Multistate Dynamic Pathways for Anisotropic Colloidal Assembly and Reconfiguration

We report the controlled interfacial assembly and reconfiguration of rectangular prism colloidal particles between microstructures of varying positional and orientational order including stable, metastable, and transient states. Structurally diverse states are realized by programming time dependent electric fields that mediate dipolar interactions determining particle position, orientation, compression, and chaining. We identify an order parameter set that defines each state as a combination of the positional and orientational order. These metrics are employed as reaction coordinates to capture the microstructure evolution between initial and final states upon field changes. Assembly trajectory manifolds between states in the low-dimensional reaction coordinate space reveal a dynamic pathway map including information about pathway accessibility, reversibility, and kinetics. By navigating the dynamic pathway map, we demonstrate reconfiguration between states on minute time scales, which is practically useful for particle-based materials processing and device responses. Our findings demonstrate a conceptually general approach to discover dynamic pathways as a basis to control assembly and reconfiguration of self-organizing building blocks that respond to global external stimuli.