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Title: Theoretical predictions for hot-carrier generation from surface plasmon decay

Abstract

Decay of surface plasmons to hot carriers finds a wide variety of applications in energy conversion, photocatalysis and photodetection. However, a detailed theoretical description of plasmonic hot-carrier generation in real materials has remained incomplete. Here we report predictions for the prompt distributions of excited 'hot' electrons and holes generated by plasmon decay, before inelastic relaxation, using a quantized plasmon model with detailed electronic structure. We find that carrier energy distributions are sensitive to the electronic band structure of the metal: gold and copper produce holes hotter than electrons by 1-2 eV, while silver and aluminium distribute energies more equitably between electrons and holes. Momentum-direction distributions for hot carriers are anisotropic, dominated by the plasmon polarization for aluminium and by the crystal orientation for noble metals. We show that in thin metallic films intraband transitions can alter the carrier distributions, producing hotter electrons in gold, but interband transitions remain dominant.

Authors:
 [1];  [2];  [3];  [4];  [2]
  1. California Inst. of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP)
  2. California Inst. of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP) and Thomas J. Watson Laboratories of Applied Physics
  3. California Inst. of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP) and Division of Physics, Mathematics and Astronomy
  4. California Inst. of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP) and Materials and Process Simulation Center
Publication Date:
Research Org.:
California Inst. of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1457531
Grant/Contract Number:  
SC0004993
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 5; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Sundararaman, Ravishankar, Narang, Prineha, Jermyn, Adam S., Goddard III, William A., and Atwater, Harry A. Theoretical predictions for hot-carrier generation from surface plasmon decay. United States: N. p., 2014. Web. doi:10.1038/ncomms6788.
Sundararaman, Ravishankar, Narang, Prineha, Jermyn, Adam S., Goddard III, William A., & Atwater, Harry A. Theoretical predictions for hot-carrier generation from surface plasmon decay. United States. doi:10.1038/ncomms6788.
Sundararaman, Ravishankar, Narang, Prineha, Jermyn, Adam S., Goddard III, William A., and Atwater, Harry A. Tue . "Theoretical predictions for hot-carrier generation from surface plasmon decay". United States. doi:10.1038/ncomms6788. https://www.osti.gov/servlets/purl/1457531.
@article{osti_1457531,
title = {Theoretical predictions for hot-carrier generation from surface plasmon decay},
author = {Sundararaman, Ravishankar and Narang, Prineha and Jermyn, Adam S. and Goddard III, William A. and Atwater, Harry A.},
abstractNote = {Decay of surface plasmons to hot carriers finds a wide variety of applications in energy conversion, photocatalysis and photodetection. However, a detailed theoretical description of plasmonic hot-carrier generation in real materials has remained incomplete. Here we report predictions for the prompt distributions of excited 'hot' electrons and holes generated by plasmon decay, before inelastic relaxation, using a quantized plasmon model with detailed electronic structure. We find that carrier energy distributions are sensitive to the electronic band structure of the metal: gold and copper produce holes hotter than electrons by 1-2 eV, while silver and aluminium distribute energies more equitably between electrons and holes. Momentum-direction distributions for hot carriers are anisotropic, dominated by the plasmon polarization for aluminium and by the crystal orientation for noble metals. We show that in thin metallic films intraband transitions can alter the carrier distributions, producing hotter electrons in gold, but interband transitions remain dominant.},
doi = {10.1038/ncomms6788},
journal = {Nature Communications},
number = 1,
volume = 5,
place = {United States},
year = {Tue Dec 16 00:00:00 EST 2014},
month = {Tue Dec 16 00:00:00 EST 2014}
}

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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

Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998

  • Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.
  • Physical Review B, Vol. 57, Issue 3, p. 1505-1509
  • DOI: 10.1103/PhysRevB.57.1505

Quantum mechanical study of the coupling of plasmon excitations to atomic-scale electron transport
journal, February 2011

  • Song, Peng; Nordlander, Peter; Gao, Shiwu
  • The Journal of Chemical Physics, Vol. 134, Issue 7, Article No. 074701
  • DOI: 10.1063/1.3554420

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