Janus particles, colloid-sized particles with two regions of different surface chemical composition, possess energetic interactions that depend not only on their separation but also on their orientation. Research on Janus and colloidal particles that are chemically patchy in even more complicated fashion has opened a new chapter in the colloid research field. This article highlights recent progress in both experiment and theory regarding synthesis and self-assembly of Janus particles, and tentatively outlines some areas of future opportunity.

Clusters in the form of aggregates of a small number of elemental units display structural, thermodynamic, and dynamic properties different from those of bulk materials. We studied the kinetic pathways of self-assembly of "Janus spheres" with hemispherical hydrophobic attraction and found key differences from those characteristic of molecular amphiphiles. Experimental visualization combined with theory and molecular dynamics simulation shows that small, kinetically favored isomers fuse, before they equilibrate, into fibrillar triple helices with at most six nearest neighbors per particle. The time scales of colloidal rearrangement combined with the directional interactions resulting from Janus geometry make this a prototypical system to elucidate, on a mechanistic level and with single-particle kinetic resolution, how chemical anisotropy and reaction kinetics coordinate to generate highly ordered structures.

Active materials represent a new class of condensed matter in which motile elements may collectively form dynamic, global structures out of equilibrium. Here, we present a general strategy to reconfigure active particles into various collective states by introducing imbalanced interactions. We demonstrate the concept with computer simulations of self-propelled colloidal spheres, and experimentally validate it in a two-dimensional (2D) system of metal-dielectric Janus colloids subjected to perpendicular a.c. electric fields. The mismatched, frequency-dependent dielectric responses of the two hemispheres of the colloids allow simultaneous control of particle motility and colloidal interactions. We realized swarms, chains, clusters and isotropic gases from the same precursor particle by changing the electric-field frequency. Large-scale polar waves, vortices and jammed domains are also observed, with the persistent time-dependent evolution of their collective structure evoking that of classical materials. This strategy of asymmetry-driven active self-organization should generalize rationally to other active 2D and three-dimensional (3D) materials.