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Extensive research on bulk‐heterojunction (BHJ) optimization has advanced organic photovoltaics (OPVs). However, the need for research addressing the issue of morphological instability and ensuring long‐term durability remains a priority. Herein, a diffusion‐governed morphological modification methodology via a sequential deposition (SD) process comprising ternary components with low miscibility is demonstrated. Sequential coating of a high glass transition temperature (Tg) material and a host binary blend induces a concentration difference between successively coated layers, allowing for effective blending of immiscible materials during solvent evaporation. The enhanced miscibility of the SD‐processed BHJ layer facilitates molecular interactions between the high Tg material and the host materials, thereby increasing the Tg of the BHJ blend. The SD‐processed OPVs exhibit superior photovoltaic performance and suppressed glass transition under thermal stress compared to reference OPVs fabricated via a conventional method. After 500 h of thermal aging at 85 °C, the SD‐BHJ OPV retains over 80% of its initial efficiency, whereas the reference device shows a drastic drop to below 80% of its initial efficiency after only 80 h. This study provides a step toward efficient, long‐term stable OPVs by overcoming the limitations of blend miscibility and poor thermal durability of conventional BHJ systems via a SD process. [ABSTRACT FROM AUTHOR]

To meet the requirements for indoor organic photovoltaic (OPV) applications, it is imperative to minimize charge recombination loss and enhance photovoltaic performance toward commercially compelling levels. Here, morphological modification in non‐fullerene blends is demonstrated to boost the efficiency and stability of indoor OPVs. For morphological modification, a ternary blend is devised by utilizing two well‐miscible non‐fullerene acceptors, which improve morphological features in the photoactive layer and suppress charge recombination loss. Morphological modification enhances OPV performance, particularly under low‐intensity indoor irradiation conditions, at which trap‐assisted recombination mainly governs the photovoltaic performance. The optimum ternary OPV shows a new record power conversion efficiency of 30.11% at a 500 lux light‐emitting diode, accompanied by excellent morphological durability under thermal stress, despite the use of "existing" photovoltaic materials designed for AM 1.5 G operation. This study elucidates the effects of morphology on OPV performance under low‐light conditions and suggests an ideal morphology for non‐fullerene OPVs with enhanced performance for indoor applications. [ABSTRACT FROM AUTHOR]

Multi-component (ternary, quaternary, and beyond) bulk heterojunction (BHJ) active layers are considered one of the most effective ways of increasing the performance of organic photovoltaics (OPVs). Herein, an alternative sequential deposition method for the development of efficient multi-component OPVs without the need for the complex optimization steps typical for blend parameters is discussed. Simple sequential spin-coating of two binary donor:acceptor blends was applied to produce modified quaternary BHJ layers, making full use of the optoelectronic advantages offered by the two binary blends and their optimized morphological features. A combination of theoretical and experimental analyses revealed the occurrence of molecular reorganization during sequential deposition which facilitated self-optimized molecular stratification and cascade energy level alignment. By using expanded universality test to account for the diverse BHJ systems, this sequential deposition methodology creates new opportunities as an alternative fabrication platform to secure high-performance multi-component BHJ OPVs for versatile (i.e., indoor and outdoor) irradiation environments while overcoming many of the drawbacks of conventional manufacturing procedures. Image 1 • Alternative manufacturing process of organic photovoltaics (OPVs) is demonstrated. • Sequential spin-coating of two binary blends produces modified multi-component bulk heterojunction layers. • Performance is optimized for both indoor and outdoor light conditions without the need for fine-tuned blend optimization. • Sequential deposition is a universal platform to achieve optimization-free, high-performance multi-component OPVs. [ABSTRACT FROM AUTHOR]

Ternary blend approaches are demonstrated as a universal means to improve overall performance of organic photovoltaics (OPVs) in both indoor and outdoor conditions. A comparative study on two donors:one acceptor (2D:1A) and one donor:two acceptors (1D:2A) ternary blends shows that both approaches are universally effective for indoor and outdoor operation; the 1D:2A devices incorporating a nonfullerene acceptor (NFA) benefit from less charge recombination and higher power conversion efficiencies (PCEs) for various irradiation conditions, while the performance of the 2D:1A blends depends on the emission spectrum of the incident light source. The synergistic merits of NFAs and ternary structure in the 1D:2A ternary OPVs secure better performance and generality regardless of the incident lighting. A combination of experimental and theoretical analyses unveils that NFAs optimize packing and arrangement of molecules to build efficient cascade ternary junctions in the 1D:2A blends, which can be important design guidelines for the third component in ternary OPVs. The optimized 1D:2A ternary OPV exhibits a new record PCE of 25.6% under a 200 lux light‐emitting diode (LED) and 26.4% under a 1000 lux LED, and superior durability under industrial relevant thermal stress, suggesting new opportunities in diverse practical applications challenging the currently dominant PV technologies. [ABSTRACT FROM AUTHOR]

The unique properties of organic photovoltaics (OPVs) offer great promise in emerging applications such as wearable electronics or the Internet of Things. For their successful utilization, OPV operation should be designed for versatile irradiation circumstances in addition to solar light since they should be capable of providing electric power when there is no sunlight or when they operate indoors. Here, a quaternary OPV (Q‐OPV) as a semitransparent, colorful energy platform that operates efficiently under both solar and artificial light irradiation is demonstrated. The experimentally optimized Q‐OPV shows a broadened spectral response and improved charge transport process with suppressed recombination, thereby providing high output powers that are sufficient to autonomously operate low‐power electronic devices. In addition, the Q‐OPV benefits from improved morphological stability with a reduced driving force for grain growth by the increased entropy in the quaternary blend system. The important features of the Q‐OPV platform such as semitransparency, high tolerance to film thickness, and color codability, while pursuing the improved performance and thermal durability, further open new opportunities as an all‐day (24/7/365) power generator in broad practical applications. [ABSTRACT FROM AUTHOR]