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Quantifying the role of surface plasmon excitation and hot carrier transport in plasmonic devices

Tagliabue, Giulia and Jermyn, Adam S. and Sundararaman, Ravishankar and Welch, Alex J. and DuChene, Joseph S. and Pala, Ragip and Davoyan, Artur R. and Narang, Prineha and Atwater, Harry A. (2018) Quantifying the role of surface plasmon excitation and hot carrier transport in plasmonic devices. Nature Communications, 9 . Art. No. 3394. ISSN 2041-1723. PMCID PMC6107582. doi:10.1038/s41467-018-05968-x.

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Harnessing photoexcited “hot” carriers in metallic nanostructures could define a new phase of non-equilibrium optoelectronics for photodetection and photocatalysis. Surface plasmons are considered pivotal for enabling efficient operation of hot carrier devices. Clarifying the fundamental role of plasmon excitation is therefore critical for exploiting their full potential. Here, we measure the internal quantum efficiency in photoexcited gold (Au)–gallium nitride (GaN) Schottky diodes to elucidate and quantify the distinct roles of surface plasmon excitation, hot carrier transport, and carrier injection in device performance. We show that plasmon excitation does not influence the electronic processes occurring within the hot carrier device. Instead, the metal band structure and carrier transport processes dictate the observed hot carrier photocurrent distribution. The excellent agreement with parameter-free calculations indicates that photoexcited electrons generated in ultra-thin Au nanostructures impinge ballistically on the Au–GaN interface, suggesting the possibility for hot carrier collection without substantial energy losses via thermalization.

Item Type:Article
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URLURL TypeDescription CentralArticle
Tagliabue, Giulia0000-0003-4587-728X
Jermyn, Adam S.0000-0001-5048-9973
Sundararaman, Ravishankar0000-0002-0625-4592
Welch, Alex J.0000-0003-2132-9617
DuChene, Joseph S.0000-0002-7145-323X
Davoyan, Artur R.0000-0002-4662-1158
Narang, Prineha0000-0003-3956-4594
Atwater, Harry A.0000-0001-9435-0201
Additional Information:© The Author(s) 2018. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit Received 08 December 2017; Accepted 11 July 2018; Published 23 August 2018. This material is based on 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 No. DE-SC0004993. R.S., A.S.J., and P.N. acknowledge support from NG NEXT at Northrop Grumman Corporation. Calculations in this work used the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02–05CH11231. A.D. and H.A.A. acknowledge support from the Air Force Office of Scientific Research under grant FA9550-16-1-0019. G.T. acknowledges support from the Swiss National Science Foundation through the Early Postdoc Mobility Fellowship, grant no. P2EZP2_159101. P.N. acknowledges support from the Harvard University Center for the Environment (HUCE). A.S.J. thanks the UK Marshall Commission and the US Goldwater Scholarship for financial support. A.J.W. acknowledges support from the National Science Foundation (NSF) under Award No. 2016217021. Author Contributions: G.T. performed experiments, numerical simulations, and IQE calculations of devices. A.S.J., R.S., and P.N. performed ab initio hot carrier generation and transport calculations. A.J.W., J.S.D., R.P., and A.R.D. contributed to experiments and data analysis. All authors contributed to interpretation of the results. G.T., J.S.D., A.R.D., and H.A.A. wrote the manuscript with contributions from all authors. H.A.A. supervised all aspects of the project. The authors declare no competing interests. Code availability: First principle methodologies available through open-source software, JDFTx, and post-processing scripts available from authors upon request. Data availability: All relevant data are available from the authors upon request.
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Northrop Grumman CorporationUNSPECIFIED
Department of Energy (DOE)DE-AC02-05CH11231
Air Force Office of Scientific Research (AFOSR)FA9550-16-1-0019
Swiss National Science Foundation (SNSF)P2EZP2_159101
Harvard UniversityUNSPECIFIED
UK Marshall CommissionUNSPECIFIED
Barry M. Goldwater ScholarshipUNSPECIFIED
PubMed Central ID:PMC6107582
Record Number:CaltechAUTHORS:20180823-080749691
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:89077
Deposited By: Tony Diaz
Deposited On:23 Aug 2018 16:11
Last Modified:07 Mar 2022 19:06

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