Hot-Carrier Generation from Plasmon Decay in Energy Conversion

Sundararaman, R., Narang, P., Jermyn, A. S., Goddard, W. A. & Atwater, H. A. Theoretical predictions for hot-carrier generation from surface plasmo decay. Nature Communications 5, 8, DOI: 10.1038/ncomms6788 (2014).


Scientific Achievement

First theoretical study combining plasmon modes with density functional theory to predict initial energy distribution of hot carriers in real metals.

Significance & impact

Understanding the initial energy distribution of plasmon-generated hot carriers guides the selection of optimal materials for plasmonic photocatalysts and efficient photoabsorbers.

  The images in Sundararaman, R., Narang, P., Jermyn, A. S., Goddard, W. A. & Atwater, H. A. Theoretical predictions for hot-carrier generation from surface plasmon decay. Nature Communications 5, 8, DOI: 10.1038/ncomms6788 (2014) are licensed under a Creative Commons Attribution 4.0 International License (http://creativecommons.org/licenses/by/4.0/).

 

The images in Sundararaman, R., Narang, P., Jermyn, A. S., Goddard, W. A. & Atwater, H. A. Theoretical predictions for hot-carrier generation from surface plasmon decay. Nature Communications 5, 8, DOI: 10.1038/ncomms6788 (2014) are licensed under a Creative Commons Attribution 4.0 International License (http://creativecommons.org/licenses/by/4.0/).

Top:  Plasmonic hot-carrier generation and injection; bottom left:  band structure and allowed transitions for copper; bottom right:  energy distribution of hot electrons and holes.

Research Details

  • Relativistic DFT+U ab initiocalculation of band structures is in excellent agreement with photoemission experiments.
  • Hot-carrier distribution is sensitive to the electronic band structure of the plasmonic metal.
  • Generated-carrier distribution also depends on the electromagnetic modes excited in the plasmonic structure.

Contact:  haa@caltech.edu