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Experimental and Ab Initio Ultrafast Carrier Dynamics in Plasmonic Nanoparticles

Brown, Ana M. and Sundararaman, Ravishankar and Narang, Prineha and Schwartzberg, Adam M. and Goddard, William A., III and Atwater, Harry A. (2017) Experimental and Ab Initio Ultrafast Carrier Dynamics in Plasmonic Nanoparticles. Physical Review Letters, 118 (8). Art. No. 087401. ISSN 0031-9007. http://resolver.caltech.edu/CaltechAUTHORS:20170221-134853641

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Abstract

Ultrafast pump-probe measurements of plasmonic nanostructures probe the nonequilibrium behavior of excited carriers, which involves several competing effects obscured in typical empirical analyses. Here we present pump-probe measurements of plasmonic nanoparticles along with a complete theoretical description based on first-principles calculations of carrier dynamics and optical response, free of any fitting parameters. We account for detailed electronic-structure effects in the density of states, excited carrier distributions, electron-phonon coupling, and dielectric functions that allow us to avoid effective electron temperature approximations. Using this calculation method, we obtain excellent quantitative agreement with spectral and temporal features in transient-absorption measurements. In both our experiments and calculations, we identify the two major contributions of the initial response with distinct signatures: short-lived highly nonthermal excited carriers and longer-lived thermalizing carriers.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1103/PhysRevLett.118.087401DOIArticle
http://journals.aps.org/prl/abstract/10.1103/PhysRevLett.118.087401PublisherArticle
https://arxiv.org/abs/1608.03309arXivDiscussion Paper
ORCID:
AuthorORCID
Sundararaman, Ravishankar0000-0002-0625-4592
Narang, Prineha0000-0003-3956-4594
Goddard, William A., III0000-0003-0097-5716
Atwater, Harry A.0000-0001-9435-0201
Additional Information:© 2017 American Physical Society. (Received 11 August 2016; published 21 February 2017) This material is based upon 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. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. The authors 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. P. N. is supported by a National Science Foundation Graduate Research Fellowship and by the Resnick Sustainability Institute. A. M. B. is supported by a National Science Foundation Graduate Research Fellowship, a Link Foundation Energy Fellowship, and the DOE “Light-Material Interactions in Energy Conversion” Energy Frontier Research Center (DE-SC0001293).
Group:JCAP, Resnick Sustainability Institute
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Department of Energy (DOE)DE-AC02-05CH11231
Northrop Grumman CorporationUNSPECIFIED
Department of Energy (DOE)DE-AC02-05CH11231
NSF Graduate Research FellowshipUNSPECIFIED
Resnick Sustainability InstituteUNSPECIFIED
Link FoundationUNSPECIFIED
Department of Energy (DOE)DE-SC0001293
Other Numbering System:
Other Numbering System NameOther Numbering System ID
WAG1257
Record Number:CaltechAUTHORS:20170221-134853641
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20170221-134853641
Official Citation:Experimental and Ab Initio Ultrafast Carrier Dynamics in Plasmonic Nanoparticles Ana M. Brown, Ravishankar Sundararaman, Prineha Narang, Adam M. Schwartzberg, William A. Goddard, III, and Harry A. Atwater Phys. Rev. Lett. 118, 087401
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:74434
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:21 Feb 2017 22:13
Last Modified:26 Sep 2018 21:05

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