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Recently, there has been significant interest in harnessing hot carriersgenerated from the decay of localized surface plasmons in metallicnanoparticles for applications in photocatalysis, photovoltaics and sensing. Inthis work, we present an atomistic approach to predict the population of hotcarriers under continuous wave illumination in large nanoparticles. For this,we solve the equation of motion of the density matrix taking into account bothexcitation of hot carriers as well as subsequent relaxation effects. We presentresults for spherical Au and Ag nanoparticles with up to $250,000$ atoms. Wefind that the population of highly energetic carriers depends both on thematerial and the nanoparticle size. We also study the increase in theelectronic temperature upon illumination and find that Ag nanoparticles exhibita much larger temperature increase than Au nanoparticles. Finally, weinvestigate the effect of using different models for the relaxation matrix butfind that qualitative features of the hot-carrier population are robust.

Atomistic theory of hot carrier relaxation in large plasmonic nanoparticles