Thermal crowning mechanism in gold-silica nanocomposites: plasmonic-photonic pairing in archetypal two-dimensional structures.

A close-packed monolayer of a two-dimensional periodic array of Silica nanospheres (SNs) with gold (Au) crowning, forming a long-ranged archetypal plasmonic-photonic nanocomposite, has been achieved. We investigate the thermal crowning mechanism in such a nanocomposite using electron microscopy and X-ray diffraction techniques. Pre- and post-annealing morphological features reveal gold crowning on top of SNs, at different annealing temperatures for various thicknesses of the sputter-deposited gold. In situ grazing incidence X-ray diffraction was employed to structurally characterize the reconstruction in the Au-layer as a function of the annealing temperature. Finite element methods were used to simulate the interaction between the paired nanocomposites and the incident electromagnetic radiations to elucidate the crowning and nanodrop formation mechanism. This study provides an insight into real-time morphological and structural changes of a dewetting plasmonic film over a photonic basis and explores a robust, reliable, and scalable route to fabricate coupled nanocomposites. Such nanocomposites allow prospective applications in optoelectronics, sensing, catalysis, and surface-enhanced Raman spectroscopy by exploiting the plasmonic-photonic pairing in archetypal two-dimensional structures.