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hot_electron_2019.pdf (1.98 MB)
Plasmon-Induced Hot-Carrier Generation differences in Gold and Silver Nanoclusters
Preprints are manuscripts made publicly available before they have been submitted for formal peer review and publication. They might contain new research findings or data. Preprints can be a draft or final version of an author's research but must not have been accepted for publication at the time of submission.
submitted on 27.03.2019, 23:03 and posted on 28.03.2019, 15:30by Oscar A. Douglas-Gallardo, Matias Berdakin, Thomas Frauenheim, Cristián G Sánchez
In the last thirty years, the study of plasmonic properties of noble metal nanostructures has become a very dynamic research area. The design and manipulation of matter in the nanometric scale demand a deep understanding of the underlying physico-chemical processes that operate in this size regimen. Here, a fully atomistic study of the spectroscopic and photodynamic properties of different icosahedral silver and gold nanoclusters have been carried out by using Time-Dependent Density Functional Tight-Binding (TD-DFTB) model. Optical absorption spectra of different icosahedral silver and gold nanoclusters of diameters between 1 and 4 nanometers has been simulated. Furthermore, the energy absorption process have been quantified by means of calculating a fully quantum absorption cross-section using the information contained in the reduced single-electron density matrix. This approach allows us take into account for the quantum confinement effects dominating in this size regime. Likewise, the plasmon-induced hot-carrier generation process under laser illuminations have been explored from a fully dynamical perspective. We have found noticeable differences in the energy absorption mechanisms and the plasmon-induced hot-carrier generation process in both metals which can be explained by their respective electronic structures. These difference can be attributed to the existence of ultra-fast electronic dissipation channels in gold nanoclusters that are absented in silver nanoclusters. To the best of our knowledge, this is the first report that addresses this topic from a real time fully atomistic time-dependent approach.