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Transport of hot carriers in plasmonic nanostructures

Jermyn, Adam S. and Tagliabue, Giulia and Atwater, Harry A. and Goddard, William A., III and Narang, Prineha and Sundararaman, Ravishankar (2019) Transport of hot carriers in plasmonic nanostructures. Physical Review Materials, 3 (7). Art. No. 075201. ISSN 2475-9953. doi:10.1103/PhysRevMaterials.3.075201.

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Plasmonic hot carrier devices extract excited carriers from metal nanostructures before equilibration and have the potential to surpass semiconductor light absorbers. However their efficiencies have so far remained well below theoretical limits, which necessitates quantitative prediction of carrier transport and energy loss in plasmonic structures to identify and overcome bottlenecks in carrier harvesting. Here, we present a theoretical and computational framework, nonequilibrium scattering in space and energy (NESSE), to predict the spatial evolution of carrier energy distributions that combines the best features of phase-space (Boltzmann) and particle-based (Monte Carlo) methods. Within the NESSE framework, we bridge first-principles electronic structure predictions of plasmon decay and carrier collision integrals at the atomic scale, with electromagnetic field simulations at the nano- to mesoscale. Finally, we apply NESSE to predict spatially-resolved energy distributions of photoexcited carriers that impact the surface of experimentally realizable plasmonic nanostructures at length scales ranging from tens to several hundreds of nanometers, enabling first-principles design of hot carrier devices.

Item Type:Article
Related URLs:
URLURL TypeDescription Paper
Jermyn, Adam S.0000-0001-5048-9973
Tagliabue, Giulia0000-0003-4587-728X
Atwater, Harry A.0000-0001-9435-0201
Goddard, William A., III0000-0003-0097-5716
Narang, Prineha0000-0003-3956-4594
Sundararaman, Ravishankar0000-0002-0625-4592
Alternate Title:Far-from-equilibrium transport of excited carriers in nanostructures
Additional Information:© 2019 American Physical Society. Received 6 March 2019; published 8 July 2019. This material is based upon work performed at 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. This research used resources of 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, as well as the Center for Computational Innovations at Rensselaer Polytechnic Institute. A.S.J. thanks the UK Marshall Commission and the US Goldwater Scholarship for financial support. G.T. acknowledges support from the Swiss National Science Foundation, Early Postdoctoral Mobility Fellowship No. P2EZP2-159101. P.N. acknowledges start-up funding from the Harvard John A. Paulson School of Engineering and Applied Sciences and partial support from the Harvard University Center for the Environment (HUCE). R.S. acknowledges start-up funding from the Department of Materials Science and Engineering at Rensselaer Polytechnic Institute.
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Department of Energy (DOE)DE-AC02-05CH11231
UK Marshall CommissionUNSPECIFIED
Barry M. Goldwater ScholarshipUNSPECIFIED
Swiss National Science Foundation (SNSF)P2EZP2-159101
Harvard UniversityUNSPECIFIED
Rensselaer Polytechnic InstituteUNSPECIFIED
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Issue or Number:7
Record Number:CaltechAUTHORS:20190627-130903657
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:96792
Deposited By: Tony Diaz
Deposited On:27 Jun 2019 20:33
Last Modified:16 Nov 2021 17:23

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