Atomistic Theory of Hot-Carrier Relaxation in Large Plasmonic Nanoparticles.

Recently, there has been significant interest in harnessing hot-carriers generated from the decay of localized surface plasmons in metallic nanoparticles for applications in photocatalysis, photovoltaics, and sensing. In this work, we develop an atomistic method that makes it possible to predict the population of hot-carriers under continuous wave illumination for large nanoparticles of relevance to experimental studies. For this, we solve the equation of motion of the density matrix, taking into account both the excitation of hot-carriers and subsequent relaxation effects.