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

doi:10.1038/ncomms10107

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

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. Ultimately, this study provides guidance on improving plasmonic applications.

Authors:

Ma, Jie ^[1] ; Wang, Zhi ^[2] ; Wang, Lin-Wang ^[1]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division

Publication Date:: 2015-12-17

Grant/Contract Number:: AC05-00OR22725; SC0004993; AC02-05CH11231

Type:: Accepted Manuscript

Journal Name:: Nature Communications

Additional Journal Information:: Journal Volume: 6; Journal ID: ISSN 2041-1723

Publisher:: Nature Publishing Group

Research Org:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Org:: USDOE Office of Science (SC)

Country of Publication:: United States

Language:: English

Subject:: 77 NANOSCIENCE AND NANOTECHNOLOGY

OSTI Identifier:: 1255542

Alternate Identifier(s):: OSTI ID: 1378695


                    Ma, Jie, Wang, Zhi, and Wang, Lin-Wang. Interplay between plasmon and single-particle excitations in a metal nanocluster.  United States: N. p.,  
        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.  doi:10.1038/ncomms10107.

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                    Ma, Jie, Wang, Zhi, and Wang, Lin-Wang. 2015.  
        "Interplay between plasmon and single-particle excitations in a metal nanocluster".  United States.  
        doi: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 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. Ultimately, 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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10.1038/ncomms10107
https://doi.org/10.1038/ncomms10107

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Works referenced in this record:

Plasmonics for improved photovoltaic devices
journal, February 2010

Atwater, Harry A.; Polman, Albert
Nature Materials, Vol. 9, Issue 3, p. 205-213
DOI: 10.1038/nmat2629

Probing Single Molecules and Single Nanoparticles by Surface-Enhanced Raman Scattering
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Nie, Shuming; Emory, Steven R.
Science, Vol. 275, Issue 5303, p. 1102-1106
DOI: 10.1126/science.275.5303.1102

Photodetection with Active Optical Antennas
journal, May 2011

Knight, M. W.; Sobhani, H.; Nordlander, P.
Science, Vol. 332, Issue 6030, p. 702-704
DOI: 10.1126/science.1203056

Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965

Kohn, W.; Sham, L. J.
Physical Review, Vol. 140, Issue 4A, p. A1133-A1138
DOI: 10.1103/PhysRev.140.A1133

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

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