<Abstract>

Nanocomposite thin films containing well-ordered nanoparticle (NP) assemblies are

ideal candidates for the fabrication of metamaterials. Achieving 3-D assembly of NPs in

nanocomposite thin films is thermodynamically challenging as the particle size gets

similar to that of a single polymer chain. The entropic penalties of polymeric matrix upon

NP incorporation leads to NP aggregation on the film surface or within the defects in

the film. Controlling the kinetic pathways of assembly process provides an alternative

path forward by arresting the system in nonequilibrium states. Here, we report the thin

film 3-D hierarchical assembly of 20 nm NPs in supramolecules with a 30 nm periodicity.

By mediating the NP diffusion kinetics in the supramolecular matrix, surface aggregation

of NPs was suppressed and NPs coassemble with supramolecules to form new 3-D

morphologies in thin films. The present studies opened a viable route to achieve designer

functional composite thin films via kinetic control.
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