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Proc Natl Acad Sci U S A. 2018 Sep 11;115(37):9134-9139. doi: 10.1073/pnas.1805357115. Epub 2018 Aug 27.

Lifetime dynamics of plasmons in the few-atom limit.

Chapkin KD1,2, Bursi L2,3, Stec GJ2,4, Lauchner A1,2, Hogan NJ1,2, Cui Y1,2, Nordlander P1,2,3,5, Halas NJ6,2,3,4.

Author information

1
Department of Electrical and Computer Engineering, Rice University, Houston, TX 77005.
2
Laboratory for Nanophotonics, Rice University, Houston, TX 77005.
3
Department of Physics and Astronomy, Rice University, Houston, TX 77005.
4
Department of Chemistry, Rice University, Houston, TX 77005.
5
Department of Material Science and Nanoengineering, Rice University, Houston, TX 77005.
6
Department of Electrical and Computer Engineering, Rice University, Houston, TX 77005; halas@rice.edu.

Abstract

Polycyclic aromatic hydrocarbon (PAH) molecules are essentially graphene in the subnanometer limit, typically consisting of 50 or fewer atoms. With the addition or removal of a single electron, these molecules can support molecular plasmon (collective) resonances in the visible region of the spectrum. Here, we probe the plasmon dynamics in these quantum systems by measuring the excited-state lifetime of three negatively charged PAH molecules: anthanthrene, benzo[ghi]perylene, and perylene. In contrast to the molecules in their neutral state, these three systems exhibit far more rapid decay dynamics due to the deexcitation of multiple electron-hole pairs through molecular plasmon "dephasing" and vibrational relaxation. This study provides a look into the distinction between collective and single-electron excitation dynamics in the purely quantum limit and introduces a conceptual framework with which to visualize molecular plasmon decay.

KEYWORDS:

excited-state dynamics; lifetime; molecular plasmons; plasmonicity; plasmonics

PMID:
30150399
PMCID:
PMC6140484
[Available on 2019-03-11]
DOI:
10.1073/pnas.1805357115

Conflict of interest statement

The authors declare no conflict of interest.

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