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Polyelectrolyte multilayers were deposited onto polystyrene and melamine formaldehyde latex particles by means of consecutive adsorption. Two different methods of multilayer growth were employed. First, adsorption of polyelectrolytes at a concentration exceeding saturation amounts was combined with the removal of the nonbound polyelectrolyte by means of centrifugation. Second, adsorption of polyelectrolyte was performed at a concentration just sufficient for saturation coverage. Both methods yielded continuous layer growth. The process of film formation was followed by electrophoresis, dynamic light scattering, single particle light scattering and fluorescence intensity measurements. Layer deposition onto partially crosslinked melamine resin latex particles, which were soluble at pH values of less than 1.6, resulted in the production of three‐dimensional thin polyelectrolyte shells upon dissolving the core. The ultrathin shells were observed by means of scanning and transmission electron microscopy. © 1998 John Wiley & Sons, Ltd.

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Structuring over many length scales is a design strategy widely used in Nature to create materials with unique functional properties. We here present a comprehensive analysis of an adult sea urchin spine, and in revealing a complex, hierarchical structure, show how Nature fabricates a material which diffracts as a single crystal of calcite and yet fractures as a glassy material. Each spine comprises a highly oriented array of Mg-calcite nanocrystals in which amorphous regions and macromolecules are embedded. It is postulated that this mesocrystalline structure forms via the crystallization of a dense array of amorphous calcium carbonate (ACC) precursor particles. A residual surface layer of ACC and/or macromolecules remains around the nanoparticle units which creates the mesocrystal structure and contributes to the conchoidal fracture behavior. Nature’s demonstration of how crystallization of an amorphous precursor phase can create a crystalline material with remarkable properties therefore provides inspiration for a novel approach to the design and synthesis of synthetic composite materials.