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.

Lifetime dynamics of plasmons in the few-atom limit / Chapkin, K. D.; Bursi, L.; Stec, G. J.; Lauchner, A.; Hogan, N. J.; Cui, Y.; Nordlander, P.; Halas, N. J.. - In: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA. - ISSN 0027-8424. - 115:37(2018), pp. 9134-9139. [10.1073/pnas.1805357115]

Lifetime dynamics of plasmons in the few-atom limit

Bursi L.;
2018

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.
2018
115
37
9134
9139
Lifetime dynamics of plasmons in the few-atom limit / Chapkin, K. D.; Bursi, L.; Stec, G. J.; Lauchner, A.; Hogan, N. J.; Cui, Y.; Nordlander, P.; Halas, N. J.. - In: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA. - ISSN 0027-8424. - 115:37(2018), pp. 9134-9139. [10.1073/pnas.1805357115]
Chapkin, K. D.; Bursi, L.; Stec, G. J.; Lauchner, A.; Hogan, N. J.; Cui, Y.; Nordlander, P.; Halas, N. J.
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11380/1298826
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