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. doi:10.1103/PhysRevLett.118.087401. https://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.
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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 | ||||||||||||||||
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Issue or Number: | 8 | ||||||||||||||||
DOI: | 10.1103/PhysRevLett.118.087401 | ||||||||||||||||
Record Number: | CaltechAUTHORS:20170221-134853641 | ||||||||||||||||
Persistent URL: | https://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: | 11 Nov 2021 05:27 |
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