Energy and Charge Transfer in Open Plasmonic Systems

Abstract

Coherent and collective charge oscillations in metal nanoparticles (MNPs), known as localized surface plasmons, offer unprecedented control and enhancement of optical processes on the nanoscale. Since their discovery in the 1950's, plasmons have played an important role in understanding fundamental properties of solid state matter and have been used for a variety of applications, from single molecule spectroscopy to directed radiation therapy for cancer treatment. More recently, experiments have demonstrated quantum interference between optically excited plasmonic materials, opening the door for plasmonic applications in quantum information and making the study of the basic quantum mechanical properties of plasmonic structures an important research topic. This text describes a quantitatively accurate, versatile model of MNP optics that incorporates MNP geometry, local environment, and effects due to the quantum properties of conduction electrons and radiation. We build the theory from first principles, starting with a silver sphere in isolation and working our way up to complex, interacting plasmonic systems with multiple MNPs and other optical resonators. We use mathematical methods from statistical physics and quantum optics in collaboration with experimentalists to reconcile long-standing discrepancies amongst experiments probing plasmons in the quantum size regime, to develop and model a novel single-particle absorption spectroscopy, to predict radiative interference effects in entangled plasmonic aggregates, and to demonstrate the existence of plasmons in photo-doped semiconductor nanocrystals. These examples show more broadly that the theory presented is easily integrated with numerical simulations of electromagnetic scattering and that plasmonics is an interesting test-bed for approximate methods associated with multiscale systems.