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All-polymer solar cells (all-PSCs) consisting of polymer donors (P Ds) and polymer acceptors (P As) have drawn tremendous research interest in recent years. It is due to not only their tunable optical, electrochemical, and structural properties, but also many superior features that are not readily available in conventional polymer–fullerene solar cells (fullerene-PSCs) including long-term stability, synthetic accessibility, and excellent film-forming properties suitable for large-scale manufacturing. Recent breakthroughs in material design and device engineering have driven the power conversion efficiencies (PCEs) of all-PSCs exceeding 11%, which is comparable to the performance of fullerene-PSCs. Furthermore, outstanding mechanical durability and stretchability have been reported for all-PSCs, which make them stand out from the other small molecule-based PSCs as a promising power supplier for wearable electronic devices. This review provides a comprehensive overview of the important work in all-PSCs, in which pertinent examples are deliberately chosen. First, we describe the key components that enabled the recent progresses of all-PSCs including rational design rules for efficient P Ds and P As, blend morphology control, and light harvesting engineering. We also review the recent work on the understanding of the stability of all-PSCs under various external conditions, which highlights the importance of all-PSCs for future implementation and commercialization. Finally, because all-PSCs have not yet achieved their full potential and are still undergoing rapid development, we offer our views on the current challenges and future prospects.

The use of hybrid organic-inorganic perovskites in optoelectronic applications are attracting an interest because of their outstanding characteristics, which enable a remarkable enhancement of device efficiency. However, solution-processed perovskite crystals unavoidably contain defect sites that cause hysteresis in perovskite solar cells (PeSCs) and blinking in perovskite light-emitting diodes (PeLEDs). Here, we report significant beneficial effects using a new treatment based on amine-based passivating materials (APMs) to passivate the defect sites of methylammonium lead tribromide (MAPbBr) through coordinate bonding between the nitrogen atoms and undercoordinated lead ions. This treatment greatly enhanced the PeLED's efficiency, with an external quantum efficiency (EQE) of 6.2%, enhanced photoluminescence (PL), a lower threshold for amplified spontaneous emission (ASE), a longer PL lifetime, and enhanced device stability. Using confocal microscopy, we observed the cessation of PL blinking in perovskite films treated with ethylenediamine (EDA) due to passivation of the defect sites in the MAPbBr.

Despite the recent breakthroughs of polymer solar cells (PSCs) exhibiting a power conversion efficiency of over 17%, toxic and hazardous organic solvents such as chloroform and chlorobenzene are still commonly used in their fabrication, which impedes the practical application of PSCs. Thus, the development of eco-friendly processing methods suitable for industrial-scale production is now considered an imperative research focus. This Review provides a roadmap for the design of efficient photoactive materials that are compatible with non-halogenated green solvents (e.g., xylenes, toluene, and tetrahydrofuran). We summarize the recent development of green processing solvents and the processing methods to match with the efficient photoactive materials used in non-fullerene solar cells. We further review progress in the use of more eco-friendly solvents (i.e., water or alcohol) for achieving truly sustainable and ecofriendly PSC fabrication. For example, the concept of water-or alcohol-dispersed nanoparticles made of conjugated materials is introduced. Also, recent important progress and strategies to develop water/alcohol-soluble photoactive materials that completely eliminate the use of conventional toxic solvents are discussed. Finally, we provide our perspectives on the challenges facing the current green processing methods and materials, such as large-area coating techniques and long-term stability. We believe this Review will inform the development of PSCs that are truly clean and renewable energy sources.

The interfacial dipolar polarization in inverted structure polymer solar cells, which arises spontaneously from the absorption of ethanolamine end groups, such as amine and hydroxyl groups on ripple-structure zinc oxide (ZnO-R), lowers the contact barrier for electron transport and extraction and leads to enhanced electron mobility, suppression of bimolecular recombination, reduction of the contact resistance and series resistance, and remarkable enhancement of the power conversion efficiency.

Highly efficient planar perovskite optoelectronic devices are realized by amine-based solvent treatment on compact TiO2 and by optimizing the morphology of the perovskite layers. Amine-based solvent treatment between the TiO2 and the perovskite layers enhances electron injection and extraction and reduces the recombination of photogenerated charges at the interface.

Organic-inorganic hybrid perovskites are emerging as promising emitting materials due to their narrow full-width at half-maximum emissions, color tunability, and high photoluminescence quantum yields (PLQYs). However, the thermal generation of free charges at room temperature results in a low radiative recombination rate and an excitation-intensity-dependent PLQY, which is associated with the trap density. Here, we report perovskite films composed of uniform nanosized single crystals (average diameter = 31.7 nm) produced by introducing bulky amine ligands and performing the growth at a lower temperature. By effectively controlling the crystal growth, we maximized the radiative bimolecular recombination yield by reducing the trap density and spatially confining the charges. Finally, highly bright and efficient green emissive perovskite light-emitting diodes that do not suffer from electroluminescence blinking were achieved with a luminance of up to 55 400 cd m, current efficiency of 55.2 cd A, and external quantum efficiency of 12.1%.

High fracture resistance of polymer solar cells (PSCs) is of great importance to ensure long-term mechanical reliability, especially considering their potential in roll-to-roll printing processes and flexible devices. In this paper, we compare mechanical properties, such as the cohesive fracture energy, elastic modulus, and crack-onset strain, of allpolymer solar cells (all-PSCs) and fullerene-based solar cells (PCBM− PSCs) based on the same, representative low-bandgap polymer donor (PTB7-Th) as a function of acceptor content. The all-PSCs exhibit higher fracture energy (2.45 J m −2 ) than PCBM−PSCs (0.29 J m −2 ) at optimized device conditions. Additionally, a 15-fold higher crack-onset strain is observed in all-PSCs than in PCBM−PSCs. Dramatically different mechanical compliances observed for all-PSCs and PCBM− PSCs are investigated in detail by analysis of the blend morphologies as a function of acceptor content (either P(NDI2HD-T) or PCBM acceptors). The superior fracture resistance of all-PSCs is attributed to the more ductile characteristics of the polymer acceptor and the large degree of plastic deformation during crack growth, in contrast to the brittle nature of PCBM and the weak interaction between the polymer-rich phase and highly aggregated PCBM-rich domains. Therefore, this work demonstrates that replacing a small-molecule acceptor (i.e., PCBM) with polymeric materials can be an effective strategy toward mechanically robust PSCs.