Abstract

Fluorescence Correlation Spectroscopy is used to investigate fluorescent molecules in solution diffusing in subwavelength rectangular apertures milled in Aluminium films. This rectangular shape allows to switch between a propagating and an evanescent excitation field within the aperture, leading to a significant tunability of the observation volume. Due to the vicinity of the metal surface, the fluorophore�??s molecular lifetime inside the aperture appears to be dramatically reduced whatever the excitation field is set to. However, for a properly tailored evanescent excitation field within the nanoaperture, the detected fluorescence rate per molecule is significantly enhanced as compared to open solution. This suggests that the observed molecular fluorescence enhancement is mainly due to the excitation near field within the subwavelength aperture.

© 2005 Optical Society of America

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Appl. Opt. (1)

Appl. Phys. Lett. (2)

L. Yin, V. K. Vlasko-Vlasov, A. Rydh, et al., �??Surface plasmons at single nanoholes in Au films,�?? Appl. Phys. Lett. 85, 467-469 (2004).
[CrossRef]

H.F. Hamann, A. Gallagher and D.J. Nesbitt, �??Near-field fluorescence imaging by localized field enhancement near a sharp probe tip,�?? Appl. Phys. Lett. 76, 1953-1957 (2000).
[CrossRef]

Biophys. J. (1)

K.T. Samiee, M. Foquet, L. Guo, E.C. Cox and H.G. Craighead, �??λ repressor oligomerization kinetics at high concentrations using fluorescence correlation spectroscopy in zero-mode waveguides,�?? Biophys. J. 88, 2145-2153 (2005).
[CrossRef]

Biopolymers (1)

E. Elson and D. Magde, �??Fluorescence correlation spectroscopy. II. An experimental realization,�?? Biopolymers 13, 29-61 (1974).
[CrossRef]

Chem. Phys. (1)

K. Kneipp, H. Kneipp, I. Itzkan, R.R. Dasari and M.S. Feld, �??Surface-enhanced non-linear Raman scattering at the single-molecule level,�?? Chem. Phys. 247, 155-162 (1999).
[CrossRef]

J Microsc (2)

N. Hayasawa, Y. Inouye and S. Kawata, �??Evanescent field excitation and measurement of dye fluorescence in a metallic probe near-field scanning optical microscope,�?? J Microsc 194, 472-476 (1999).
[CrossRef]

J. Azoulay, A. Débarre, A. Richard and P. Tchénio, �??Field enhancement and apertureless near-field optical spectroscopy of single molecules,�?? J Microsc 194, 486-490 (1999).
[CrossRef]

Nature (2)

B. Knoll and F. Keilmann, �??Near-field probing of vibrational absorption for chemical microscopy,�?? Nature 399, 134-136 (1999).
[CrossRef]

T.W. Ebbesen, H. J. Lezec, H. F. Ghaemi, et al., �??Extraordinary optical transmission through subwavelength hole arrays,�?? Nature 391, 667-669 (1998).
[CrossRef]

Opt. Commun. (1)

A. Degiron, H. J. Lezec, N. Yamamoto, et al., �??Optical transmission properties of a single subwavelength aperture in a real metal,�?? Opt. Commun. 239, 61-66 (2004).
[CrossRef]

Opt. Express (1)

Phys. Rev. (1)

E. M. Purcell, �??Spontaneous emission probabilities at radio frequencies�??, Phys. Rev. 69, 681 (1946).

Phys. Rev. Lett. (8)

H. Gersen, M. F. Garcia-Parajo, L. Novotny, et al., �??Influencing the Angular Emission of a Single Molecule,�?? Phys. Rev. Lett. 85, 5312-5315 (2000).
[CrossRef]

D. Magde, E. Elson and W.W. Webb, �??Thermodynamic Fluctuations in a Reacting System Measurement by Fluorescence Correlation Spectroscopy,�?? Phys. Rev. Lett. 29, 705-708 (1972).
[CrossRef]

R.X. Brian, R.C. Dunn and X.S. Xie, �??Single Molecule Emission Characteristics in Near-Field Microscopy,�?? Phys. Rev. Lett. 75, 4772-4775 (1995).
[CrossRef]

H. Rigneault, J. Capoulade, J. Dintinger, J. Wenger, N. Bonod, E. Popov, T. W. Ebbesen, and P.-F. Lenne, �??Enhancement of single-molecule fluorescence detection in subwavelength apertures,�?? accepted for publication in Phys. Rev. Lett. (2005).

H. Yokota, K. Saito and T. Yanagida, �??Single Molecule Imaging of Fluorescently Labeled Proteins on Metal by Surface Plasmons in Aqueous Solution,�?? Phys. Rev. Lett. 80, 4606-4609 (1998).
[CrossRef]

F.D. Stefani, K. Vasilev, N. Bocchio, N. Stoyanova and M. Kreiter, �??Surface-Plasmon-Mediated Single-Molecule Fluorescence Through a Thin Metallic Film,�?? Phys. Rev. Lett. 94, 023005-1-4 (2005).
[CrossRef]

T. Ichimura, N. Hayasawa, M. Hashimoto, Y. Inouye and S. Kawata, �??Tip-Enhanced Coherent Anti-Stokes Raman Scattering for Vibrational Nanoimaging,�?? Phys. Rev. Lett. 92, 220801-220804 (2004).
[CrossRef]

E.J. Sánchez, L. Novotny and X.S. Xie, �??Near-Field Fluorescence Microscopy Based on Two-Photon Excitation with Metal Tips,�?? Phys. Rev. Lett. 82, 4014-4017 (1999).
[CrossRef]

Proc SPIE (1)

Y. Inouye, N. Hayasawa, K. Hayashi, Z. Sekkat and S. Kawata, �??Near-field scanning optical microscope using a metallized cantilever tip for nanospectroscopy,�?? Proc SPIE Int. Soc. Eng. 3791, 40-48 (1999).

Science (4)

M.J. Levene, J. Korlach, S.W. Turner, M. Foquet, H.G. Craighead and W.W. Webb, �??Zero-mode waveguides for single-molecule analysis at high concentrations,�?? Science 299, 682-686 (2003).
[CrossRef]

H. J. Lezec, A. Degiron, E. Devaux, et al., �??Beaming light from a subwavelength aperture,�?? Science 297, 820-822 (2002).
[CrossRef]

S. Nie and S.R. Emory, �??Probing single molecule and single nanoparticles by surface enhanced Raman scattering,�?? Science 275, 1102-1106 (1997).
[CrossRef]

W.P. Ambrose, P.M. Goodwin, J.C. Martin et al., �??Alterations of Single Molecule Fluorescence Lifetimes in Near-Field Optical Microscopy,�?? Science 265, 364-366 (1994).
[CrossRef]

Other (2)

Single-Molecule Detection in Solution - Methods and Applications, edited by C. Zander, J. Enderlein and R.A. Keller (VCH-Wiley, Berlin/New York, 2002).

Near-Field Optics and Surface Plasmon Polaritons, edited by S. Kawata (Springer, Berlin, 2001).

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