Uncovering the fundamental mechanisms behind plasmon mediated processes is the key to improve the efficiency of plasmonic materials. Light-induced processes in silver nanoparticles are of great interest, thanks to their strong absorption properties in the UV/Vis region. Due to the complexity and the ultrafast nature, nonradiative plasmon decay processes that occur in femtosecond time scale is challenging to recognize experimentally and theoretically. Real-time time-dependent density functional theory (RT-TDDFT) is an ideal tool to track fast electronic motion subjected to a perturbation. Previous work suggests plasmon dephasing into hot carriers in silver nanoparticles. Our recent studies shine light on the emergence of non-linear optical properties in a tetrahedral silver cluster as a result of plasmon decay. In this work, we focus on several silver nanoparticles with various sizes and shapes, namely, Ag10+2 (Td), Ag13+5 (Ih), Ag13-1(Oh), Ag19+1 (D5h), Ag20 (Td), and Ag55-3 (Ih). We investigate how the symmetry of the nanoparticle promote or impede the non-linear properties and the size dependency towards multiphoton absorption in silver nanoclusters.

Non-linear optical activation in silver nanoclusters as a plasmon decay mechanism

ACS Spring Meeting 2021

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