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Theoretical predictions for hot-carrier generation from surface plasmon decay

Sundararaman, Ravishankar and Narang, Prineha and Jermyn, Adam S. and Goddard, William A., III and Atwater, Harry A. (2014) Theoretical predictions for hot-carrier generation from surface plasmon decay. Nature Communications, 5 . Art. No. 5788. ISSN 2041-1723. PMCID PMC4284641. doi:10.1038/ncomms6788.

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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.

Item Type:Article
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URLURL TypeDescription CentralArticle
Sundararaman, Ravishankar0000-0002-0625-4592
Narang, Prineha0000-0003-3956-4594
Jermyn, Adam S.0000-0001-5048-9973
Goddard, William A., III0000-0003-0097-5716
Atwater, Harry A.0000-0001-9435-0201
Additional Information:© 2014 Macmillan Publishers Limited. This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit Received 03 September 2014. Accepted 07 November 2014. Published 16 December 2014. We thank Marco Bernardi for detailed feedback on and suggestions towards improving this manuscript; Tonatiuh Rangel, Jamal Mustafa and Marco Bernardi for private communications of noble metal GW band structures; and Yuan Ping for useful discussions. This material is based on the work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993. P.N. is supported by a National Science Foundation Graduate Research Fellowship and by the Resnick Sustainability Institute.
Group:Resnick Sustainability Institute, JCAP
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Department of Energy (DOE)DE-SC0004993
Resnick Sustainability InstituteUNSPECIFIED
NSF Graduate Research FellowshipUNSPECIFIED
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PubMed Central ID:PMC4284641
Record Number:CaltechAUTHORS:20141219-150047470
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Official Citation:Sundararaman, R. et al. Theoretical predictions for hot-carrier generation from surface plasmon decay. Nat. Commun. 5:5788 doi: 10.1038/ncomms6788 (2014).
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:53056
Deposited By: Heidi Rusina
Deposited On:19 Dec 2014 23:17
Last Modified:10 Nov 2021 19:47

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