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Many experimental systems consist of large ensembles of uncoupled or weaklyinteracting elements operating as a single whole; this is the case in manyexperimental systems in nano-optics and plasmonics including colloidalsolutions, plasmonic nanoparticles, dielectric resonators, antenna arrays, andothers. In such experiments, measurements of the optical spectra of ensembleswill differ from measurements of the independent elements even if theseelements are designed to be identical as a result of small variations fromelement to element, known as polydispersity. In particular, sharp spectralfeatures arising from narrow-band resonances will tend to appear broader andcan even be washed out completely. Here, we explore this effect ofinhomogeneous broadening as it occurs in colloidal nano-polymers comprisingself-assembled nanorod chains in solution. Using a technique combiningfinite-difference time-domain (FDTD) simulations and Monte-Carlo sampling, wepredict the inhomogeneously-broadened optical spectra of these colloidalnano-polymers, and observe significant qualitative differences compared to theunbroadened spectra. The approach combining an electromagnetic simulationtechnique with Monte-Carlo sampling is widely applicable for quantifying theeffects of inhomogeneous broadening in a variety of physical systems, includingthose with many degrees of freedom which are otherwise computationallyintractable.

Monte-Carlo-based electromagnetic modeling of nanoscale structures: accounting for inhomogeneous broadening in polydisperse ensembles