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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. doi: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. 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 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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DOI:  10.1038/ncomms10107
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Works referenced in this record:

Plasmon-induced hot carrier science and technology
journal, January 2015

  • Brongersma, Mark L.; Halas, Naomi J.; Nordlander, Peter
  • Nature Nanotechnology, Vol. 10, Issue 1
  • DOI: 10.1038/nnano.2014.311

Time-Dependent Density Functional Theory Studies of Optical Properties of Ag Nanoparticles: Octahedra, Truncated Octahedra, and Icosahedra
journal, May 2012

  • Bae, Gyun-Tack; Aikens, Christine M.
  • The Journal of Physical Chemistry C, Vol. 116, Issue 18
  • DOI: 10.1021/jp300789x

First-Principles Computational Visualization of Localized Surface Plasmon Resonance in Gold Nanoclusters
journal, November 2014

  • Iida, Kenji; Noda, Masashi; Ishimura, Kazuya
  • The Journal of Physical Chemistry A, Vol. 118, Issue 47
  • DOI: 10.1021/jp5088042

Femtosecond Nanoplasmonic Dephasing of Individual Silver Nanoparticles and Small Clusters
journal, April 2015

  • Mittal, Richa; Glenn, Rachel; Saytashev, Ilyas
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 9
  • DOI: 10.1021/acs.jpclett.5b00264

Quantum coherent plasmon in silver nanowires: A real-time TDDFT study
journal, June 2014

  • Ding, Feizhi; Guidez, Emilie B.; Aikens, Christine M.
  • The Journal of Chemical Physics, Vol. 140, Issue 24
  • DOI: 10.1063/1.4884388

Gold Nanowires: A Time-Dependent Density Functional Assessment of Plasmonic Behavior
journal, August 2013

  • Piccini, GiovanniMaria; Havenith, Remco W. A.; Broer, Ria
  • The Journal of Physical Chemistry C, Vol. 117, Issue 33
  • DOI: 10.1021/jp405769e

Distinguishing between plasmon-induced and photoexcited carriers in a device geometry
journal, July 2015

  • Zheng, Bob Y.; Zhao, Hangqi; Manjavacas, Alejandro
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8797

Electronic structure methods for studying surface-enhanced Raman scattering
journal, January 2008

  • Jensen, Lasse; Aikens, Christine M.; Schatz, George C.
  • Chemical Society Reviews, Vol. 37, Issue 5
  • DOI: 10.1039/b706023h

Plasmons in supported size-selected silver nanoclusters
journal, January 2015

  • Lünskens, Tobias; Heister, Philipp; Thämer, Martin
  • Physical Chemistry Chemical Physics, Vol. 17, Issue 27
  • DOI: 10.1039/C5CP01582K

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

The Optical Properties of Metal Nanoparticles:  The Influence of Size, Shape, and Dielectric Environment
journal, January 2003

  • Kelly, K. Lance; Coronado, Eduardo; Zhao, Lin Lin
  • The Journal of Physical Chemistry B, Vol. 107, Issue 3
  • DOI: 10.1021/jp026731y

End and Central Plasmon Resonances in Linear Atomic Chains
journal, May 2007

Plasmons in molecules: Microscopic characterization based on orbital transitions and momentum conservation
journal, September 2014

  • Krauter, Caroline M.; Schirmer, Jochen; Jacob, Christoph R.
  • The Journal of Chemical Physics, Vol. 141, Issue 10
  • DOI: 10.1063/1.4894266

Modeling Fast Electron Dynamics with Real-Time Time-Dependent Density Functional Theory: Application to Small Molecules and Chromophores
journal, April 2011

  • Lopata, Kenneth; Govind, Niranjan
  • Journal of Chemical Theory and Computation, Vol. 7, Issue 5
  • DOI: 10.1021/ct200137z

The Structures of Ag 55 + and Ag 55 - :  Trapped Ion Electron Diffraction and Density Functional Theory
journal, October 2005

  • Schooss, Detlef; Blom, Martine N.; Parks, Joel H.
  • Nano Letters, Vol. 5, Issue 10
  • DOI: 10.1021/nl0513434

Plasmons driven by single electrons in graphene nanoislands
journal, January 2013

  • Manjavacas, Alejandro; Thongrattanasiri, Sukosin; de Abajo, F. Javier García
  • Nanophotonics, Vol. 2, Issue 2
  • DOI: 10.1515/nanoph-2012-0035

Tunable plasmons in atomically thin gold nanodisks
journal, March 2014

  • Manjavacas, A.; García de Abajo, F. J.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4548

Mechanisms and Applications of Plasmon-Induced Charge Separation at TiO 2 Films Loaded with Gold Nanoparticles
journal, May 2005

  • Tian, Yang; Tatsuma, Tetsu
  • Journal of the American Chemical Society, Vol. 127, Issue 20
  • DOI: 10.1021/ja042192u

Radiative effects in plasmonic aluminum and silver nanospheres and nanorods
journal, December 2014

Theoretical predictions for hot-carrier generation from surface plasmon decay
journal, December 2014

  • Sundararaman, Ravishankar; Narang, Prineha; Jermyn, Adam S.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms6788

Plasmons in Molecules
journal, January 2013

  • Bernadotte, Stephan; Evers, Ferdinand; Jacob, Christoph R.
  • The Journal of Physical Chemistry C, Vol. 117, Issue 4
  • DOI: 10.1021/jp3113073

Origin and TDDFT Benchmarking of the Plasmon Resonance in Acenes
journal, October 2013

  • Guidez, Emilie B.; Aikens, Christine M.
  • The Journal of Physical Chemistry C, Vol. 117, Issue 41
  • DOI: 10.1021/jp4059033

The case for plasmon-derived hot carrier devices
journal, January 2015

Hot Electrons Do the Impossible: Plasmon-Induced Dissociation of H 2 on Au
journal, December 2012

  • Mukherjee, Shaunak; Libisch, Florian; Large, Nicolas
  • Nano Letters, Vol. 13, Issue 1
  • DOI: 10.1021/nl303940z

Plasmonic Properties of Metallic Nanoparticles: The Effects of Size Quantization
journal, December 2011

  • Townsend, Emily; Bryant, Garnett W.
  • Nano Letters, Vol. 12, Issue 1
  • DOI: 10.1021/nl2037613

Theoretical Studies of Plasmonics using Electronic Structure Methods
journal, June 2011

  • Morton, Seth M.; Silverstein, Daniel W.; Jensen, Lasse
  • Chemical Reviews, Vol. 111, Issue 6
  • DOI: 10.1021/cr100265f

Which resonances in small metallic nanoparticles are plasmonic?
journal, November 2014

Theory and computation of hot carriers generated by surface plasmon polaritons in noble metals
journal, June 2015

  • Bernardi, Marco; Mustafa, Jamal; Neaton, Jeffrey B.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8044

Quantum plasmon resonances of individual metallic nanoparticles
journal, March 2012

  • Scholl, Jonathan A.; Koh, Ai Leen; Dionne, Jennifer A.
  • Nature, Vol. 483, Issue 7390
  • DOI: 10.1038/nature10904

From Discrete Electronic States to Plasmons: TDDFT Optical Absorption Properties of Ag n ( n = 10, 20, 35, 56, 84, 120) Tetrahedral Clusters
journal, July 2008

  • Aikens, Christine M.; Li, Shuzhou; Schatz, George C.
  • The Journal of Physical Chemistry C, Vol. 112, Issue 30
  • DOI: 10.1021/jp802707r

High-resolution x-ray photoemission spectra of silver
journal, September 1976

Efficient Real-Time Time-Dependent Density Functional Theory Method and its Application to a Collision of an Ion with a 2D Material
journal, February 2015

Quantum Description of the Plasmon Resonances of a Nanoparticle Dimer
journal, February 2009

  • Zuloaga, Jorge; Prodan, Emil; Nordlander, Peter
  • Nano Letters, Vol. 9, Issue 2
  • DOI: 10.1021/nl803811g

Plasmon-Induced Hot Carriers in Metallic Nanoparticles
journal, July 2014

  • Manjavacas, Alejandro; Liu, Jun G.; Kulkarni, Vikram
  • ACS Nano, Vol. 8, Issue 8
  • DOI: 10.1021/nn502445f

Solid state photovoltaic cells based on localized surface plasmon-induced charge separation
journal, October 2011

  • Takahashi, Yukina; Tatsuma, Tetsu
  • Applied Physics Letters, Vol. 99, Issue 18
  • DOI: 10.1063/1.3659476

Probing Single Molecules and Single Nanoparticles by Surface-Enhanced Raman Scattering
journal, February 1997

Plasmonic Energy Collection through Hot Carrier Extraction
journal, December 2011

  • Wang, Fuming; Melosh, Nicholas A.
  • Nano Letters, Vol. 11, Issue 12
  • DOI: 10.1021/nl203196z

Symmetry and Electronic Structure of Noble-Metal Nanoparticles and the Role of Relativity
journal, August 2004

Optical properties of aggregated metal systems: Interband transitions
journal, February 1977

Conventional and acoustic surface plasmons on noble metal surfaces: A time-dependent density functional theory study
journal, December 2012

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

Plasmon resonance analysis with configuration interaction
journal, January 2014

  • Guidez, Emilie B.; Aikens, Christine M.
  • Physical Chemistry Chemical Physics, Vol. 16, Issue 29
  • DOI: 10.1039/c4cp01365d

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

Enhancement of Single-Molecule Fluorescence Using a Gold Nanoparticle as an Optical Nanoantenna
journal, July 2006

Plasmonic-metal nanostructures for efficient conversion of solar to chemical energy
journal, November 2011

  • Linic, Suljo; Christopher, Phillip; Ingram, David B.
  • Nature Materials, Vol. 10, Issue 12
  • DOI: 10.1038/nmat3151

Time-Dependent Density Functional Theory Studies of Optical Properties of Au Nanoparticles: Octahedra, Truncated Octahedra, and Icosahedra
journal, September 2015

  • Bae, Gyun-Tack; Aikens, Christine M.
  • The Journal of Physical Chemistry C, Vol. 119, Issue 40
  • DOI: 10.1021/acs.jpcc.5b05978
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    journal, May 2018

    • Shi, Qianqian; Sikdar, Debabrata; Fu, Runfang
    • Advanced Materials, Vol. 30, Issue 26
    • DOI: 10.1002/adma.201801118

    Electronic Rearrangement in Molecular Plasmons: An Electron Density and Electrostatic Potential-Based Study
    journal, March 2018

    Strong Collectivity of Optical Transitions in Lead Halide Perovskite Quantum Dots
    journal, January 2020

    Plasmonic hot electron transport drives nano-localized chemistry
    journal, March 2017

    • Cortés, Emiliano; Xie, Wei; Cambiasso, Javier
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms14880

    Single plasmon hot carrier generation in metallic nanoparticles
    journal, May 2019

    • Román Castellanos, Lara; Hess, Ortwin; Lischner, Johannes
    • Communications Physics, Vol. 2, Issue 1
    • DOI: 10.1038/s42005-019-0148-2

    Direct hot-carrier transfer in plasmonic catalysis
    journal, January 2019

    • Kumar, Priyank V.; Rossi, Tuomas P.; Kuisma, Mikael
    • Faraday Discussions, Vol. 214
    • DOI: 10.1039/c8fd00154e

    Plasmon-induced nonlinear response of silver atomic chains
    journal, January 2018

    • Yan, Lei; Guan, Mengxue; Meng, Sheng
    • Nanoscale, Vol. 10, Issue 18
    • DOI: 10.1039/c8nr02086h

    Insight into the charge transport correlation in Au x clusters and graphene quantum dots deposited on TiO 2 nanotubes for photoelectrochemical oxygen evolution
    journal, January 2018

    • Zeng, Zhiping; Li, Yu-Bing; Chen, Shufen
    • Journal of Materials Chemistry A, Vol. 6, Issue 24
    • DOI: 10.1039/c8ta02802h

    Effect of quantum tunneling on the efficiency of excitation energy transfer in plasmonic nanoparticle chain waveguides
    journal, January 2018

    • Ilawe, Niranjan V.; Oviedo, M. Belén; Wong, Bryan M.
    • Journal of Materials Chemistry C, Vol. 6, Issue 22
    • DOI: 10.1039/c8tc01466c

    Momentum-resolved TDDFT algorithm in atomic basis for real time tracking of electronic excitation
    journal, October 2018

    • Lian, Chao; Hu, Shi-Qi; Guan, Meng-Xue
    • The Journal of Chemical Physics, Vol. 149, Issue 15
    • DOI: 10.1063/1.5036543

    Hot electron mediated enhancement in the decay rates of persistent photocurrent in gold nanoparticles embedded indium oxide films
    journal, May 2019

    • Sen, Prabal; Kar, Durgesh; Laha, Ranjit
    • Applied Physics Letters, Vol. 114, Issue 21
    • DOI: 10.1063/1.5086037

    Plasmon excitations in chemically heterogeneous nanoarrays
    journal, June 2020

    Quantum plasmonic nanoantennas
    journal, June 2017

    Coulomb effects on the photoexcited quantum dynamics of electrons in a plasmonic nanosphere
    journal, October 2018

    Theory and technology of SPASERs
    journal, January 2017

    • Premaratne, Malin; Stockman, Mark I.
    • Advances in Optics and Photonics, Vol. 9, Issue 1
    • DOI: 10.1364/aop.9.000079
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