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Cubic Nonlinearity Driven Up-Conversion in High-Field Plasmonic Hot Carrier Systems

Narang, Prineha and Sundararaman, Ravishankar and Jermyn, Adam S. and Goddard, William A., III and Atwater, Harry A. (2016) Cubic Nonlinearity Driven Up-Conversion in High-Field Plasmonic Hot Carrier Systems. Journal of Physical Chemistry C, 120 (37). pp. 21056-21062. ISSN 1932-7447. doi:10.1021/acs.jpcc.6b03463.

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Surface plasmon resonances confine electromagnetic fields to the nanoscale, producing high field strengths suitable for exploiting nonlinear optical properties. We examine the prospect of detecting and utilizing one such property in plasmonic metals: the imaginary part of the cubic susceptibility, which corresponds to two plasmons decaying together to produce high energy carriers. Here we present ab initio predictions of the rates and carrier distributions generated by direct interband and phonon-assisted intraband transitions in one and two-plasmon decay. We propose detection of the higher energy carriers generated from two-plasmon decays that are inaccessible in one-plasmon decay as a viable signature of these processes in ultrafast experiments.

Item Type:Article
Related URLs:
URLURL TypeDescription
Narang, Prineha0000-0003-3956-4594
Sundararaman, Ravishankar0000-0002-0625-4592
Jermyn, Adam S.0000-0001-5048-9973
Goddard, William A., III0000-0003-0097-5716
Atwater, Harry A.0000-0001-9435-0201
Additional Information:© 2016 American Chemical Society. Received: April 5, 2016; Revised: June 20, 2016; Publication Date (Web): June 20, 2016. Special Issue: Richard P. Van Duyne Festschrift. 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 Number DE-SC0004993. P.N. is supported by a National Science Foundation Graduate Research Fellowship and by the Resnick Sustainability Institute. A.S.J. acknowledges support from the Barry M. Goldwater Scholarship. 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. The authors declare no competing financial interest.
Group:JCAP, Resnick Sustainability Institute
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
NSF Graduate Research FellowshipUNSPECIFIED
Resnick Sustainability InstituteUNSPECIFIED
Barry M. Goldwater ScholarshipUNSPECIFIED
Northrop Grumman CorporationUNSPECIFIED
Department of Energy (DOE)DE-AC02-05CH11231
Issue or Number:37
Record Number:CaltechAUTHORS:20160718-092335284
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Official Citation:Cubic Nonlinearity Driven Up-Conversion in High-Field Plasmonic Hot Carrier Systems Prineha Narang, Ravishankar Sundararaman, Adam S. Jermyn, William A. Goddard, III, and Harry A. Atwater The Journal of Physical Chemistry C 2016 120 (37), 21056-21062 DOI: 10.1021/acs.jpcc.6b03463
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:69086
Deposited By: Tony Diaz
Deposited On:27 Jul 2016 16:16
Last Modified:11 Nov 2021 04:09

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