Particle Arrangements and Optical Changes Induced by the Water Swelling of Melanin-Like Polydopamine Layers

The assembled structures of melanin particles, i.e., colloidal particles coated with a melanin-like polydopamine (PDA) layer, create vivid structural colors. While the thickness of the PDA layer influences the particle arrangement and optical properties, the underlying mechanism has remained controversial. We demonstrate that the water-swelling characteristics of PDA are crucial factors governing the dispersion and aggregation of these particles in solution. Detailed comparisons between dry and wet conditions revealed that the PDA layer readily absorbs water molecules, which leads to significant swelling in the thicker layers. The swelling of the PDA layers determined whether the particles remained dispersed or partially aggregated in the water, ultimately controlling the particle arrangement in the dry state once the water evaporated. These findings provide insights into the self-assembly of colloidal particles and offer a strategy for tuning the periodic particle order. This feature is pivotal for various applications in optical and sensing technologies.