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Emission and excitation contributions to enhanced single molecule fluorescence by gold nanometric apertures

Jérôme Wenger, Davy Gérard, José Dintinger, Oussama Mahboub, Nicolas Bonod, Evgeny Popov, Thomas W. Ebbesen, and Hervé Rigneault

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Abstract

We detail the role of single nanometric apertures milled in a gold film to enhance the fluorescence emission of Alexa Fluor 647 molecules. Combining fluorescence correlation spectroscopy and lifetime measurements, we determine the respective contributions of excitation and emission in the observed enhanced fluorescence. We characterize a broad range of nanoaperture diameters from 80 to 310 nm, and highlight the link between the fluorescence enhancement and the local photonic density of states. These results are of great interest to increase the effectiveness of fluorescence-based single molecule detection and to understand the interaction between a quantum emitter and a nanometric metal structure.

©2008 Optical Society of America

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Figures (6)
Fig. 1.
Fig. 1. (a) Schematic view of the experimental setup combining FCS and TCSPC. (b) Nanoaperture configuration. (c) Notations used to describe the molecular transition rates.

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Fig. 2.
Fig. 2. (a) Typical fluorescence autocorrelations in a 120 nm aperture (crosses, raw data) and numerical fits according to Eq. (7) (lines). (b) Snapshot of the raw fluorescence signal corresponding to (a).

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Fig. 3.
Fig. 3. Fluorescence rates per molecule CRM versus excitation power in open solution and in single nanoapertures. Circles are experimental data, lines are numerical fits using Eq. (2).

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Fig. 4.
Fig. 4. (a) Fluorescence enhancement ηF derived from Fig. 3. (b) Fluorescence enhancement below saturation ηF,low (empty markers) and at saturation ηF,sat (filled markers) deduced from the numerical fits in Fig. 3 according to Eqs. (2), (4) and (6).

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Fig. 5.
Fig. 5. (a) Normalized fluorescence decay traces measured in open solution (black dots) and in single nanoapertures. Dots are experimental data, lines are numerical fits following the procedure described in Sec. 3.3. The shorter decay trace (grey) is the overall instrument response function (IRF). (b) Fluorescence lifetime reduction versus the aperture diameter (as compared to open solution), deduced from the numerical fits in (a) using Eq. (8).

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Fig. 6.
Fig. 6. Physical contributions to nanoaperture enhanced fluorescence, plotted versus the aperture diameter and normalized to the open solution case. (a) Fluorescence enhancement below saturation ηF,low , (b) Emission rate enhancement ηkem , (c) Lifetime reduction ηktot , (d) Excitation enhancement ηIe , (e) Ratio ηkem /ηktot , (f) Propagation constant γ of the fundamental mode inside the aperture (solid line: real part, dashed line: imaginary part).

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Equations (8)

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CRM = κ ϕ σ I e 1 + I e I s
CRM = k em k tot σ I e 1 + I e I s
CRM low = k em k tot σ I e ( I e ≪ I s )
η F , low = CRM aper CRM sol = η k em η k tot η I e ( I e ≪ I s )
CRM sat = k em k tot σ I s = k em 1 + k isc k d ( I e ≫ I s )
η F , sat = η k em ( I e ≫ I s )
g ( 2 ) ( τ ) = 1 + 1 N ( 1 − 〈 B 〉 〈 F 〉 ) 2 [ 1 + n T exp ⁡ ( − τ τ b T ) ] 1 ( 1 + τ τ d ) 1 + s 2 τ τ d
O ( t ) ∝ ( A 1 + A 2 ) exp ( − k tot t ) − A 1 exp ( − k 1 t ) − A 2 exp ( − k 2 t )
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