Predictive Modelling of Structure Formation in Semiconductor Films Produced by Meniscus-guided Coating

Meniscus-guided coating methods, such as zone casting, dip coating and solution shearing, are scalable laboratory models for large-area solution coating of functional materials for thin-film electronics. Unfortunately, the general lack of understanding of how the coating parameters affect the dry-film morphology upholds trial-and-error experimentation and delays lab-to-fab translation. We present herein a model that predicts dry-film morphologies produced by meniscus-guided coating of a crystallizing solute. Our model reveals how the interplay between coating velocity and evaporation rate determines the crystalline domain size, shape anisotropy and regularity. If coating is fast, evaporation drives the system quickly past supersaturation, giving isotropic domain structures. If coating is slow, depletion due to crystallization stretches domains in the coating direction. The predicted morphologies have been experimentally confirmed by zone-casting experiments of the organic semiconductor 4-tolyl-bithiophenyl-diketopyrrolopyrrole. Although here we considered a small molecular solute, our model can be applied broadly to polymers and organic-inorganic hybrids such as perovskites.