The performance of organic solar cells is determined by the delicate, meticulously optimized bulk-heterojunction microstructure, which consists of finely mixed and relatively separated donor/acceptor regions. Here we demonstrate an abnormal strong burn-in degradation in highly efficient polymer solar cells caused by spinodal demixing of the donor and acceptor phases, which dramatically reduces charge generation and can be attributed to the inherently low miscibility of both materials. Even though the microstructure can be kinetically tuned for achieving high-performance, the inherently low miscibility of donor and acceptor leads to spontaneous phase separation in the solid state, even at room temperature and in the dark. A theoretical calculation of the molecular parameters and construction of the spinodal phase diagrams highlight molecular incompatibilities between the donor and acceptor as a dominant mechanism for burn-in degradation, which is to date the major short-time loss reducing the performance and stability of organic solar cells.

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Development of high-quality organic nanoparticle inks is a significant scientific challenge for the industrial production of solution-processed organic photovoltaics (OPVs) with eco-friendly processing methods. In this work, we demonstrate a novel, robot-based, high-throughput procedure performing automatic poly(3-hexylthio-phene-2,5-diyl) and indene-C bisadduct nanoparticle ink synthesis in nontoxic alcohols. A novel methodology to prepare particle dispersions for fully functional OPVs by manipulating the particle size and solvent system was studied in detail. The ethanol dispersion with a particle diameter of around 80-100 nm exhibits reduced degradation, yielding a power conversion efficiency of 4.52%, which is the highest performance reported so far for water/alcohol-processed OPV devices. By successfully deploying the high-throughput robot-based approach for an organic nanoparticle ink preparation, we believe that the findings demonstrated in this work will trigger more research interest and effort on eco-friendly industrial production of OPVs.

a Solution-processed organic photovoltaic devices are advantageous due to their low-cost large area manufacturing techniques, such as slot-die coating, gravure printing and roll-to-roll coating. The final microstructure of a polymer:fullerene bulk-heterojunction (BHJ) film is a fine interplay between solution thermodynamics (e.g. solubility, miscibility. . .) and kinetics (e.g. solvent evaporation, polymer ordering, phase separation. . .) during the drying process. In order to design better performing organic photovoltaic devices, gaining knowledge over the drying properties of polymer:fullerene thin films is essential.A novel in situ thin film drying characterization chamber, equipped with white-light reflectometry, laser light scattering and photoluminescence, is presented in combination with grazing-incidence X-ray diffraction on two different polymer:fullerene bulk heterojunctions based on poly-(3-hexylthiophene-2,5-diyl) (P3HT) and polythieno [3,2b]thiophene-diketopyrrolopyrrole-co-thiophene (DPP-TT-T) polymers.With photoluminescence applied for the first time as an in situ method for such drying studies, these single-chamber measurements track the fine interplay between thermodynamics and kinetics of thin film drying and provide invaluable information on solution behavior and microstructure formation.

A multipurpose interconnection layer based on poly(3,4-ethylenedioxythiophene) doped with poly(styrene sulfonate) (PEDOT:PSS), and d-sorbitol for monolithic perovskite/silicon tandem solar cells is introduced. The interconnection of independently processed silicon and perovskite subcells is a simple add-on lamination step, alleviating common fabrication complexities of tandem devices. It is demonstrated experimentally and theoretically that PEDOT:PSS is an ideal building block for manipulating the mechanical and electrical functionality of the charge recombination layer by controlling the microstructure on the nano-and mesoscale. It is elucidated that the optimal functionality of the recombination layer relies on a gradient in the d-sorbitol dopant distribution that modulates the orientation of PEDOT across the PEDOT:PSS film. Using this modified PEDOT:PSS composite, a monolithic two-terminal perovskite/silicon tandem solar cell with a steady-state efficiency of 21.0%, a fill factor of 80.4%, and negligible open circuit voltage losses compared to single-junction devices is shown. The versatility of this approach is further validated by presenting a laminated two-terminal monolithic perovskite/organic tandem solar cell with 11.7% power conversion efficiency. It is envisioned that this lamination concept can be applied for the pairing of multiple photovoltaic and other thin film technologies, creating a universal platform that facilitates mass production of tandem devices with high efficiency.