Optoelectronically Directed Self-Assembly of Active and Passive Particles into Programmable and Reconfigurable Colloidal Structures

Abstract: Controlled assembly of active-passive colloidal mixtures offers a route to reconfigurable microscale machines, but their self-assembly pathways remain poorly understood. We study the directed assembly of metallo-dielectric Janus particles (JPs) and passive polystyrene (PS) beads using optoelectrically reconfigurable AC-field patterning, which allows precise control over particle composition and binding sequence. Through experiments, analytical modeling, and simulations, we show that dipolar interactions drive robust JP-JP and JP-PS dimer formation with frequency-dependent stability. At intermediate and high frequencies, JP-PS binding is strongly attractive, whereas at low frequencies it becomes effectively repulsive due to electrical double-layer screening and electrohydrodynamic flows at the metallic hemisphere. In multi-particle systems, PS beads act as cooperative hubs that hierarchically recruit JPs, yielding higher-order hybrid structures. We identify structural isomers - for example, 3JP + 1PS clusters can form chain-like or triangular configurations depending on assembly sequence. Simulations confirm both as equilibrium states, with the triangular isomer slightly more stable. Similar polymorphism appears in larger clusters (4JPs). Overall, we establish a framework for controlled active-passive colloidal assembly, showing how frequency-tunable interactions and structural polymorphism enable the design of reconfigurable colloidal machines for applications in microrobotics, targeted delivery, and adaptive materials.