Versatile Deposition of Complex Colloidal Assemblies from the Evaporation of Hanging Drops

Abstract Existing strategies designed to produce ordered arrangements of colloidal particles on solid supports are of great interest for their wide range of applications, from colloidal lithography, plasmonic and biomimetic surfaces to tags for anti‐counterfeiting, but they all share various degrees of complexity hampering their facile implementation. Here, a drastically simplified methodology is presented to achieve ordered particle deposition, consisting in adding micromolar amounts of cationic surfactant to a colloidal suspension drop and let it evaporate in an upside‐down configuration. Confinement at the air/water interface enables particle assembly into monolayers, which are then transferred on the substrate producing highly ordered structures displaying vivid, orientation‐dependent structural colors. The method is compatible with many particle types and substrates, while controlling system parameters allows tuning the deposit size and morphology, from monocrystals to polycrystalline disks and “irises”, from single‐component to crystal alloys with Moiré patterns, demonstrating its practicality for a variety of processes.