Unconventional Optical Matter of Hybrid Metal-Dielectric Nanoparticles at Interfaces.

Optical matter, a transient arrangement formed by the interaction of light with micro/nanoscale objects, provides responsive and highly tunable materials that allow for controlling and manipulating light and/or matter. A combined experimental and theoretical exploration of optical matter is essential to advance our understanding of the phenomenon and potentially design applications. Most studies have focused on nanoparticles composed of a single material (either metallic or dielectric), representing two extreme regimes, one where the gradient force (dielectric) and one where the scattering force (metallic) dominates. To understand their role, it is important to investigate hybrid materials with different metallic-to-dielectric ratios. Here, we combine numerical calculations and experiments on hybrid metal-dielectric core-shell particles (200 nm gold spheres coated with silica shells with thicknesses ranging from 0 to 100 nm). We reveal how silica shell thickness critically influences the essential properties of optical binding, such as interparticle distance, reducing it below the anticipated optical binding length. Notably, for silica shells thicker than 50 nm, we observed a transition from a linear arrangement perpendicular to polarization to a hexagonal arrangement accompanied by a circular motion. Further, the dynamic swarming assembly changes from the conventional dumbbell-shaped to lobe-like morphologies. These phenomena, confirmed by both experimental observations and dynamic numerical calculations, demonstrate the complex dynamics of optical matter and underscore the potential for tuning its properties for applications.