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All‐polymer solar cells have experienced rapid development in recent years by the emergence of polymerized small molecular acceptors (PSMAs). However, the strong chain entanglements of polymer donors (PDs) and polymer acceptors (PAs) decrease the miscibility of the resulting polymer mixtures, making it challenging to optimize the blend morphology. Herein, we designed three PAs, namely PBTPICm‐BDD, PBTPICγ‐BDD and PBTPICF‐BDD, by smartly using a BDD unit as the polymerized unit to copolymerize with different Y‐typed non‐fullerene small molecular acceptors (NF‐SMAs), thus achieving a certain degree of distortion and giving the polymer system enough internal space to reduce the entanglements of the polymer chains. Such effects increase the chances of the PD being interspersed into the acceptor material, which improve the solubility between the PD and PA. The PBTPICγ‐BDD and PBTPICF‐BDD displayed better miscibility with PBQx‐TCl, leading to a well optimized morphology. As a result, high power conversion efficiencies (PCEs) of 17.50 % and 17.17 % were achieved for PBQx‐TCl : PBTPICγ‐BDD and PBQx‐TCl : PBTPICF‐BDD devices, respectively. With the addition of PYFT‐o as the third component into PBQx‐TCl : PBTPICγ‐BDD blend to further extend the absorption spectral coverage and finely tune microstructures of the blend morphology, a remarkable PCE of 18.64 % was realized finally. [ABSTRACT FROM AUTHOR]

A double‐fibril network of the photoactive layer morphology is recognized as an ideal structure facilitating exciton diffusion and charge carrier transport for high‐performance organic solar cells (OSCs). However, in the layer‐by‐layer processed OSCs (LbL‐OSCs), polymer donors and small molecule acceptors (SMAs) are separately deposited, and it is challenging to realize a fibril network of pure SMAs with the absence of tight interchain entanglement as polymers. In this work, crystalline small molecule donors (SMDs), named TDZ‐3TR and SeDZ‐3TR, were designed and introduced into the L8‐BO acceptor solution, forcing the phase separation and molecular fibrilization. SeDZ‐3TR showed higher crystallinity and lower miscibility with L8‐BO acceptor than TDZ‐3TR, enabling more driving force to favor the phase separation and better molecular fibrilization of L8‐BO. On the other hand, two donor polymers of PM6 and D18 with different fibril widths and lengths were put together to optimize the fibril network of the donor layer. The simultaneously optimization of the acceptor and donor layers resulted in a more ideal double‐fibril network of the photoactive layer and an impressive power conversion efficiency (PCE) of 19.38 % in LbL‐OSCs. [ABSTRACT FROM AUTHOR]

Highlights: Alkyl-tailored Y-SMAs named YR-SeNF series with near-infrared absorption, different molecular crystallinity and self-assembly abilities are developed. The related organic solar cells (OSCs) with an active layer processed from halogen-free solvents and spin-coating-free technologies achieve a ~ 19% efficiency. Ternary OSCs offer a robust operating stability under MPP tracking and well-keep > 80% of the initial efficiency for even over 400 h. Power-conversion-efficiencies (PCEs) of organic solar cells (OSCs) in laboratory, normally processed by spin-coating technology with toxic halogenated solvents, have reached over 19%. However, there is usually a marked PCE drop when the blade-coating and/or green-solvents toward large-scale printing are used instead, which hampers the practical development of OSCs. Here, a new series of N-alkyl-tailored small molecule acceptors named YR-SeNF with a same molecular main backbone are developed by combining selenium-fused central-core and naphthalene-fused end-group. Thanks to the N-alkyl engineering, NIR-absorbing YR-SeNF series show different crystallinity, packing patterns, and miscibility with polymeric donor. The studies exhibit that the molecular packing, crystallinity, and vertical distribution of active layer morphologies are well optimized by introducing newly designed guest acceptor associated with tailored N-alkyl chains, providing the improved charge transfer dynamics and stability for the PM6:L8-BO:YR-SeNF-based OSCs. As a result, a record-high PCE approaching 19% is achieved in the blade-coating OSCs fabricated from a green-solvent o-xylene with high-boiling point. Notably, ternary OSCs offer robust operating stability under maximum-power-point tracking and well-keep > 80% of the initial PCEs for even over 400 h. Our alkyl-tailored guest acceptor strategy provides a unique approach to develop green-solvent and blade-coating processed high-efficiency and operating stable OSCs, which paves a way for industrial development. [ABSTRACT FROM AUTHOR]

The improvement of power conversion efficiency (PCE) and stability of the perovskite solar cell (PSC) is hindered by carrier recombination originating from the defects at the buried interface of the PSC. It is crucial to suppress the nonradiative recombination and facilitate carrier transfer in PSC via interface engineering. Herein, P‐biguanylbenzoic acid hydrochloride (PBGH) is developed to modify the tin oxide (SnO2)/perovskite interface. The effects of PBGH on carrier transportation, perovskite growth, defect passivation, and PSC performance are systematically investigated. On the one hand, the PBGH can effectively passivate the trap states of Sn dangling bonds and O vacancies on the SnO2 surface via Lewis acid/base coordination, which is conducive to improving the conductivity of SnO2 film and accelerating the electron extraction. On the other hand, PBGH modification assists the formation of high‐quality perovskite film with low defect density due to its strong interaction with PbI2. Consequently, the PBGH‐modified PSC exhibits a champion power conversion efficiency (PCE) of 24.79%, which is one of the highest PCEs among all the FACsPbI3‐based PSCs reported to date. In addition, the stabilities of perovskite films and devices under high temperature/humidity and light illumination conditions are also systematically studied. [ABSTRACT FROM AUTHOR]

A desired morphology is essential for achieving efficient polymer solar cells. Donors and acceptors with appropriate crystallization can lead to a suitable phase-separated morphology for effective photocurrent generation process. Inspired by the success of Y6 acceptors and the 2D side chain engineering on popular polymer donors and small molecule acceptors, the usage of unique 2D 3,4-ethylene dioxythiophene (EDOT) side chains on Y6 to regulate its crystallinity, compatibility, and thus the related blend morphology is explored. In this study, two molecules of BTP-EDOT-4F and BTP-EDOT-4Cl with such unique 2D EDOT side chains are designed and synthesized. Due to the advantage of EDOT side chain, when these molecules are blended with PM6, the decent power conversion efficiencies (PCEs) of 16.78% and 15.87% are obtained. Furthermore, BTP-EDOT-4F is selected as the third component and added into PM6:L8-BO binary system to form ternary blends. The optimized crystallinity, compatibility, and morphology of such ternary blend are discovered in the presence of BTP-EDOT-4F, which enables efficient exciton dissociation and charge transport as well as decreased recombination, resulting in higher short circuit current density Jsc) and fill factor. Finally, the outstanding PCE of 18.56% is achieved in ternary blends containing PM6, L8-BO, and BTP-EDOT-4F. [ABSTRACT FROM AUTHOR]

High density of defects at interface severely affects the performance of perovskite solar cells (PSCs). Herein, cobalt (II) hexafluoro‐2,4‐pentanedionat (CoFAc), a hinge‐type fluorine‐rich complex, is introduced onto the surface of formamidinium cesium lead iodide (FACsPbI3) film to address the issues of perovskite/Spiro‐OMeTAD interface. The existence of CoFAc passivates both organic cation and halide anion vacancies by establishing powerful hydrogen bonds with HC(NH2)2+ (FA+) and strong ionic bonds with Pb2+ in perovskite films. In addition, CoFAc serves as a connecting link to enhance interfacial hole‐transport kinetics via interacting with Spiro‐OMeTAD. Consequently, FACsPbI3 PSCs with CoFAc modification display a champion power conversion efficiency (PCE) of 24.64% with a charming open‐circuit voltage (VOC) of 1.191 V, which is the record VOC among all the reported organic‐inorganic hybrid PSCs with TiO2 as electron transport layer. Furthermore, CoFAc‐modified devices exhibit an outstanding long‐term stability, which can maintain 95% of their initial PCEs after exposure to ambient atmosphere for 1500 h without any encapsulation. [ABSTRACT FROM AUTHOR]

Constructing terpolymer has attracted increasing attention as a strategy to improve the performance of polymer solar cell. Terpolymer usually offers an opportunity to lower the frontier molecular orbital energy level, introduces additional absorption band and sometimes optimizes the morphology of the active blend. Generally, the additional segment in terpolymer backbone inevitably introduces backbone disorder, which causes entropy rises. However, selecting a suitable dipole unit introduces extra driving forces for crystallization by enhancing intermolecular interactions. This provides a handy knob for tradeoff between intermolecular interaction and backbone disorder, thus regulating the blend morphology. Herein, a high dipole and electron‐deficient group of pyrrolo[3,4‐f]benzotriazole‐5,7(6H)‐dione (TzBI) is incorporated into the high‐performance donor polymer and a series of terpolymers with different content of TzBI are designed. As expected, the morphology is optimized gradually for improving charge generation and charge transport, also suppressing charge recombination. The champion device with 10% TzBI exhibited a power conversion efficiency (PCE) of 18.36%, which is 5% increase compared to the controlled device. This study presents a charming terpolymer strategy by highly electron‐deficient and high dipole segment to realize a tradeoff between intermolecular interaction and backbone disorder, facilitating the optimization of morphology and elevation of fill factor and device efficiency. [ABSTRACT FROM AUTHOR]

Side‐chain engineering with heteroatoms is not only effective in tuning frontier molecular orbitals, but also possible for forming secondary bonds which can be utilized to planarize the molecular backbone, hence, improving the photon absorption as well as charge‐transport abilities of polymer solar‐cell (PSC) materials. Herein, two types of unconventional side chains, namely carboxylate and carbamate, containing various heteroatoms are introduced to the thiophene bridges in high performance benzodithiophene (BDT) based donor polymers to from the novel polymers PTzTz‐C and PTzTz‐N, respectively. In these polymers, non‐covalent O⋅⋅⋅S and N⋅⋅⋅H interactions induce a high tendency to aggregation. In a ternary‐blend PSC with PTzTz‐N added to the high‐performance D18 : BTP‐eC9 blend, complimentary absorption and improved thin‐film morphology were observed with a top power conversion efficiency of 18.76 %, which is an improvement of almost 5 % over the D18 : BTP‐eC9 binary blends. [ABSTRACT FROM AUTHOR]

Formamidinium methylammonium lead iodide (FAMAPbI3) perovskite has been intensively investigated as a potential photovoltaic material because it has higher phase stability than its pure FAPbI3 perovskite counterpart. However, its power conversion efficiency (PCE) is significantly inferior due to its high density of surface detects and mismatched energy level with electrodes. Herein, a bifunctional passivator, methyl haloacetate (methyl chloroacetate, (MClA), methyl bromoacetate (MBrA)), is designed to reduce defect density, to tune the energy levels and to improve interfacial charge extraction in the FAMAPbI3 perovskite cell by synergistic passivation of both CO groups and halogen anions. As predicted by modeling undercoordinated Pb2+, the MBrA shows a very strong interaction with Pb2+ by forming a dimer complex ([C6H10Br2O4Pb]2+), which effectively reduces the defect density of the perovskite and suppresses non‐radiative recombination. Meanwhile, the Br− in MBrA passivates iodine‐deficient defects. Consequently, the MBrA‐modified device presents an excellent PCE of 24.29%, an open‐circuit voltage (Voc) of 1.18 V (Voc loss ≈ 0.38 V), which is one of the highest PCEs among all FAMAPbI3‐based perovskite solar cells reported to date. Furthermore, the MBrA‐modified devices without any encapsulation exhibit remarkable long‐term stability with only 9% of PCE loss after exposure to ambient air for 1440 h. [ABSTRACT FROM AUTHOR]

The single bulk‐heterojunction active layer based on non‐fullerene acceptors (NFAs) has dominated the power conversional efficiencies above 18% in state‐of‐the‐art organic solar cells (OSCs). However, a deep understanding of the relationship between charge carrier process and film microstructure remains unclear for emerging NFA OSCs. Herein, with the superstar PM6:Y6 blend as a model, the charge generation process in active layers is successfully manipulated by designing three different film microstructures, and they are correlated with the final photovoltaic performance in OSC devices. The amount of intermediate intra‐moiety excited states from the nanoscale Y6 aggregates can be effectively enhanced by controlling the phase separation domains and film crystallinity in the bicontinuous PM6:Y6 networks. This robustly improves the hole transfer, and thus promotes charge generation. As a result, the optimal films show superior device performance, that is, the high efficiencies of 16.53% and 17.98% for PM6:Y6‐ and D18:Y6‐based single junction OSCs, respectively. The results presented here give a rational guide for optimizing the charge carrier process through controlling morphological microstructures toward high‐performance NFA OSCs. [ABSTRACT FROM AUTHOR]

A benzodithiophene-free donor polymer was designed for enabling 19.36% efficiency green-solvent-processable organic solar cells (OSCs), which is the highest value for OSCs processed by halogen-free solvents. [Display omitted] • A high molecular weight benzodithiophene-free donor polymer of PDTP-BDD was developed for organic solar cells. • The layer-by-layer processing of PDTP-BDD based devices in halogen-free solvents was studied. • The champion power conversion efficiency of 19.36% was achieved finally. In this work, a newly benzodithiophene-free D-A polymer donor, named PDTP-BDD, was developed for realizing green-solvent processed high-performance OSCs. By bridging two electron-rich unit of dithieno[3,2-b:2′,3′-d]pyridin-5(4H)-one (DTP) and electron-deficient benzo[1,2-c:4,5c′]dithiophene-4,8-dione (BDD) with thiophene units, PDTP-BDD possesses high absorption in the short wavelength range and a deep HOMO energy level. The rigid building blocks also make PDTP-BDD has strong aggregation and poor solubility in common halogen-free solvents (such as o -xylene) at room temperature, but it is readily dissolved and disaggregated at high temperature (120 °C). After cooling down to a lower temperature (60 °C), PDTP-BDD self-assembled and pre-aggregated slowly in the solution at a long time. By employing a delayed processing strategy in the layer-by-layer processed OSCs (LbL-OSCs), an optimized fibril network of the underling layer was realized, enabling the permeation of acceptor into the donor network. The optimized PDTP-BDD/L8-BO-based LbL-OSCs realized a high PCE of 18.42 %. By adding a small amount of D18 to further optimize the PDTP-BDD fibril network, an impressive PCE of 19.36 % was achieved finally in the resulting ternary LbL-OSCs, which is the highest value for OSCs processed by halogen-free solvents. [ABSTRACT FROM AUTHOR]