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The improvement of emitters
with plasmonic
nanostructures is of large importance for applications in lighting and quantum optics. Selective modification of only radiative decay channels is
critical for light-emitting devices that benefit only from radiative
enhancement. We have
investigated a novel class of optical antenna designs that are
optimized specifically with respect to this radiative outcoupling of
plasmons into far-field light.
We have studied the resonant enhancement of the fluorescence emission from dye molecules close to single optical nanoantennas. Dimer
antenna structures were fabricated consisting of two interacting
gold nanorods with varying lengths and interparticle separation. Two-dimensional confocal
fluorescence lifetime scans are used to visualize the spontaneous emission
enhancement of the molecular fluorescence around the antenna
clusters. At every position, a fluorescence decay curve is measured as shown in Figure 1.

Figure 1 Normalized fluorescence decay measured at
a resonant nanoantenna (diamonds, black) and away from the
nanoantenna (open dots, red), with exponential decay fits (lines,
black). Inset: SEM image of the resonant gold nanoantenna,
consisting of two 90x60x20 nm3 gold nanorods with an
antenna gap of 20 nm.
By fabricating arrays of nanoantennas with controlled length and interparticle gap distance, we have measured the radiative rate enhancement to the antenna parameters, as shown in Figure 2. The radiative rate shows a maximum related to the spectral resonance position of the longitudinal plasmon mode at the fluorescence emission wavelength of 730 nm. For antennas with a narrow gap, an additional increase of the decay rate is observed compared to uncoupled antennas.
Figure 2 (left) Antenna array containing clusters of 4 antennas with different design parameters. (right) Enhancement of the fluorescence decay rate of the fast decay component around the antenna clusters.
A clear effect of antenna coupling on
the spontaneous emission enhancement was found and explained, using
a theoretical model, by the strong local field enhancement in the
antenna gap (see Figure 3). We conclude that, although enhancement is limited by
metal losses, these can be small enough to result in considerable
quantum efficiency improvement.

Figure 3 Radiative and nonradiative decay rates
gR, gNR for a dipole emitter are shown versus antenna arm
length L, for the strongly coupled antenna arms.
(Top graphs) Calculated near-field intensities around two resonant
antennas with spots indicating the location of the emitter in the calculations
(scale bar denotes 100 nm).
By designing
metal antennas with optimized arm length and gap width, the
spontaneous emission of a fluorescent dye was enhanced by more than
a factor 5, while the quantum efficiency was improved from 40% to
53%. This holds promise for enhanced light extraction from luminescent devices and for quantum optics using single emitters.
Reference:
O. L. Muskens, V. Giannini, J. A. Sánchez Gil, J. Gómez Rivas, Strong enhancement of the radiative decay rate of emitters by single plasmonic nanoantennas,
Nano Lett. 7(9), 2871:75 (2007)
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