Crystallizing Substrates Drag Supported Nanoparticles

Abstract

When a solid support undergoes crystallization, the advancing amorphous-to-crystalline transformation front separates regions of distinct surface energy, creating a moving interfacial energy boundary. A supported nanoparticle straddling such a boundary experiences an asymmetric particle-substrate interfacial energy environment that constitutes a lateral thermodynamic driving force for migration. Here, using in situ transmission electron microscopy to track Pt nanoparticle motion statistically, paired with time-resolved diffraction and 4D-STEM analysis to characterize support crystallization, we demonstrate that propagating crystallization fronts in amorphous AlO$_x$ thin films actively drag supported Pt nanoparticles over long distances. Temporal correlation between the onsets of support crystallization and rapid particle migration, together with 4D-STEM virtual crystallinity maps, establishes that the front drives particle motion. Phase-field simulations confirm that particle-substrate interfacial energy contrast alone sustains particle drag, and identify curvature gradients along the particle surface as the mechanism by which the advancing front redistributes mass and displaces the particle. These results establish a general mechanism by which any propagating surface-energy boundary on a substrate can act as a deterministic driver of supported nanoparticle transport.