Author
Listed:
- Marco Bernardi
(University of California at Berkeley, 366 LeConte Hall #7300, Berkeley, California 94720, USA
Lawrence Berkeley National Laboratory)
- Jamal Mustafa
(University of California at Berkeley, 366 LeConte Hall #7300, Berkeley, California 94720, USA
Lawrence Berkeley National Laboratory)
- Jeffrey B. Neaton
(University of California at Berkeley, 366 LeConte Hall #7300, Berkeley, California 94720, USA
Lawrence Berkeley National Laboratory
Molecular Foundry, Lawrence Berkeley National Laboratory
Kavli Institute for Energy Nanosciences at Berkeley)
- Steven G. Louie
(University of California at Berkeley, 366 LeConte Hall #7300, Berkeley, California 94720, USA
Lawrence Berkeley National Laboratory)
Abstract
Hot carriers (HC) generated by surface plasmon polaritons (SPPs) in noble metals are promising for application in optoelectronics, plasmonics and renewable energy. However, existing models fail to explain key quantitative details of SPP-to-HC conversion experiments. Here we develop a quantum mechanical framework and apply first-principles calculations to study the energy distribution and scattering processes of HCs generated by SPPs in Au and Ag. We find that the relative positions of the s and d bands of noble metals regulate the energy distribution and mean free path of the HCs, and that the electron–phonon interaction controls HC energy loss and transport. Our results prescribe optimal conditions for HC generation and extraction, and invalidate previously employed free-electron-like models. Our work combines density functional theory, GW and electron–phonon calculations to provide microscopic insight into HC generation and ultrafast dynamics in noble metals.
Suggested Citation
Marco Bernardi & Jamal Mustafa & Jeffrey B. Neaton & Steven G. Louie, 2015.
"Theory and computation of hot carriers generated by surface plasmon polaritons in noble metals,"
Nature Communications, Nature, vol. 6(1), pages 1-9, November.
Handle:
RePEc:nat:natcom:v:6:y:2015:i:1:d:10.1038_ncomms8044
DOI: 10.1038/ncomms8044
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