We theoretically analyze, fabricate, and characterize a three-dimensional plasmonic nanostructure that exhibits a strong and isotropic magnetic response in the visible spectral domain. Using two different bottom-up approaches that rely on self-organization and colloidal nanochemistry, we fabricate clusters consisting of dielectric core spheres, which are smaller than the wavelength of the incident radiation and are decorated by a large number of metallic nanospheres. Hence, despite having a complicated inner geometry, such a core-shell particle is sufficiently small to be perceived as an individual object in the far field. The optical properties of such complex plasmonic core-shell particles are discussed for two different core diameters.

Metallic nanostructures that sustain plasmonic resonances are indispensable ingredients for many functional devices. Whereas structures fabricated with top-down methods entail the advantage of a nearly unlimited control over all plasmonic properties, they are in most cases unsuitable for a low cost fabrication on large surfaces; and eventually a truly nanometric size domain is difficult to reach due to limitations in the fabrication resolution. Although ordinary bottom-up techniques based on colloidal nanolithography promise to lift these limitations, they often suffer from their incapability to self-assemble nanoparticles at large surfaces and at a density necessary to observe effects that strongly deviate from those of isolated nanoparticles. Here, we rely on the application of sequential bottom-up fabrication steps to realize honeycomb structures from gold nanoparticles that show strong extinction bands in the near-infrared. The extraordinary properties are only facilitated by densely packing the nanoparticles into clusters with a finite size; causing the clusters to act as plasmonic macromolecules. These strongly interacting bottom-up materials with a deterministic geometry but fabricated by self-assembly might be of use in future sensing applications and in material platforms to mediate strong light−matter-interactions.

A method for the production of homogeneous layers of nanoparticles of arbitrary shape is presented. The method relies on a ligand exchange with a functionalized polymer and a subsequent self‐assembly of a thin film on the substrates. The interparticle distances in the layer can be adjusted by the length of the polymer. In the case of spherical particles, the approach yields quasi‐hexagonal structures; in the case of anisotropic particles, the minimum distance between adjacent particles is controlled. Regular arrangements of the nanoparticles covering areas of several square centimeters are achieved.