circuit current of 23.16 mA cm?2 and a fill factor of 69.66%, which is the highest value among binary SMSCs ever reported. This result indicates that a combination of materials with matched photoelectric properties and subtle morphology control is the inevitable route to high‐performance SMSCs.  相似文献   

10.
    
A conjugated small molecule containing a benzodithiophene unit shows high performance in bulk heterojunction (BHJ) solar cells. Using the simple solution spinning process, a high PCE is achieved by employing this molecule as the donor in BHJ solar cells.  相似文献   

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Nonfullerene polymer solar cells develop quickly. However, nonfullerene small‐molecule solar cells (NF‐SMSCs) still show relatively inferior performance, attributing to the lack of comprehensive understanding of the structure–performance relationship. To address this issue, two isomeric small‐molecule acceptors, NBDTP‐Fout and NBDTP‐Fin, with varied oxygen position in the benzodi(thienopyran) (BDTP) core are designed and synthesized. When blended with molecular donor BDT3TR‐SF, devices based on the two isomeric acceptors show disparate photovoltaic performance. Fabricated with an eco‐friendly processing solvent (tetrahydrofuran), the BDT3TR‐SF:NBDTP‐Fout blend delivers a high power conversion efficiency of 11.2%, ranked to the top values reported to date, while the BDT3TR‐SF:NBDTP‐Fin blend almost shows no photovoltaic response (0.02%). With detailed investigations on inherent optoelectronic processes as well as morphological evolution, this performance disparity is correlated to the interfacial tension of the two combinations and concludes that proper interfacial tension is a key factor for effective phase separation, optimal blend morphology, and superior performance, which can be achieved by the “isomerization” design on molecular acceptors. This work reveals the importance of modulating the materials miscibility by interfacial‐tension‐oriented molecular design, which provides a general guideline toward efficient NF‐SMSCs.  相似文献   

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Small molecule solar cells (SMSCs) lag a long way behind polymer solar cells. A key limit is the less controllable morphology of small molecule materials, which can be aggravated when incorporating anisotropic nonfullerene acceptors. To fine‐tune the blending morphology within SMSCs, a π‐conjunction curtailing design is applied, which produces a efficient benzodithionopyran‐cored molecular acceptor for nonfullerene SMSCs (NF‐SMSCs). When blended with a molecular donor BDT3TR‐SF to fabricate NF‐SMSCs, the π‐conjunction curtailed molecular acceptor NBDTP‐M obtains an optimal power conversion efficiency (PCE) of up to 10.23%, which is much higher than that of NBDTTP‐M of longer π‐conjunction. It retains 93% of the PCE of devices fabricated in a glove box when all spin‐coating and post‐treating procedures are conducted in ambient air with relative humidity of 25%, which suggests the good air‐processing capability of π‐conjunction curtailed molecules. Detailed X‐ray scattering investigations indicate that the BDT3TR‐SF:NBDTP‐M blend exhibits a blend morphology featuring fine interpenetrating networks with smaller domains and higher phase purity, which results in more efficient charge generation, more balanced charge transport, and less recombination compared to the low‐performance BDT3TR‐SF:NBDTTP‐M blend. This work provides a guideline for molecular acceptors' design toward efficient, low‐cost, air‐processed NF‐SMSCs.  相似文献   

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Compared to the bulk heterojunction (BHJ) devices, the quasiplanar heterojunction (Q-PHJ) exhibits a more stable morphology and superior charge transfer performance. To achieve both high efficiency and long-term stability, it is necessary to design new materials for Q-PHJ devices. In this study, QxIC-CF3 and QxIC-CH3 are designed and synthesized for the first time. The trifluoromethylation of the central core exerts a modulatory effect on the molecular stacking pattern, leveraging the strong electrostatic potential and intermolecular interactions. Compared with QxIC-CH3, the single crystal structure reveals that QxIC-CF3 exhibits a more compact 2D linear stacking behavior. These benefits, combined with the separated electron and hole transport channels in Q-PHJ device, lead to increased charge mobility and reduced energy loss. The devices based on D18/QxIC-CF3 exhibit an efficiency of 18.1%, which is the highest power conversion efficiency (PCE) for Q-PHJ to date. Additionally, the thermodynamic stability of the active layer morphology enhances the lifespan of the aforementioned devices under illumination conditions. Specifically, the T80 is 420 h, which is nearly twice that of the renowned Y6-based BHJ device (T80 = 220 h). By combining the advantages of the trifluoromethylation and Q-PHJ device, efficient and stable organic solar cell devices can be constructed.  相似文献   

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Active layer material plays a critical role in promoting the performance of an organic solar cell (OSC). Small-molecule (SM) materials have the merits of well-defined chemical structures, few batch-to-batch variations, facile synthesis and purification procedures, and easily tuned properties. SM-donor and non-fullerene acceptor (NFA) innovations have recently produced all-small-molecule (ASM) devices with power conversion efficiencies that exceed 17% and approach those of their polymer-based counterparts, thereby demonstrating their great future commercialization potential. In this review, recent progress in both SM donors and NFAs to illustrate structure–property relationships and various morphology-regulation strategies are summarized. Finally, ASM-OSC challenges and outlook are discussed.  相似文献   

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All‐polymer solar cells (all‐PSCs) based on n‐ and p‐type polymers have emerged as promising alternatives to fullerene‐based solar cells due to their unique advantages such as good chemical and electronic adjustability, and better thermal and photochemical stabilities. Rapid advances have been made in the development of n‐type polymers consisting of various electron acceptor units for all‐PSCs. So far, more than 200 n‐type polymer acceptors have been reported. In the last seven years, the power conversion efficiency (PCE) of all‐PSCs rapidly increased and has now surpassed 10%, meaning they are approaching the performance of state‐of‐the‐art solar cells using fullerene derivatives as acceptors. This review discusses the design criteria, synthesis, and structure–property relationships of n‐type polymers that have been used in all‐PSCs. Additionally, it highlights the recent progress toward photovoltaic performance enhancement of binary, ternary, and tandem all‐PSCs. Finally, the challenges and prospects for further development of all‐PSCs are briefly considered.  相似文献   

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19.
    
Understanding the conformation effect on molecular packing, miscibility, and photovoltaic performance is important to open a new avenue for small‐molecule acceptor (SMA) design. Herein, two novel acceptor–(donor‐acceptor1‐donor)–acceptor (A‐DA1D‐A)‐type asymmetric SMAs are developed, namely C‐shaped BDTP‐4F and S‐shaped BTDTP‐4F . The BDTP‐4F ‐based polymer solar cells (PSCs) with PM6 as donor, yields a power conversion efficiency (PCE) of 15.24%, significantly higher than that of the BTDTP‐4F ‐based device (13.12%). The better PCE for BDTP‐4F ‐based device is mainly attributed to more balanced charge transport, weaker bimolecular recombination, and more favorable morphology. Additionally, two traditional A‐D‐A‐type SMAs ( IDTP‐4F and IDTTP‐4F ) are also synthesized to investigate the conformation effect on morphology and device performance. Different from the device result above, here, IDTP‐4F with S‐shape conformation outperforms than IDTTP‐4F with C‐shape conformation. Importantly, it is found that for these two different types of SMA, the better performing binary blend has similar morphological characteristics. Specifically, both PM6:BDTP‐4F and PM6:IDTP‐4F blend exhibit perfect nanofibril network structure with proper domain size, obvious face‐on orientation and enhance donor‐acceptor interactions, thereby better device performance. This work indicates tuning molecular conformation plays pivotal role in morphology and device effciciency, shining a light on the molecular design of the SMAs.  相似文献   

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Optimizing the molecular structures of organic photovoltaic (OPV) materials is one of the most effective methods to boost power conversion efficiencies (PCEs). For an excellent molecular system with a certain conjugated skeleton, fine tuning the alky chains is of considerable significance to fully explore its photovoltaic potential. In this work, the optimization of alkyl chains is performed on a chlorinated nonfullerene acceptor (NFA) named BTP-4Cl-BO (a Y6 derivative) and very impressive photovoltaic parameters in OPV cells are obtained. To get more ordered intermolecular packing, the n-undecyl is shortened at the edge of BTP-eC11 to n-nonyl and n-heptyl. As a result, the NFAs of BTP-eC9 and BTP-eC7 are synthesized. The BTP-eC7 shows relatively poor solubility and thus limits its application in device fabrication. Fortunately, the BTP-eC9 possesses good solubility and, at the same time, enhanced electron transport property than BTP-eC11. Significantly, due to the simultaneously enhanced short-circuit current density and fill factor, the BTP-eC9-based single-junction OPV cells record a maximum PCE of 17.8% and get a certified value of 17.3%. These results demonstrate that minimizing the alkyl chains to get suitable solubility and enhanced intermolecular packing has a great potential in further improving its photovoltaic performance.  相似文献   

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