Fullerene acceptors typically possess excellent electron-transporting properties and can work as guest components in ternary organic solar cells to enhance the charge extraction and efficiencies. However, conventional fullerene small molecules typically suffer from undesirable segregation and dimerization, thus limiting their applications in organic solar cells. Herein we report the use of a poly(fullerene-alt-xylene) acceptor (PFBO-C12) as guest component enables a significant efficiency increase from 16.9% for binary cells to 18.0% for ternary all-polymer solar cells. Ultrafast optic and optoelectronic studies unveil that PFBO-C12 can facilitate hole transfer and suppress charge recombination. Morphological investigations show that the ternary blends maintain a favorable morphology with high crystallinity and smaller domain size. Meanwhile, the introduction of PFBO-C12 reduces voltage loss and enables all-polymer solar cells with excellent light stability and mechanical durability in flexible devices. This work demonstrates that introducing polyfullerenes as guest components is an effective approach to achieving highly efficient ternary all-polymer solar cells with good stability and mechanical robustness.

Electron transporting materials (ETMs) play vital roles in determining the efficiency and stability of inverted perovskite solar cells. The widely used PCBM is prone to undesirable aggregation and migration in a cell, thus impairing device stability. In this work, we develop a new type of ETMs by polymerizing C60 fullerene with an aromantic linker unit. The resultant polyfullerene (PFBS-C12) not only maintains the good optoelectronic properties of fullerenes, but also can address the aforementioned aggregation problem of PCBM. The polyfullerene-based blade-coated cells exhibit a high efficiency of 23.2 % and good device stability that maintain 96 % of initial efficiency after > 1300-hour light soaking. An aperture efficiency of 18.9 % is also achieved on a 53.6-cm 2 perovskite mini-module. This work provides a new strategy for designing ETMs that retain the key figure-of-merits of conventional fullerene molecules and enable more stable perovskite solar devices simultaneously.

The elaborate balance between the open‐circuit voltage (VOC) and the short‐circuit current density (JSC) is critical to ensure efficient organic solar cells (OSCs). Herein, the chalcogen containing branched chain engineering is employed to address this dilemma. Three novel nonfullerene acceptors (NFAs), named BTP‐2O, BTP‐O‐S, and BTP‐2S, featuring different peripheral chalcogen containing branched chains are synthesized. Compared with symmetric BTP‐2O and BTP‐2S grafting two alkoxy or alkylthio branched chains, the asymmetric BTP‐O‐S grafting one alkoxy and one alkylthio branched chains shows mediate absorption range, applicable miscibility, and favorable crystallinity. Benefiting from the enhanced π–π stacking and charge transport, an optimal power conversion efficiency (PCE) of 17.3% is obtained for the PM6:BTP‐O‐S‐based devices, with a good balance between VOC (0.912 V) and JSC (24.5 mA cm−2), and a high fill factor (FF) of 0.775, which is much higher than those of BTP‐2O (16.1%) and BTP‐2S‐based (16.4%) devices. Such a result represents one of the highest efficiencies among the binary OSCs with VOC surpassing 0.9 V. Moreover, the BTP‐O‐S‐based devices fabricated by using green solvent yield a satisfactory PCE of 17.1%. This work highlights the synergistic effect of alkoxy and alkylthio branched chains for high‐performance OSCs by alleviating voltage loss and enhancing FF.

A group of regioregular polymer acceptors is synthesized by polymerizing Y6 moieties with different linker units including thiophene, vinylene, 2,2'-bithiophene, and thieno[3,2-b]thiophene, and their optoelectrical properties and photovoltaic performances are studied systematically. It is found that the linker units have significant impacts on the backbone planarity, conjugation, and hence optoelectrical properties of polymer acceptors. The vinylene-based PYF-V-o polymer shows a smaller dihedral angle between the end groups and vinylene units and a more rigid polymer backbone, thus affording bathochromic absorption and better electron-transporting capacity. As a result, the PM6:PYF-V-o based all-polymer solar cells (all-PSCs) are able to achieve the highest power conversion efficiency of 16.4% with an unprecedented small voltage loss of 0.49 V. Moreover, the PM6:PYF-V-o blend exhibits good resistance to environmental stressors and the air-processed PM6:PYF-V-o cells can still maintain a high efficiency of 16.1%, which is the best air-processed all-PSC efficiency reported to date. This study provides the structural-property guidance that can be used to facilitate the development of polymer acceptors for all-PSCs.

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