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Slow Relaxation of Surface Plasmon Excitations in Au55: The Key to Efficient Plasmonic Heating in Au/TiO2.

Gold nanoparticles distinguish themselves from other nanoparticles due to their unique surface plasmon resonance properties that can be exploited for a multiplicity of applications. The promise of plasmonic heating in systems of Au nanoparticles on transition metal oxide supports, for example, Au/TiO2, rests with the ability of the surface plasmon in Au nanoparticles to effectively transfer energy into the transition metal oxide. Here, we report a critical observation regarding Au nanoparticle (Au55) surface plasmon excitations, that is, the relaxation of the surface plasmon excitation is very slow, on the order of several picoseconds. Starting from five plasmon states in Au55 nanoparticles using nonadiabatic molecular dynamics simulations, we find that the relaxation time constant resulting from these simulations is ∼6.8 ps, mainly resulting from a long-lived intermediate state found at around -0.8 eV. This long-lived intermediate state aligns with the conduction band edge of TiO2, thereby facilitating energy transfer injection from the Au55 nanoparticle into the TiO2. The current results rule out the previously reported molecular-like relaxation dynamics for Au55.