Effective-medium description of dense clusters of plasmonic nanoparticles with spatial dispersion

We study the electromagnetic behavior of dense, spherical clusters made of hundreds of plasmonic nanoparticles under illumination by a plane wave. Using high-precision T-matrix numerical calculations, we compute the multipolar response of clusters up to 80 nm in radius and up to 44% in particle volume fraction. We then investigate whether it is possible to obtain an effective-medium description for the clusters, taking into account weak spatial dispersion in a fully consistent way. We find that the average scattered field as well as the average inner field of the spherical cluster can be accurately reproduced by applying an extended Mie theory to an equivalent homogeneous sphere characterized by three effective parameters: an electric permittivity ${\ensuremath{\varepsilon}}_{\mathrm{eff}}$ and a magnetic permeability ${\ensuremath{\mu}}_{\mathrm{eff}}$, associated to transverse modes, and a wave vector ${k}_{\mathrm{L}}$, associated to a longitudinal mode in the sphere. Our results show that artificial magnetism arises from interparticle couplings in the dense cluster, despite inclusions not displaying any individual magnetic dipole. We also find that, although largely overlooked in the literature on metamaterials, the presence of the longitudinal mode is essential to accurately reproduce the fields of the cluster, on par with the role of artificial magnetism. Our paper therefore proves that, even for high concentration in inclusions, it is possible empirically to treat a cluster of plasmonic particles as a sphere made of a spatially dispersive homogeneous medium. This offers a practical solution facilitating the computation of electromagnetic responses of such dense random media in diverse configurations of interest for the design of metamaterials and metasurfaces.