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Theoretical predictions for hot-carrier generation from surface plasmon decay

Author

Listed:
  • Ravishankar Sundararaman

    (Joint Center for Artificial Photosynthesis, California Institute of Technology)

  • Prineha Narang

    (Joint Center for Artificial Photosynthesis, California Institute of Technology
    Thomas J. Watson Laboratories of Applied Physics, California Institute of Technology)

  • Adam S. Jermyn

    (Joint Center for Artificial Photosynthesis, California Institute of Technology
    Mathematics and Astronomy, California Institute of Technology)

  • William A. Goddard III

    (Joint Center for Artificial Photosynthesis, California Institute of Technology
    Materials and Process Simulation Center, California Institute of Technology)

  • Harry A. Atwater

    (Joint Center for Artificial Photosynthesis, California Institute of Technology
    Thomas J. Watson Laboratories of Applied Physics, California Institute of Technology)

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.

Suggested Citation

  • Ravishankar Sundararaman & Prineha Narang & Adam S. Jermyn & William A. Goddard III & Harry A. Atwater, 2014. "Theoretical predictions for hot-carrier generation from surface plasmon decay," Nature Communications, Nature, vol. 5(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:5:y:2014:i:1:d:10.1038_ncomms6788
    DOI: 10.1038/ncomms6788
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    Cited by:

    1. Giles Allison & Amrita Kumar Sana & Yuta Ogawa & Hidemi Kato & Kosei Ueno & Hiroaki Misawa & Koki Hayashi & Hironori Suzuki, 2021. "A Fabry-Pérot cavity coupled surface plasmon photodiode for electrical biomolecular sensing," Nature Communications, Nature, vol. 12(1), pages 1-7, December.
    2. Can O. Karaman & Anton Yu. Bykov & Fatemeh Kiani & Giulia Tagliabue & Anatoly V. Zayats, 2024. "Ultrafast hot-carrier dynamics in ultrathin monocrystalline gold," Nature Communications, Nature, vol. 15(1), pages 1-8, December.

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