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Interplay between plasmon and single-particle excitations in a metal nanocluster

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  • Jie Ma

    (Lawrence Berkeley National Laboratory)

  • Zhi Wang

    (Lawrence Berkeley National Laboratory)

  • Lin-Wang Wang

    (Lawrence Berkeley National Laboratory)

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.

Suggested Citation

  • Jie Ma & Zhi Wang & Lin-Wang Wang, 2015. "Interplay between plasmon and single-particle excitations in a metal nanocluster," Nature Communications, Nature, vol. 6(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:6:y:2015:i:1:d:10.1038_ncomms10107
    DOI: 10.1038/ncomms10107
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