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The power conversion efficiency (PCE) of organic solar cells (OSCs) is improved dramatically in recent years and now approaches >19% for single‐junction cells and >20% for tandem cells. Therefore, the practical use of OSCs is becoming a reality. This perspective summarizes the state of the art of OSC characteristics and discusses the challenges that remain in further improving PCE. The short‐circuit current density (J SC) of the state‐of‐the‐art OSCs almost approaches 30 mA cm−2. As the internal quantum efficiencies of these devices exceed 90%, for further improvement in J SC, it is necessary to suppress reflection at interfaces and increase the active layer thickness to absorb as many photons as possible. Further suppression of the nonradiative voltage loss is imperative, as there is still large room for improvement compared to inorganic and perovskite counterparts. Hence, increasing the exciton lifetime and photoluminescence quantum yield of nonfullerene acceptors are pivotal to improving the open‐circuit voltage of OSCs. The fill factors of the latest OSCs approach 80%; however, because the optimized active layer thickness remains ≈100 nm, further suppression of bimolecular charge recombination is needed. Finally, this perspective discusses to what extent PCE can be improved and what can be done to achieve this.

Simultaneously controlling defects and film morphology at the buried interface is a promising approach to improve the power conversion efficiency (PCE) of inverted perovskite solar cells (PSCs). Here, two new donor‒acceptor type semiconductive covalent organic frameworks (COFs) are developed, COF TPA and COF ICZ . The carefully designed COFs structure not only effectively regulates the morphology and defects of the buried interface film, but also realizes the alignment with the energy level of the perovskite film and enhances the extraction and transmission of the interface charge. Among them, COF ICZ -treated inverted PSCs achieved a maxmum PCE of 25.68% (certified 25.14%), the inverted PCE reached a minimum PCE of 22.92% for 1 cm 2 device. The efficiency of inverted PSCs with a 1.68 eV wide bandgap reached 22.92%, which is the highest datum of the reported 1.68 eV wide bandgap PSC. This lays the groundwork for the commercialization of perovskite/silicon tandem solar cells. Additionally, the unencapsulated devices demonstrated a high degree of stability during operational use and when subjected to conditions of high humidity and temperature., (© 2024 Wiley‐VCH GmbH.)

At present, a variety of benzo[1,2‐b:4,5‐b′]dithiophene (BDT)‐based polymer donors are designed and synthesized, which have made great progress toward achieving high power conversion efficiencies (PCEs) of polymer solar cells (PSCs). Despite many advantages of benzo[1,2‐b:4,5‐b′]difuran (BDF) compared with BDT unit, the overall performance of BDF polymer‐based PSCs lags far behind that of the counterpart BDT‐based polymers. Recently, great advances have been achieved in BDF polymer‐based PSCs with the highest PCEs over 16%, suggesting that BDF‐based polymers have the significant potential to catch up or even surpass the performance of BDT‐based polymers. In this review, the recent advances of BDF polymers in PSCs are first summarized and then the design strategies and the chemical structure–performance relationships of BDF polymers are discussed. Finally, perspectives on the future development of BDF polymers for high‐efficiency PSCs are provided.

Perovskite solar cells (PSCs) have achieved revolutionary progress during the past decades with a rapidly boosting rate in power conversion efficiencies from 3.8% to 26.1%. However, high-efficiency PSCs with organic hole-transporting materials (HTMs) suffer from inferior long-term stability and high costs. The replacement of organic HTMs with inorganic counterparts such as metal oxides can solve the above-mentioned problems to realize highly robust and cost-effective PSCs. Nevertheless, the widely used simple metal oxide-based HTMs are limited by the low conductivity and poor light transmittance due to the fixed atomic environment. As an emerging family of inorganic HTMs, complex metal oxides with superior structural/compositional flexibility have attracted rapidly increasing interest recently, showing superior carrier conductivity/mobility and superb light transmittance. Herein, the recent advancements in the design and development of complex metal oxide-based HTMs for high-performance PSCs are summarized by emphasizing the superiority of complex metal oxides as HTMs over simple metal oxide-based counterparts. Consequently, several distinct strategies for the design of complex metal oxide-based HTMs are proposed. Last, the future directions and remaining challenges of inorganic complex metal oxide-based HTMs for PSCs are also presented. This review aims to provide valuable guidelines for the further advancements of robust, high-efficiency, and low-cost PSCs., (© 2024 Wiley‐VCH GmbH.)

Restricted by the energy-gap law, state-of-the-art organic solar cells (OSCs) exhibit relatively low open-circuit voltage (V OC ) because of large nonradiative energy losses (ΔE nonrad ). Moreover, the trade-off between V OC and external quantum efficiency (EQE) of OSCs is more distinctive; the power conversion efficiencies (PCEs) of OSCs are still <15% with V OC s of >1.0 V. Herein, the electronic properties and aggregation behaviors of non-fullerene acceptors (NFAs) are carefully considered and then a new NFA (Z19) is delicately designed by simultaneously introducing alkoxy and phenyl-substituted alkyl chains to the conjugated backbone. Z19 exhibits a hypochromatic-shifted absorption spectrum, high-lying lowest unoccupied molecular orbital energy level and ordered 2D packing mode. The D18:Z19-based blend film exhibits favorable phase separation with face-on dominated molecular orientation, facilitating charge transport properties. Consequently, D18:Z19 binary devices afford an exciting PCE of 19.2% with a high V OC of 1.002 V, surpassing Y6-2O-based devices. The former is the highest PCE reported to date for OSCs with V OC s of >1.0 V. Moreover, the ΔE nonrad of Z19- (0.200 eV) and Y6-2O-based (0.155 eV) devices are lower than that of Y6-based (0.239 eV) devices. Indications are that the design of such NFA, considering the energy-gap law, could promote a new breakthrough in OSCs., (© 2024 Wiley‐VCH GmbH.)

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., (© 2024 Wiley‐VCH GmbH.)

Organic solar cells (OSCs) are a promising low-cost thin-film photovoltaic technology while the fabrication of transparent conductive oxide (TCO) and metal electrodes still remains a factor that hinders the scaling-up and commercialization of OSCs. Carbon-based materials are regarded as potential alternatives due to their excellent properties, such as low cost, solution processibility, high conductance, and good chemical stability. In this mini-review, the recent progress of carbon-based materials such as graphite, carbon nanosheets, graphene, and carbon nanotubes to replace the TCO and metal electrodes of OSCs is surveyed. The preparation methods of different carbon-based materials are also discussed. Based on current progress, we summarize the outlooks and challenges of carbon-based electrodes. We anticipate this mini-review will inspire more research efforts to develop high-performance and OSC-matched carbon materials for more efficient and stable carbon-electrode-based OSCs., (© 2023 Wiley-VCH GmbH.)

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., (© 2022 The Authors. Advanced Science published by Wiley-VCH GmbH.)

Recently, the strategy of polymerized small-molecule acceptors (PSMAs) has attracted extensive attention for applications in all-polymer solar cells (all-PSCs). Although side-chain engineering is considered as a simple and effective strategy for manipulating polymer properties, the corresponding effect on photovoltaic performance of PSMAs in all-PSCs has not been systemically investigated. Herein, a series of PSMAs based on the benzotriazole (BTz)-core fused SMAs with different N-alkyl chains including branched 2-butyloctyl, linear n-octyl, and methyl on the BTz unit, namely PZT-C12, PZT-C8, and PZT-C1, respectively, is presented. Comparative studies show that the size of alkyl chains has a significant impact on the solid-state behavior of PZT polymers, which in turn affects their light absorption and charge transporting capacities, and subsequently the all-PSC performances. When combining with the polymer donor PBDB-T, PZT-C1 affords a champion power conversion efficiency of 14.9%, compared to 13.1% of PZT-C12, and 13.8% of PZT-C8 in the resultant all-PSCs, mainly benefiting from its better crystallinity and the more favorable blend morphology. This work emphasizes the importance of optimizing side-chain substituents on PSMAs for improving the device efficiency of all-PSCs., (© 2022 Wiley-VCH GmbH.)

Although the rapid development of polymer solar cells (PSCs) has been achieved, it is still a great challenge to explore efficient ways for improving power conversion efficiency (PCE) of PSCs from materials and device engineering. Ternary strategy has been confirmed as an efficient way to improve PCE of PSCs by employing three kinds of materials. In this work, one polymer donor PM6, and two non-fullerene materials N3 and MF1 are selected to prepare ternary PSCs with layer-by-layer (LbL) or bulk-heterojunction (BHJ) structure. The LbL and BHJ-PSCs exhibit PCEs of 16.75% and 16.76% with 15 wt% MF1 content in acceptors, corresponding to over 5% or 4% PCE improvement compared with N3-based binary PSCs with LbL or BHJ structure. The PCE improvement is mainly attributed to the fill factor enhancement from 73.29% to 76.95% for LbL-PSCs or from 74.13% to 77.51% for BHJ-PSCs by employing the ternary strategy. This work indicates that ternary strategy has great potential in preparing highly efficient LbL-PSCs via simultaneously optimizing molecular arrangement and the thickness of each layer., (© 2021 Wiley-VCH GmbH.)

All-polymer solar cells (all-PSCs) progressed tremendously due to recent advances in polymerized small molecule acceptors (PSMAs), and their power conversion efficiencies (PCEs) have exceeded 15 %. However, the practical applications of all-PSCs are still restricted by a lack of PSMAs with a broad absorption, high electron mobility, low energy loss, and good batch-to-batch reproducibility. A multi-selenophene-containing PSMA, PFY-3Se, was developed based on a selenophene-fused SMA framework and a selenophene π-spacer. Compared to its thiophene analogue PFY-0Se, PFY-3Se shows a ≈30 nm red-shifted absorption, increased electron mobility, and improved intermolecular interaction. In all-PSCs, PFY-3Se achieved an impressive PCE of 15.1 % with both high short-circuit current density of 23.6 mA cm -2 and high fill factor of 0.737, and a low energy loss, which are among the best values in all-PSCs reported to date and much better than PFY-0Se (PCE=13.0 %). Notably, PFY-3Se maintains similarly good batch-to-batch properties for realizing reproducible device performance, which is the first reported and also very rare for the PSMAs. Moreover, the PFY-3Se-based all-PSCs show low dependence of PCE on device area (0.045-1.0 cm 2 ) and active layer thickness (110-250 nm), indicating the great potential toward practical applications., (© 2021 Wiley-VCH GmbH.)

Over the past few years, non-fullerene organic solar cells have been a focus of research and their power conversion efficiencies have been improved dramatically from about 6 % to over 14 %. In addition to innovations in non-fullerene acceptors, the ongoing development of polymer donors has contributed significantly to the rapid progress of non-fullerene organic solar cell performance. This Minireview highlights the polymer donors that enable high-performance non-fullerene organic solar cells. We show the impressive photovoltaic devices results achieved by some of important classes of conjugated polymer systems in non-fullerene organic solar cells. We discuss the molecular design strategies as far as developing matching polymer donors for non-fullerene acceptors. We conclude with a brief summary and outlook for advances in donor polymers required for commercialization., (© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The 2D asymmetric benzodithiophene (BDT) unit is used as a donor unit to construct one new polymer PBDTBDD-Th with benzo[1,2-c:4,5-c']dithiophene-4,8-dione (BDD) as acceptor building block. In comparison to the polymer PBDTsTh-BDD with a side chain containing a sulfur atom, the devices based on PBDTBDD-Th/ITIC show better performance due to the introduction of carbon atoms in the side chain, which could weaken the self-aggregations of polymer chains. As a result, the devices based on PBDTBDD-Th/ITIC blends yield power conversion efficiencies (PCEs) over 10%, much higher than those based on PBDTsTh-BDD/ITIC blends (7.09%). The exciton dissociation probabilities (P diss ) of a device based on PBDTBDD-Th/ITIC blends is 95.3%, which suggests that the device achieves good exciton dissociation and charge transfer. In general, the polymer PBDTBDD-Th shows capability to increase the PCEs of polymer solar cells (PSCs) with a non-fullerene acceptor., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A novel small molecule acceptor MeIC with a methylated end-capping group is developed. Compared to unmethylated counterparts (ITCPTC), MeIC exhibits a higher lowest unoccupied molecular orbital (LUMO) level value, tighter molecular packing, better crystallites quality, and stronger absorption in the range of 520-740 nm. The MeIC-based polymer solar cells (PSCs) with J71 as donor, achieve high power conversion efficiency (PCE), up to 12.54% with a short-circuit current (J SC ) of 18.41 mA cm -2 , significantly higher than that of the device based on J71:ITCPTC (11.63% with a J SC of 17.52 mA cm -2 ). The higher J SC of the PSC based on J71:MeIC can be attributed to more balanced μ h /μ e , higher charge dissociation and charge collection efficiency, better molecular packing, and more proper phase separation features as indicated by grazing incident X-ray diffraction and resonant soft X-ray scattering results. It is worth mentioning that the as-cast PSCs based on MeIC also yield a high PCE of 11.26%, which is among the highest value for the as-cast nonfullerene PSCs so far. Such a small modification that leads to so significant an improvement of the photovoltaic performance is a quite exciting finding, shining a light on the molecular design of the nonfullerene acceptors., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Two 1D-2D asymmetric benzodithiophenes (BDTs) as donor building blocks are designed and synthesized, combining the advantages of both 1D and 2D symmetric BDTs. The photovoltaic properties of the asymmetric BDT-based polymers are improved greatly in comparison with corresponding symmetric BDT-based polymers. This work provides a new approach to design prospective organic optoelectronic materials employing the symmetry-breaking strategy., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Conjugated acceptor-donor-acceptor small molecules using different electron linkers are designed, synthesized, and used in organic solar cells. All of these small molecules show high photoconversion efficiencies (PCEs), ranging from 3.18-6.15% under simulated AM 1.5G condition. A maximum PCE of 6.15% combined with a high Voc of 0.85 V, a Jsc of 10.79 mA cm(-2) and a notable FF of 67.1% are achieved with T3/PC71 BM blend based devices using polydimethylsiloxane as additive., (Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)