Title: Plasmon Decay and Hot Carrier Generation in Plasmonic Nano Particles from Ab Initio

Abstract: Metallic nanostructures efficiently localize the electromagnetic energy to subwavelength regime. The localized electromagnetic energy is quick to dephase into hot electrons and holes, a phenomenon commonly phrased as losses, but which may be harnessed in photochemical reactions. We analyze the coherent dynamics of light absorption, plasmon buildup and subsequent hot carrier generation for Ag, Au and Cu nanoclusters using real time time-dependent density functional theory. Quantitative results on hot-electron distribution and plasmon energetics are obtained by analyzing the single particle density matrix. In our bottom-up approach, quantitative differences on hot-electron distributions in nanoparticles are found varying in material and shape. In the presented approach, the plasmonic fields are handled self-consistently and no empirical input, such as dielectric functions are required.