Plasmonic surface nanostructuring of Au-dots@SiO₂ via laser-irradiation induced dewetting

The in situ observation of Au dot formation and the self-assembly dynamics of Au nanoparticles (NPs) was successfully demonstrated via dewetting of Au thin films on SiO₂ glass substrates under nano-second pulsed laser irradiation using a multi-quantum beam high-voltage electron microscope. Moreover, using electron energy-loss spectroscopy (EELS) performed in a scanning transmission electron microscope (STEM), the plasmonic properties of the formed Au/SiO₂ nanostructure were analyzed to demonstrate its validity in advanced optical devices. The uniformly distributed Au NPs evolved into a dot alignment through movement and coalescence processes was demonstrated in this in situ observation. We carried out the plasmon-loss images of the plan view and the cross-section of the Au/SiO₂ nanostructures were obtained at the plasmon-loss peak energy for investigate the three-dimensional distribution of surface plasmon. Furthermore, discrete-dipole approximation (DDA) calculations were used to simulate the plasmonic properties, such as the surface plasmon resonance and the surface plasmon field distribution, of isolated single Au/SiO₂ nanostructures. This STEM-EELS-acquired surface plasmon map of the cross-sectional sample is in excellent agreement with the DDA calculations. This results demonstrated the influence of the contact condition between Au NP and SiO₂ glass on the plasmonic properties, and may improve the technology for developing advanced optical devices.