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Solution casting under ambient conditions of thin films of the ferroelectric copolymer poly(vinylidene fluoride-co-trifluoroethylene) (P(VDF-TrFE)) is highly attractive for cost-effective production of flexible memory devices. However, rough and porous films obtained under ambient conditions typically give a low yield of working devices. A major challenge is ambient water vapor condensing into the drying solution, causing non-solvent vapor-induced phase separation (VIPS). By integrating solution-stage modeling, microscopic analysis and thin-film device characterization, we show that the hydrophilicity of solvent is a deciding factor in obtaining properly functioning capacitive memory elements based on P(VDF-TrFE) under ambient conditions. Our numerical study, involving the ternary phase diagram of the polymer/water/solvent blend as well multicomponent dynamic phase field modeling, predicts the occurrence of VIPS for a given solvent hygroscopicity and demonstrates an increase in early stage domain size with decreasing relative humidity, whereas the opposite trend is predicted for the rate of demixing. Experimentally observed morphologies are consistent with the numerical simulations. For a sufficiently low solvent hygroscopicity, >90% production yield of devices operating at voltages on par with upscaled thin-film flexible electronics is achieved.

Processing of ferroelectric polymers for microelectronics: from morphological analysis to functional devices