{"database":"biostudies-other","file_versions":[],"scores":null,"additional":{"omics_type":["Unknown"],"volume":["6"],"submitter":["Ma J"],"journal":["Nature communications"],"pagination":["10107"],"full_dataset_link":["https://www.ebi.ac.uk/biostudies/studies/S-EPMC4703846"],"abstract":["Plasmon-generated hot carriers are used in photovoltaic or photochemical applications. However, the interplays between the plasmon and single-particle excitations in nanosystems have not been theoretically addressed using ab initio methods. Here we show such interplays in a Ag55 nanocluster using real-time time-dependent density functional theory simulations. We find that the disappearance of the zero-frequency peak in the Fourier transform of the band-to-band transition coefficient is a hallmark of the plasmon. We show the importance of the d-states for hot-carrier generations. If the single-particle d-to-s excitations are resonant to the plasmon frequency, the majority of the plasmon energy will be converted into hot carriers, and the overall hot-carrier generation is enhanced by the plasmon; if such resonance does not exist, we observe an intriguing Rabi oscillation between the plasmon and hot carriers. Phonons play a minor role in plasmonic dynamics in such small systems. This study provides guidance on improving plasmonic applications."],"repository":["biostudies-other"],"pmcid":["PMC4703846"],"data_source":["Europe PMC"],"pubmed_authors":["Wang LW","Ma J","Wang Z"],"additional_accession":[]},"is_claimable":false,"name":"Interplay between plasmon and single-particle excitations in a metal nanocluster.","description":"Plasmon-generated hot carriers are used in photovoltaic or photochemical applications. However, the interplays between the plasmon and single-particle excitations in nanosystems have not been theoretically addressed using ab initio methods. Here we show such interplays in a Ag55 nanocluster using real-time time-dependent density functional theory simulations. We find that the disappearance of the zero-frequency peak in the Fourier transform of the band-to-band transition coefficient is a hallmark of the plasmon. We show the importance of the d-states for hot-carrier generations. If the single-particle d-to-s excitations are resonant to the plasmon frequency, the majority of the plasmon energy will be converted into hot carriers, and the overall hot-carrier generation is enhanced by the plasmon; if such resonance does not exist, we observe an intriguing Rabi oscillation between the plasmon and hot carriers. Phonons play a minor role in plasmonic dynamics in such small systems. This study provides guidance on improving plasmonic applications.","dates":{"release":"2015-01-01T00:00:00Z","publication":"2015 ","modification":"2019-03-27T02:06:25Z","creation":"2019-03-27T02:06:25Z"},"accession":"S-EPMC4703846","cross_references":{"pubmed":["26673449"],"doi":["10.1038/ncomms10107 "]}}