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Ab initio phonon coupling and optical response of hot electrons in plasmonic metals

Brown, Ana M. and Sundararaman, Ravishankar and Narang, Prineha and Goddard, William A., III and Atwater, Harry A. (2016) Ab initio phonon coupling and optical response of hot electrons in plasmonic metals. Physical Review B, 94 (7). Art. No. 075120. ISSN 2469-9950. http://resolver.caltech.edu/CaltechAUTHORS:20160613-140325024

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Abstract

Ultrafast laser measurements probe the nonequilibrium dynamics of excited electrons in metals with increasing temporal resolution. Electronic structure calculations can provide a detailed microscopic understanding of hot electron dynamics, but a parameter-free description of pump-probe measurements has not yet been possible, despite intensive research, because of the phenomenological treatment of electron-phonon interactions. We present ab initio predictions of the electron-temperature dependent heat capacities and electron-phonon coupling coefficients of plasmonic metals. We find substantial differences from free-electron and semiempirical estimates, especially in noble metals above transient electron temperatures of 2000 K, because of the previously neglected strong dependence of electron-phonon matrix elements on electron energy. We also present first-principles calculations of the electron-temperature dependent dielectric response of hot electrons in plasmonic metals, including direct interband and phonon-assisted intraband transitions, facilitating complete theoretical predictions of the time-resolved optical probe signatures in ultrafast laser experiments.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1103/PhysRevB.94.075120DOIArticle
http://journals.aps.org/prb/abstract/10.1103/PhysRevB.94.075120PublisherArticle
http://arxiv.org/abs/1602.00625arXivDiscussion 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:© 2016 American Physical Society. Received 1 February 2016; revised manuscript received 26 July 2016; published 11 August 2016. 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. 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. P.N. and W.A.G. acknowledge financial support from NG NEXT for this project. P.N. is supported by a National Science Foundation Graduate Research Fellowship and by the Resnick Sustainability Institute. A.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 (Grant No. DE-SC0001293).
Group:JCAP, Resnick Sustainability Institute
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
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
WAG1175
Record Number:CaltechAUTHORS:20160613-140325024
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20160613-140325024
Official Citation:Ab initio phonon coupling and optical response of hot electrons in plasmonic metals Ana M. Brown, Ravishankar Sundararaman, Prineha Narang, William A. Goddard, III, and Harry A. Atwater Phys. Rev. B 94, 075120
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:67884
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:13 Jun 2016 21:27
Last Modified:03 Aug 2018 15:53

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