Using surface plasmonics to turn on fullerene's dark excitons

Despoja, Vito and Mowbray, D. J. (2014) Using surface plasmonics to turn on fullerene's dark excitons. Physical Review B, 89 (19). pp. 195433-10. ISSN 1098-0121

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Using our recently proposed Bethe-Salpeter G_0W_0 formulation, we explore the optical absorption spectra of fullerene (C_60) near coinage metal surfaces (Cu, Ag, and Au). We pay special attention to how the surface plasmon ω_S influences the optical activity of fullerene. We find that the lower-energy fullerene excitons at 3.77 and 4.8 eV only weakly interact with the surface plasmon. However, we find that the surface plasmon strongly interacts with the most intense fullerene π exciton, i.e., the dipolar mode at ℏω+≈6.5 eV, and the quadrupolar mode at ℏω−≈6.8 eV. When fullerene is close to a copper surface (z_0≈5.3 Å), the dipolar mode ω_+ and “localized” surface plasmons in the molecule/surface interface hybridize to form two coupled modes which both absorb light. As a result, the molecule gains an additional optically active mode. Moreover, in resonance, when ω_S≈ω_±, the strong interaction with the surface plasmon destroys the ω− quadrupolar character and it becomes an optically active mode. In this case, the molecule gains two additional very intense optically active modes. Further, we find that this resonance condition, ω_S≈ω_±, is satisfied by silver and gold metal surfaces.

Item Type: Article
Date: May 2014
Subjects: NATURAL SCIENCES > Physics
Additional Information: Copyright (2014) by the American Physical Society.
Divisions: Faculty of Science > Department of Physics
Publisher: American Physical Society
Depositing User: Gordana Stubičan Ladešić
Date Deposited: 01 Jul 2014 14:09
Last Modified: 01 Jul 2014 14:09

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