Combining text mining, in situ characterization, and ab initio calculations to rationalize BiFeO3 crystallization pathways

The combination of three highly complementary scientific domains is demonstrated to rationalize bismuth ferrite (BiFeO<sub>3</sub> [BFO]) crystallization pathways: text mining to extract processing recipes from existing literature, in situ X-ray scattering to follow crystallization pathways of solution-processed thin films, and ab initio calculations to develop a comprehensive understanding of thin-film formation from thermodynamic principles. Multiferroic BFO is chosen as an example material of interest for technological applications to demonstrate and validate this combined approach. Thermodynamic modeling showed that the production of a short-lived intermediate bismutite phase (Bi<sub>2</sub>O<sub>2</sub>CO<sub>3</sub>) influences the energies of competing reactions forming BFO and Bi<sub>2</sub>Fe<sub>4</sub>O<sub>9</sub>, increasing the thermodynamic driving force toward the formation of BFO rather than Bi<sub>2</sub>Fe<sub>4</sub>O<sub>9</sub> impurity phase over a large temperature window. Finally, the synergy between the scientific domains is exemplified through the rational guidelines developed for controlling high-quality and phase-pure material fabrication.