Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 138, Issue 17, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.4802000
Keywords
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Funding
- U.S. National Science Foundation (NSF) [CHE-1012207/001]
- U.S. Department of Energy (DOE) [DE-SC0001785]
- United States-Israel Binational Science Foundation [2008124]
- ERC [22662]
- National Science Foundation's MRSEC program at the Materials Research Center of Northwestern University [DMR-1121262]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1012207] Funding Source: National Science Foundation
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [1121262] Funding Source: National Science Foundation
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We consider the transient non-equilibrium electronic distribution that is created in a metal nanoparticle upon plasmon excitation. Following light absorption, the created plasmons decohere within a few femtoseconds, producing uncorrelated electron-hole pairs. The corresponding non-thermal electronic distribution evolves in response to the photo-exciting pulse and to subsequent relaxation processes. First, on the femtosecond timescale, the electronic subsystem relaxes to a Fermi-Dirac distribution characterized by an electronic temperature. Next, within picoseconds, thermalization with the underlying lattice phonons leads to a hot particle in internal equilibrium that subsequently equilibrates with the environment. Here we focus on the early stage of this multistep relaxation process, and on the properties of the ensuing non-equilibrium electronic distribution. We consider the form of this distribution as derived from the balance between the optical absorption and the subsequent relaxation processes, and discuss its implication for (a) heating of illuminated plasmonic particles, (b) the possibility to optically induce current in junctions, and (c) the prospect for experimental observation of such light-driven transport phenomena. (C) 2013 AIP Publishing LLC.
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