posted on 2017-05-03, 00:00authored byLiang-Yan Hsu, Wendu Ding, George C. Schatz
In
this study, we overview resonance energy transfer between molecules
in the presence of plasmonic structures and derive an explicit Förster-type
expression for the rate of plasmon-coupled resonance energy transfer
(PC-RET). The proposed theory is general for energy transfer in the
presence of materials with any space-dependent, frequency-dependent,
or complex dielectric functions. Furthermore, the theory allows us
to develop the concept of a generalized spectral overlap (GSO) <i>J̃</i> (the integral of the molecular absorption coefficient,
normalized emission spectrum, and the plasmon coupling factor) for
understanding the wavelength dependence of PC-RET and to estimate
the rate of PC-RET <i>W</i><sub>ET</sub>. Indeed, <i>W</i><sub>ET</sub> = (8.785 × 10<sup>–25</sup> mol)
ϕ<sub>D</sub>τ<sub>D</sub><sup>–1</sup><i>J̃</i>, where ϕ<sub>D</sub> is donor fluorescence quantum yield and τ<sub>D</sub> is the emission lifetime. Simulations of the GSO for PC-RET show
that the most important spectral region for PC-RET is not necessarily
near the maximum overlap of donor emission and acceptor absorption.
Instead a significant plasmonic contribution can involve a different
spectral region from the extinction maximum of the plasmonic structure.
This study opens a promising direction for exploring exciton transport
in plasmonic nanostructures, with possible applications in spectroscopy,
photonics, biosensing, and energy devices.