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Enhancing the luminescence property without sacrificing the charge collection is one key to high-performance organic solar cells (OSCs), while limited by the severe non-radiative charge recombination. Here, we demonstrate efficient OSCs with high luminescence via the design and synthesis of an asymmetric non-fullerene acceptor, BO-5Cl. Blending BO-5Cl with the PM6 donor leads to a record-high electroluminescence external quantum efficiency of 0.1%, which results in a low non-radiative voltage loss of 0.178 eV and a power conversion efficiency (PCE) over 15%. Importantly, incorporating BO-5Cl as the third component into a widely-studied donor:acceptor (D:A) blend, PM6:BO-4Cl, allows device displaying a high certified PCE of 18.2%. Our joint experimental and theoretical studies unveil that more diverse D:A interfacial conformations formed by asymmetric acceptor induce optimized blend interfacial energetics, which contributes to the improved device performance via balancing charge generation and recombination. High-performance organic solar cells call for novel designs of acceptor molecules. Here, He et al. design and synthesize a non-fullerene acceptor with an asymmetric structure for diverse donor:acceptor interfacial conformations and report a certificated power conversion efficiency of 18.2%.

Unveiling the correlations among molecular structures, morphological characteristics, macroscopic properties and device performances is crucial for developing better photovoltaic materials and achieving higher efficiencies. To achieve this goal, a comprehensive study is performed based on four state-of-the-art non-fullerene acceptors (NFAs), which allows to systematically examine the above-mentioned correlations from different scales. It’s found that extending conjugation of NFA shows positive effects on charge separation promotion and non-radiative loss reduction, while asymmetric terminals can maximize benefits from both terminals. Another molecular optimization is from alkyl chain tuning. The shortened alkyl side chain results in strengthened terminal packing and decreased π-π distance, which contribute high carrier mobility and finally the high charge collection efficiency. With the most-acquired benefits from molecular structure and macroscopic factors, PM6:BTP-S9-based organic photovoltaics (OPVs) exhibit the optimal efficiency of 17.56% (certified: 17.4%) with a high fill factor of 78.44%, representing the best among asymmetric acceptor based OPVs. This work provides insight into the structure-performance relationships, and paves the way toward high-performance OPVs via molecular design. Understanding correlations between molecular structures and macroscopic properties is critical in realising highly efficient organic photovoltaics. Here, the authors conduct a comprehensive study based on four non-fullerene acceptors revealing how the extended conjugation, asymmetric terminals and alkyl chain length can affect device performance.

Although the multiple-component (MC) blend strategy has been frequently used as a very effective way to improve the performance of organic solar cells (OSCs), there is a strong need to understand the fundamental working mechanism and material selection rule for achieving optimal MC-OSCs. Here we present the ‘dilution effect’ as the mechanism for MC-OSCs, where two highly miscible components are molecularly intermixed. Contrary to the aggregation-induced non-radiative decay, the dilution effect enables higher luminescence quantum efficiencies and open-circuit voltages (VOC) in MC-OSCs via suppressed electron–vibration coupling. The continuously broadened bandgap together with reduced electron–vibration coupling also explains the composition-dependent VOC in ternary blends well. Moreover, we show that electrons can transfer between different acceptors, depending on the energy offset between them, which contributes to the largely unperturbed charge transport and high fill factors in MC-OSCs. The discovery of the dilution effect enables the demonstration of a high power conversion efficiency of 18.31% in an MC-OSC.A strategy based on molecular intermixing of two highly miscible components enables the demonstration of high efficiency multiple-component organic solar cells.

HighlightsA solid additive-assisted layer-by-layer (SAA-LBL) processing was developed to facilitate the inter-diffusion between polymer donor and acceptor and optimize the morphology of quasi-planar heterojunction for high-performance organic solar cells (OSCs).The pre-phase separation between fatty acid and polymer donor, easily tuned via controlling the cohesive energy, is critical to form the desired vertical phase-separation morphology.The SAA-LBL is generally applicable to various OSC systems, and enables the record efficiency of 19.02% among the binary OSCs.Morphology is of great significance to the performance of organic solar cells (OSCs), since appropriate morphology could not only promote the exciton dissociation, but also reduce the charge recombination. In this work, we have developed a solid additive-assisted layer-by-layer (SAA-LBL) processing to fabricate high-efficiency OSCs. By adding the solid additive of fatty acid (FA) into polymer donor PM6 solution, controllable pre-phase separation forms between PM6 and FA. This intermixed morphology facilitates the diffusion of acceptor Y6 into the donor PM6 during the LBL processing, due to the good miscibility and fast-solvation of the FA with chloroform solution dripping. Interestingly, this results in the desired morphology with refined phase-separated domain and vertical phase-separation structure to better balance the charge transport /collection and exciton dissociation. Consequently, the binary single junction OSCs based on PM6:Y6 blend reach champion power conversion efficiency (PCE) of 18.16% with SAA-LBL processing, which can be generally applicable to diverse systems, e.g., the PM6:L8-BO-based devices and thick-film devices. The efficacy of SAA-LBL is confirmed in binary OSCs based on PM6:L8-BO, where record PCEs of 19.02% and 16.44% are realized for devices with 100 and 250 nm active layers, respectively. The work provides a simple but effective way to control the morphology for high-efficiency OSCs and demonstrates the SAA-LBL processing a promising methodology for boosting the industrial manufacturing of OSCs.

Although asymmetric molecular design has been widely demonstrated effective for organic photovoltaics (OPVs), the correlation between asymmetric molecular geometry and their optoelectronic properties is still unclear. To access this issue, we have designed and synthesized several symmetric-asymmetric non-fullerene acceptors (NFAs) pairs with identical physical and optoelectronic properties. Interestingly, we found that the asymmetric NFAs universally exhibited increased open-circuit voltage compared to their symmetric counterparts, due to the reduced non-radiative charge recombination. From our molecular-dynamic simulations, the asymmetric NFA naturally exhibits more diverse molecular interaction patterns at the donor (D):acceptor (A) interface as compared to the symmetric ones, as well as higher D:A interfacial charge-transfer state energy. Moreover, it is observed that the asymmetric structure can effectively suppress triplet state formation. These advantages enable a best efficiency of 18.80%, which is one of the champion results among binary OPVs. Therefore, this work unambiguously demonstrates the unique advantage of asymmetric molecular geometry, unveils the underlying mechanism, and highlights the manipulation of D:A interface as an important consideration for future molecular design. The correlation between asymmetric molecular geometry of non-fullerene acceptors and their optoelectronic properties was unclear. Here, the authors found asymmetric ones exhibit increased open-circuit voltage compared to their symmetric counterparts due to reduced non-radiative charge recombination.

The interfacial molecular dipole enhances the photovoltaic performance of perovskite solar cells (PSCs) by facilitating improved charge extraction. However, conventional self-assembled monolayers (SAMs) face challenges like inadequate interface coverage and weak dipole interactions. Herein, we develop a strategy using a self-assembled ferroelectric layer to modify the interfacial properties of PSCs. Specifically, we employ 1-adamantanamine hydroiodide (ADAI) to establish robust chemical interactions and create a dipole layer over the perovskite. The oriented molecular packing and spontaneous polarity of ferroelectric ADAI generate a substantial interfacial dipole, adjusting band bending at the anode, reducing band misalignment, and suppressing charge recombination. Consequently, our formamidinium lead iodide-based conventional PSC achieves efficiencies of 25.13% (0.06 cm 2 ) and 23.5% (1.00 cm 2 ) while exhibiting enhanced stability. Notably, we demonstrate an impressive efficiency of 25.59% (certified at 25.36%) in a 0.06 cm 2 area for the inverted champion device, showcasing the promise of ferroelectric SAMs for PSCs performance enhancement. The conventional approach with applying self-assembled monolayer suffers from limited interface coverage and weaker dipole interactions. Here, authors employ ferroelectric molecule to construct a dipole layer, achieving certified efficiency of 25.36% for inverted perovskite solar cells.

Highlights Additive-assisted layer-by-layer (LBL) deposition enables organic solar cells to achieve an unprecedented power conversion efficiency of 20.8%, the highest efficiency to date. The gradient fibrillar morphology enabled by additive-assisted LBL processing promotes the formation of bulk p-i-n structure, improving exciton and carrier diffusion, and reducing recombination losses. The wrinkle pattern morphology achieved by additive-assisted LBL processing is constructed to enhance the light capture capability. Recently published in Joule, Feng Liu and colleagues from Shanghai Jiaotong University reported a record-breaking 20.8% power conversion efficiency in organic solar cells (OSCs) with an interpenetrating fibril network active layer morphology, featuring a bulk p-i-n structure and proper vertical segregation achieved through additive-assisted layer-by-layer deposition. This optimized hierarchical gradient fibrillar morphology and optical management synergistically facilitates exciton diffusion, reduces recombination losses, and enhances light capture capability. This approach not only offers a solution to achieving high-efficiency devices but also demonstrates the potential for commercial applications of OSCs.

Heterostructure is the basic building block for functional optoelectronic devices. Heterostructures consisting of two-dimensional (2D) transition metal dichalcogenides (TMDs) and organic semiconductors are currently attracting great interest for high-performance optoelectronics. However, how to design heterostructure for highly efficient optoelectronic devices remains a big challenge. Here we design high-performance organic semiconductor/WSe 2 heterostructure photodetectors by tailoring the charge transfer effect between 2,2′-((2Z,2′Z)-(((4,4,9,9-tetrakis(4-hexylphenyl)-4,9- dihydros-indaceno[1,2-b:5,6-b′]dithiophene-2,7-diyl)bis(4-((2-ethylhexyl)oxy)thiophene-5,2-diyl))bis(methanylylidene))bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1-diylidene)) dimalononitrile (IEICO-4F) organic semiconductors with various thicknesses and monolayer WSe 2 . With the increase of IEICO-4F layer thickness, the photoluminescence (PL) characteristics of WSe 2 could be completely quenched due to the charge transfer from the lowest unoccupied molecular orbital (LUMO) level of IEICO-4F to the conduction band minimum (CBM) of WSe 2 . Benefiting from the exquisite charge transfer behavior, the IEICO-4F/WSe 2 heterojunction photodetector with optimized 6.0-nm thick IEICO-4F shows high performance including the responsivity of 8.32 A/W and specific detectivity of 4.65 × 10 11 Jones at incident light of 808 nm. This work demonstrates a simple approach based on PL characteristics to design high-performance IEICO-4F/WSe 2 heterojunction, thus paving the way for the development of excellent optoelectronic devices based on organic/TMD heterostructures.

High‐performance perovskite solar cells (PVSCs) with low energy consumption and green processing are highly desired, but constrained by the difficulty in morphology control and the poor understanding on morphology evolution mechanisms. To address this issue, here we studied the effect of antisolvents on the perovskite film formation. We found that both the antisolvents and the perovskite composition affect the perovskite film morphology greatly via influencing the intermediate phase, and different perovskite compositions require different antisolvents to reach the optimal morphology. This provides the opportunity to achieve high‐performance PVSCs with green antisolvent, that is, isopropanol (iPA) by changing the perovskite compositions, and leads to a power conversion efficiency (PCE) of 21.50% for PVSCs based on MA0.6FA0.4PbI3. Further, we fabricated “fully green” PVSCs with all layers prepared by green solvents, and the optimal PCE can reach 19%, which represents the highest among PVSCs with full‐green processing. This work provides insight into the perovskite morphology evolution and paves the way toward “green” processing PVSCs. Green antisolvent and full‐green solvents‐processed high‐performance perovskite solar cells with efficiencies of 21.5 and 19.5% have been demonstrated by fine tuning the intermediate phase via antisolvent selection and composition engineering.

Organic–inorganic halide perovskite solar cells (OIHPSCs) offer a fantastic opportunity to harness solar energy in a low cost and efficient way. This ambition for commercialization has been greatly encouraged by the surge in device performance from 3.8% in 2009 to the state-of-the-art 22.7%. For high device performance, tailoring the interfacial properties is demonstrated essentially important. Being in a molecular scale, the self-assembly monolayers (SAMs) are proved a facile but effective tool for interface modification. And lots of studies have demonstrated that SAMs have a variety of positive effects for perovskite solar cells, including mediating the morphology, improving energy level alignment, passivating trap states, etc. In this mini review, we give an insightful summary on the recent application of SAMs in OIHPSCs, analyze the mechanisms to improve device performance, and provide guidance to SAM-boosted perovskite solar cells for high performance and practical application. Finally, a landscape is depicted for future application of SAMs in perovskite solar cells.