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Highlights High-quality large-area perovskite films are prepared using a solid–liquid two-step film formation method combined with CsBr modification for the buried interface and Urea additive for perovskite crystallization. The inverted perovskite solar modules’ performance is enhanced to 20.56% in 61.56 cm2 with improved stability.

Abstract Organic photovoltaics (OPVs) represent one of the most promising photovoltaic technologies owing to their high capacity to convert solar energy to electricity. With the continuous structure upgradation of photovoltaic materials, especially that of non‐fullerene acceptors (NFAs), the OPV field has witnessed rapid progress with power conversion efficiency (PCE) exceeding 19%. However, it remains challenging to overcome the intrinsic trade‐off between the photocurrent and photovoltage, restricting the further promotion of the OPV efficiency. In this regard, it is urgent to further tailor the structure of NFAs to broaden their absorption spectra while mitigating the energy loss of relevant devices concomitantly. Heteroatom substitution on the fused‐ring π‐core of NFAs is an efficient way to achieve this goal. In addition to improve the near‐infrared light harvest by strengthening the intramolecular charge transfer, it can also enhance the molecular stacking via forming multiple noncovalent interactions, which is favorable for reducing the energetic disorder. Therefore, in this review we focus on the design rules of NFAs, including the polymerized NFAs, of which the core moiety is substituted by various kinds of heteroatoms. We also afford a comprehensive understanding on the structure–property−performance relationships of these NFAs. Finally, we anticipate the challenges restricting the efficiency promotion and industrial utilization of OPV, and provide potential solutions based on the further heteroatom optimization on NFA core‐moiety.

Abstract Dielectric constant of non-fullerene acceptors plays a critical role in organic solar cells in terms of exciton dissociation and charge recombination. Current acceptors feature a dielectric constant of 3-4, correlating to relatively high recombination loss. We demonstrate that selenium substitution on acceptor central core can effectively modify molecule dielectric constant. The corresponding blend film presents faster hole-transfer of ~5 ps compared to the sulfur-based derivative (~10 ps). However, the blends with Se-acceptor also show faster charge recombination after 100 ps upon optical pumping, which is explained by the relatively disordered stacking of the Se-acceptor. Encouragingly, dispersing the Se-acceptor in an optimized organic solar cell system can interrupt the disordered aggregation while still retain high dielectric constant. With the improved dielectric constant and optimized fibril morphology, the ternary device exhibits an obvious reduction of non-radiative recombination to 0.221 eV and high efficiency of 19.0%. This work unveils heteroatom-substitution induced dielectric constant improvement, and the associated exciton dynamics and morphology manipulation, which finally contributes to better material/device design and improved device performance.

Abstract All-small-molecule organic solar cells with good batch-to-batch reproducibility combined with non-halogen solvent processing show great potential for commercialization. However, non-halogen solvent processing of all-small-molecule organic solar cells are rarely reported and its power conversion efficiencies are very difficult to improve. Herein, we designed and synthesized a small molecule donor BM-ClEH that can take advantage of strong aggregation property induced by intramolecular chlorine-sulfur non-covalent interaction to improve molecular pre-aggregation in tetrahydrofuran and corresponding micromorphology after film formation. Tetrahydrofuran-fabricated all-small-molecule organic solar cells based on BM-ClEH:BO-4Cl achieved high power conversion efficiencies of 15.0% in binary device and 16.1% in ternary device under thermal annealing treatment. In contrast, weakly aggregated BM-HEH without chlorine-sulfur non-covalent bond is almost inefficient under same processing conditions due to poor pre-aggregation induced disordered π-π stacking, indistinct phase separation and exciton dissociation. This work promotes the development of non-halogen solvent processing of all-small-molecule organic solar cells and provides further guidance.

Abstract Piezoelectric biomaterials have attracted great attention owing to the recent recognition of the impact of piezoelectricity on biological systems and their potential applications in implantable sensors, actuators, and energy harvesters. However, their practical use is hindered by the weak piezoelectric effect caused by the random polarization of biomaterials and the challenges of large-scale alignment of domains. Here, we present an active self-assembly strategy to tailor piezoelectric biomaterial thin films. The nanoconfinement-induced homogeneous nucleation overcomes the interfacial dependency and allows the electric field applied in-situ to align crystal grains across the entire film. The β-glycine films exhibit an enhanced piezoelectric strain coefficient of 11.2 pm V−1 and an exceptional piezoelectric voltage coefficient of 252 × 10−3 Vm N−1. Of particular significance is that the nanoconfinement effect greatly improves the thermostability before melting (192 °C). This finding offers a generally applicable strategy for constructing high-performance large-sized piezoelectric bio-organic materials for biological and medical microdevices.

The intrinsic trade-off between efficiency and stability is a challenging issue for organic photovoltaics. Here, the authors develop non-fullerene acceptors with tailored side-group hindrance and backbone planarity and realise efficiency of 18.3% and good stability for xylene-processed solar cells

Abstract The recently reported efficient polymerized small‐molecule acceptors (PSMAs) usually adopt a regioregular backbone by polymerizing small‐molecule acceptors precursors with a low‐reactivity 5‐brominated 3‐(dicyanomethylidene)indan‐1‐one (IC) end group or its derivatives, leading to low molecular weight, and thus reduce active layer mechanical properties. Herein, a series of newly designed chlorinated PSMAs originating from isomeric IC end groups are developed by adjusting chlorinated positions and copolymerized sites on end groups to achieve high molecular weight, favorable intermolecular interaction, and improved physicochemical properties. Compared with regioregular PY2Se‐Cl‐o and PY2Se‐Cl‐m, regiorandom PY2Se‐Cl‐ran has a similar absorption profile, moderate lowest unoccupied molecular orbital level, and favorable intermolecular packing and crystallization properties. Moreover, the binary PM6:PY2Se‐Cl‐ran blend achieves better ductility with a crack‐onset strain of 17.5% and improved power conversion efficiency (PCE) of 16.23% in all‐polymer solar cells (all‐PSCs) due to the higher molecular weight of PY2Se‐Cl‐ran and optimized blend morphology, while the ternary PM6:J71:PY2Se‐Cl‐ran blend offers an impressive PCE approaching 17% and excellent device stability, which are all crucial for potential practical applications of all‐PSCs in wearable electronics. To date, the efficiency of 16.86% is the highest value reported for the regiorandom PSMAs‐based all‐PSCs and is also one of the best values reported for the all‐PSCs. Our work provides a new perspective to develop efficient all‐PSCs, with all high active layer ductility, impressive PCE, and excellent device stability, towards practical applications.

The incorporation of plasmonic core-shell nanostructures at the grain boundaries of perovskite films reduces the charge recombination loss through photo-brightening of trap states.

Despite the rapidly increased power conversion efficiency (PCE) of perovskite solar cells (PVSCs), it is still quite challenging to bring such promising photovoltaic technology to commercialization. One of the challenges is the upscaling from small-sized lab devices to large-scale modules or panels for production. Currently, most of the efficient inverted PVSCs are fabricated on top of poly[bis(4-phenyl)(2, 4, 6-trimethylphenyl)amine] (PTAA), which is a commonly used hole-transporting material, using spin-coating method to be incompatible with large-scale film deposition. Therefore, it is important to develop proper coating methods such as blade-coating or slot-die coating that can be compatible for producing large-area, high-quality perovskite thin films. It is found that due to the poor wettability of PTAA, the blade-coated perovskite films on PTAA surface are often inhomogeneous with large number of voids at the buried interface of the perovskite layer. To solve this problem, self-assembled monolayer (SAM)-based hole-extraction layer (HEL) with tunable headgroups on top of the SAM can be modified to provide better wettability and facilitate better interactions with the perovskite coated on top to passivate the interfacial defects. The more hydrophilic SAM surface can also facilitate the nucleation and growth of perovskite films fabricated by blade-coating methods, forming a compact and uniform buried interface. In addition, the SAM molecules can also be modified so their highest occupied molecular orbital (HOMO) levels can have a better energy alignment with the valence band maxima (VBM) of perovskite. Benefitted by the high-quality buried interface of perovskite on SAM-based substrate, the champion device shows a PCE of 18.47% and 14.64% for the devices with active areas of 0.105 cm2 and 1.008 cm2, respectively. In addition, the SAM-based device exhibits decent stability, which can maintain 90% of its initial efficiency after continuous operation for over 500 h at 40 ℃ in inert atmosphere. Moreover, the SAM-based perovskite mini-module exhibits a PCE of 14.13% with an aperture area of 18.0 cm2. This work demonstrates the great potential of using SAMs as efficient HELs for upscaling PVSCs and producing high-quality buried interface for large-area perovskite films.

The so-called pseudo-bilayer (PB) organic solar cell (OSC) device architecture can promote enhanced exciton dissociation and charge transport, leading to improved device performance. Here, the authors report high-efficiency OSCs that features a PB architecture and optimized ternary system.

Designing efficient blue perovskite LEDs by using mixed halides perovskite is still a challenge, limited mainly by the phase segregation issue. Here, the authors demonstrate in situ fabrication of quasi-2D CsPbClBr2 nanocrystal films with mixed ligands to overcome the constraint.

Summary: Organic solar cells (OSCs) suffer from severe upscaling loss due to the inevitable formation of inhomogeneities and the intrinsically low charge mobilities of organic materials limiting the charge extraction efficiency, especially in the situation where cell width reaches centimeter scale. Here, we report the introduction of a nematic liquid crystal donor, BTR-Cl, into a typical non-fullerene blending system of PM6:BTP-eC9. The participation of BTR-Cl contributes to a significantly improved crystallinity and ordering of the host components and facilitates efficient three-dimensional charge transport in the active layer. Simultaneously improved fill factor and current density are thus achieved in BTR-Cl-doped OSCs, corresponding to a superior efficiency of 18.31%. More importantly, a high efficiency of 16.88% along with a robust fill factor of 73.4% is retained when enlarging the effective device area from 0.034 to 1.01 cm2, highlighting the importance of three-dimensional charge transport in reducing the upscaling loss of OSCs.

Lead halide perovskite quantum dots (PQDs) promise applications in optoelectronics but are limited by sensitivity to wet environments. Here the authors develop a Pb-S bonding approach to synthesize PQDs@silica nanodots that are capable of emitting and lasing in aqueous environments for long periods.

Abstract The correlation between structure and function lies at the heart of materials science and engineering. Especially, modern functional materials usually contain inhomogeneities at an atomic level, endowing them with interesting properties regarding electrons, phonons, and magnetic moments. Over the past few decades, many of the key developments in functional materials have been driven by the rapid advances in short‐range crystallographic techniques. Among them, pair distribution function (PDF) technique, capable of utilizing the entire Bragg and diffuse scattering signals, stands out as a powerful tool for detecting local structure away from average. With the advent of synchrotron X‐rays, spallation neutrons, and advanced computing power, the PDF can quantitatively encode a local structure and in turn guide atomic‐scale engineering in the functional materials. Here, the PDF investigations in a range of functional materials are reviewed, including ferroelectrics/thermoelectrics, colossal magnetoresistance (CMR) magnets, high‐temperature superconductors (HTSC), quantum dots (QDs), nano‐catalysts, and energy storage materials, where the links between functions and structural inhomogeneities are prominent. For each application, a brief description of the structure‐function coupling will be given, followed by selected cases of PDF investigations. Before that, an overview of the theory, methodology, and unique power of the PDF method will be also presented.

Abstract Currently, there are only very few dopant‐free polymer hole‐transporting materials (HTMs) that can enable perovskite solar cells (PVSCs) to demonstrate a high power conversion efficiency (PCE) of greater than 20%. To address this need, a simple and efficient way is developed to synthesize novel crossconjugated polymers as high performance dopant‐free HTMs to endow PVSCs with a high PCE of 21.3%, which is among the highest values reported for single‐junction inverted PVSCs. More importantly, rational understanding of the reasons why two isomeric polymer HTMs (PPE1 and PPE2) with almost identical photophysical properties, hole‐transporting ability, and surface wettability deliver so distinctly different device performance under similar device fabrication conditions is manifested. PPE2 is found to improve the quality of perovskite films cast on top with larger grain sizes and more oriented crystallization. These results help unveil the new HTM design rules to influence the perovskite growth/crystallization for improving the performance of inverted PVSCs.

We report a simplified reflection mode Fabry-Perot interferometry method for determination of electro-optic (EO) coefficients of poled polymer thin films. Rather than fitting the detailed shape of the Fabry-Perot resonance curve, our simplification involves a technique to experimentally determine the voltage-induced shift in the angular position of the resonance minimum. Rigorous analysis based on optical properties of individual layers of the multilayer structure is not necessary in the data analysis. Although angle scans are involved, the experimental setup does not require a θ-2θ rotation stage and the simplified analysis is an advantage for polymer synthetic efforts requiring quick and reliable screening of new materials. Numerical and experimental results show that our proposed method can determine EO coefficients to within an error of ~8% if poled values for the refractive indices are used.