Organic photovoltaic (OPV) devices have shown remarkable performance progress in recent years, reaching current record power conversion efficiency (PCE) values of 16.4% for single junction and 17.3% for multi junction devices, owing mostly to the impressive developments made within synthesis of new non-fullerene acceptors. This progress places organic solar cells at the forefront of thin-film photovoltaic technology. However, in order to meet industrial demands and reach high performance values in industrial settings, further research and development efforts within Roll-to-Roll (R2R) and Sheet-to-Sheet (S2S) processing of OPV devices under ambient conditions are required. Furthermore, OPV modules being manufactured through such up-scaled processing techniques should ideally be developed from low cost materials, and show good stability towards various different operational stress conditions. In this work, we demonstrate combined R2R and S2S development of ITO-free OPV devices, which are based on the non-fullerene material system PBDB-T:ITIC. The 2 devices are processed from R2R vacuum sputtering and S2S slot-die coating at ambient conditions, and reach cell PCE values of 5.5%. In addition, we introduce a correlation between different barrier films, both commercial and sputtered inorganic coatings on ultra-clean PET, and the lifetime of the developed devices. The results therefore demonstrate an important step in the development of OPV devices from R2R and S2S processes in industrial settings.

The development of nonfullerene acceptors (NFAs) has led to dramatic improvements in the device efficiencies of organic photovoltaic (OPV) cells. To date it is, however, still unclear how those laboratory‐scale efficiencies transfer to commercial modules, and how stable these devices will be when processed via industrially compatible methods. Herein, the degradation behavior of lab‐scale and scalable OPV devices using similar nonfullerene‐based active layers is assessed. It is demonstrated that the scalable NFA OPV exhibits completely reversible degradation when assessed in ISOS‐O‐1 outdoor conditions, which is in contrast to the laboratory‐scale devices assessed via the indoor ISOS‐L‐2 protocol. Results from transient photovoltage (TPV) indicate the presence of charge trap formation, and a number of potential mechanisms are proposed for the selective occurrence of this in laboratory‐scale devices tested in ISOS‐L laboratory conditions—ultimately concluding that it has its origins in the different device architectures used. The study points at the risk of assessing active layer stability from laboratory‐scale devices and degradation studies alone and highlights the importance of using a diverse range of testing conditions and ISOS protocols for such assessment.

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We compare pristine and degraded samples that were subjected to outdoor degradation following standard ISOS-O2 protocol. The ideality factors for different incident wavelengths obtained from open circuit voltage versus irradiation level and current density-voltage (J-V) measurements at different temperatures, indicate that for aged samples recombination is governed by Shockley-Red-Hall mechanism occurring in a region near the anode. Samples were also characterized using impedance spectroscopy and fitted to an electrical model. Impedance parameters were used to obtain mobility, indicating a clear degradation of the active layer blend for aged samples. The change in the chemical capacitance also reveals a worsening in carrier extraction. Finally, 2D numerical simulations and fits to experimental J-V curves confirm the existence of a layer near the anode contact with poorer mobility and a decrease of the anode work function for the degraded samples.

Light-trapping nanostructures have for decades been researched as a route to enhance the performance of organic solar cells (OSCs). Whereas the power conversion efficiencies (PCEs) of OSCs have reached above 18 %, industrially compatible devices made by scalable processing in air, using only nontoxic solvents and materials, have shown significantly lower performance values. Although light-trapping nanostructures may improve this, the methods for integrating the nanostructures are typically not compatible with industrial scale up. In this work, scalable, industrially compatible, nonfullerenebased OSCs are developed with integrated light-trapping nanostructures at the back electrodes in the devices. The OSCs are made by using scalable roll-to-roll (R2R) and sheet-to-sheet (S2S) processes and the nanostructures are made by using rollto-plate (R2P) nanoimprint lithography. A fully scalable solution is thereby developed for industrially compatible nanostructured OSCs. The nanostructured devices show enhancements in PCE up to 25 % compared to reference cells, owing to an enhancement in the short-circuit current density (15 %) by enhanced absorption, and improved charge carrier extraction leading to an enhancement in the fill factor (7 %). Optical modeling is utilized to verify the optical effect of the nanostructures. The best devices attain a PCE of 6.5 %, which is the highest reported efficiency for air-processed slot-die coated ITO-free flexible PBDB-T : ITIC devices, here using nontoxic solvents.