Polymer conformation in solution is more important for R2R solar cell performance than the crystallinity of the final coated film.

The active layer crystallization during roll-to-roll coating of organic solar cells is studied in situ. We developed an X-ray setup where the coater unit is an integrated part of the small angle X-ray scattering instrument, making it possible to control the coating process while recording scattering measurements in situ, enabling us to follow the crystal formation during drying. By varying the distance between the coating head and the point where the X-ray beam hits the film, we obtained measurements of 4 different stages of drying. For each of those stages, the scattering from as long a foil as possible is summed together, with the distance from coating head to scattering point kept constant. The results are average crystallographic properties for the active layer coated on a 30 m long foil. With this insight into the dynamics of crystallization in a roll-coated polymer film, we find that the formation of textured and untextured crystallites seems uncorrelated, and happens at widely different rates. Untextured P3HT crystallites form later in the drying process than expected which may explain previous studies speculating that untextured crystallization depends on concentration. Textured crystallites, however, begin forming much earlier and steadily increases as the film dries, showing a development similar to other in situ studies of these materials.

In an effort to understand recent results showing differences between the power conversion efficiencies of lead halide (CH 3 NH 3 PbI 3−x Cl x ) solar cells on glass versus flexible substrates, this study investigates the influence that substrate and processing methods have on morphological and crystallographic development. Using our in situ slot-die micro roll-to-roll coater setup, we measured small and wide angle X-ray scattering in grazing incidence while the material dried, enabling us to follow the crystallization from just after the deposition and up to 25 minutes later. The data showed differing crystallographic developments between the substrates, especially seen through the behaviour of a crystalline precursor which survived longer on the flexible substrates than on glass. Additionally, the common degradation product PbI 2 was absent on the thickest flexible substrate. This leads us to conjecture that the flexible substrates absorb part of the solvent, thereby delaying evaporation and changing the solvent environment around the perovskite. As a further test, we produced solar cells with the same substrates and confirmed that the ones made on flexible substrates performed worse than those made on glass, but that when including an ITO layer in the stack it seemed to act as a buffer, whereby the solar cell performance was improved.

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