Ab initio quantum dynamics of plasmonic charge carriers

Surface plasmons respond strongly to electric fields and generate energetic (hot) charge carriers that can be used in optoelectronic devices. However, utilization of hot carriers has to outcompete fast carrier relaxation in metals. Often, the reported efficiencies of nanoscale devices based on plasmon excitations are low and the mechanisms of device operation remain inconsistent within the field. Further de-velopments hinge on fundamental understanding of the nature and kinetics of plasmon decay processes. We provide an overview of time domain ab initio modeling of hot carrier dynamics, demonstrating that atomistic details of the sur-face structure of plasmonic materials, and their chemical interaction with semi-conducting and molecular charge acceptors and substrates, play key roles in governing the dynamics pathways. Considered case studies represent various dynamics channels and illustrate solar energy and optoelectronic applications.