Kinetically Controlled Fabrication of Single‐Crystalline TiO ₂ Nanobrush Architectures with High Energy {001} Facets

This study demonstrates that precise control of nonequilibrium growth conditions during pulsed laser deposition (PLD) can be exploited to produce single‐crystalline anatase TiO ₂ nanobrush architectures with large surface areas terminated with high energy {001} facets. The data indicate that the key to nanobrush formation is controlling the atomic surface transport processes to balance defect aggregation and surface‐smoothing processes. High‐resolution scanning transmission electron microscopy data reveal that defect‐mediated aggregation is the key to TiO ₂ nanobrush formation. The large concentration of defects present at the intersection of domain boundaries promotes aggregation of PLD growth species, resulting in the growth of the single‐crystalline nanobrush architecture. This study proposes a model for the relationship between defect creation and growth mode in nonequilibrium environments, which enables application of this growth method to novel nanostructure design in a broad range of materials.