In comparison to the top-down approaches, nanocomposite thin films are more compatible with nanoparticle (NP) chemistry, device integration and scalable manufacturing. It has been long promised as an ideal option to fabricate metamaterial to harvest collective properties from 3D NP assemblies. However, most of accessible NP assemblies governed by the phase diagram are not suitable to achieve targeted properties and require rather lengthy assembly process. Here, we investigated the kinetic pathway of NP assembly in lamellar supramolecular nanocomposite thin films during solvent annealing and after solvent removal. By balancing the solvent field, diffusion rate and thermodynamic driving force during rapid solvent removal (less than 3 seconds), we realized well-ordered 3D NP assemblies far away from the equilibrium state. The degree of ordering depends on the terminal solvent fraction rather than the solvent removal rate. The periodicity of nanocomposite and the NP size can be readily decoupled and reduced to ~50% of the equilibrium value to modulate the optical properties of thin film coatings. The current study provides a facile approach to access non-equilibrium structure in nanocomposites for the fabrication of functional metamaterial coatings.<br/>

Toward designer nanocomposites

2019 Spring National Meeting

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