The development of renewable energy technologies is crucial for the goal of a global sustainable society. For reaching this goal, solar energy technologies that rely on the efficient utilization of abundant sunlight play an important role. To this end, plasmon-enhanced processes enabled by metal nanoparticles provide particularly promising avenues for harvesting sunlight.
Plasmon-enhanced technologies are based on metal nanoparticles that support localized surface plasmon resonances. Thanks to these resonances, metal nanoparticles exhibit large photoabsorption cross-sections, which makes them efficient light absorbers. Upon light absorption, the absorbed energy is confined in the nanometer-scale volume of the nanoparticle, and a particularly attractive approach for utilizing this energy is through plasmonic catalysis. In this process, the plasmon resonance decays on a femtosecond timescale, creating high-energy electrons and holes, so-called hot carriers. These plasmon-generated hot carriers could trigger chemical reactions in molecules adsorbed on the nanoparticle surface, turning metal nanoparticles into solar-to-chemical energy converters.
Detailed understanding of plasmonic hot-carrier generation at the atomic scale is highly important for plasmonic catalysis as chemical reactions take place at this size scale. In this spirit, the main objectives of this project were to develop computational first-principles methods for addressing plasmonic hot-carrier generation with atomistic resolution and to gain understanding of the atomic-scale effects on plasmonic hot-carrier generation by utilizing the developed methods. These aims were achieved in the project and the developed understanding and methods form a basis for further explorations of atomic-scale contributions.
