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

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 Ag 55 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.

Authors:
 [1];  [2];  [1]
+ Show Author Affiliations
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1255542
Alternate Identifier(s):
OSTI ID: 1378695
Grant/Contract Number:  
AC05-00OR22725; SC0004993; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Ma, Jie, Wang, Zhi, and Wang, Lin-Wang. Interplay between plasmon and single-particle excitations in a metal nanocluster. United States: N. p., 2015. Web. doi:10.1038/ncomms10107.
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Ma, Jie, Wang, Zhi, & Wang, Lin-Wang. Interplay between plasmon and single-particle excitations in a metal nanocluster. United States. https://doi.org/10.1038/ncomms10107
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Ma, Jie, Wang, Zhi, and Wang, Lin-Wang. Thu . "Interplay between plasmon and single-particle excitations in a metal nanocluster". United States. https://doi.org/10.1038/ncomms10107. https://www.osti.gov/servlets/purl/1255542.
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@article{osti_1255542,
title = {Interplay between plasmon and single-particle excitations in a metal nanocluster},
author = {Ma, Jie and Wang, Zhi and Wang, Lin-Wang},
abstractNote = {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 Ag 55 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.},
doi = {10.1038/ncomms10107},
journal = {Nature Communications},
number = ,
volume = 6,
place = {United States},
year = {2015},
month = {12}
}
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https://doi.org/10.1038/ncomms10107
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