Abstract

Fluorescence spectroscopy is widely used to probe the electromagnetic intensity amplification on optical antennas, yet measuring the excitation intensity amplification is a challenge, as the detected fluorescence signal is an intricate combination of excitation and emission. Here, we describe a novel approach to quantify the electromagnetic amplification in aperture antennas by taking advantage of the intrinsic non linear properties of the fluorescence process. Experimental measurements of the fundamental f and second harmonic 2f amplitudes of the fluorescence signal upon excitation modulation are used to quantify the electromagnetic intensity amplification with plasmonic aperture antennas.

© 2012 OSA

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  1. L. Novotny and N. van Hulst, “Antennas for light,” Nat. Photonics5, 83–90 (2011).
    [CrossRef]
  2. J. A. Schuller, E. S. Barnard, W. S. Cai, Y. C. Jun, J. S. White, and M. L. Brongersma, “Plasmonics for extreme light concentration and manipulation,” Nature Mater.9, 193–204 (2010).
    [CrossRef]
  3. A. Kinkhabwala, Z. F. Yu, S. H. Fan, Y. Avlasevich, K. Mullen, and W. E. Moerner, “Large single-molecule fluorescence enhancements produced by a bowtie nanoantenna,” Nat. Photonics3, 654–657 (2009).
    [CrossRef]
  4. H. Ko, S. Singamaneni, and V. V. Tsukruk, “Nanostructured surfaces and assemblies as SERS media,” Small4, 1576–1599 (2008).
    [CrossRef] [PubMed]
  5. P. Mühlschlegel, H. J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science308, 1607–1609 (2005).
    [CrossRef] [PubMed]
  6. Y. Fu and J. R. Lakowicz, “Modification of single molecule fluorescence near metallic nanostructures,” Laser Photon. Rev.3, 221–232 (2009).
    [CrossRef]
  7. R. Hostein, H. Aouani, H. Rigneault, and J. Wenger, “Deciphering fluorescence signals by quantifying separately the excitation intensity from the number of emitters,” Opt. Lett.36, 3317–3319 (2011).
    [CrossRef] [PubMed]
  8. K. Fujita, M. Kobayashi, S. Kawano, M. Yamanaka, and S. Kawata, “High-resolution confocal microscopy by saturated excitation of fluorescence,” Phys. Rev. Lett.99, 228105 (2007).
    [CrossRef]
  9. M. Yamanaka, S. Kawano, K. Fujita, N. I. Smith, and S. Kawata, “Beyond the diffraction-limit biological imaging by saturated excitation microscopy,” J. Biomed. Opt.13, 050507 (2008).
    [CrossRef] [PubMed]
  10. H. J. Lezec, A. Degiron, E. Devaux, R. A. Linke, L. Martin-Moreno, F. J. Garcia-Vidal, and T. W. Ebbesen, “Beaming light from a subwavelength aperture,” Science297, 820–822 (2002).
    [CrossRef] [PubMed]
  11. F. J. Garcia-Vidal, L. Martin-Moreno, T. W. Ebbesen, and L. Kuipers, “Light passing through subwavelength apertures,” Rev. Mod. Phys.82, 729–787 (2010).
    [CrossRef]
  12. H. Aouani, O. Mahboub, N. Bonod, E. Devaux, E. Popov, H. Rigneault, T. W. Ebbesen, and J. Wenger, “Bright unidirectional fluorescence emission of molecules in a nanoaperture with plasmonic corrugations,” Nano Lett.11, 637–644 (2011).
    [CrossRef] [PubMed]
  13. Y. C. Jun, K. C. Y. Huang, and M. L. Brongersma, “Plasmonic beaming and active control over fluorescent emission,” Nature Commun.2, 283 (2011).
    [CrossRef]
  14. H. Aouani, O. Mahboub, E. Devaux, H. Rigneault, T. W. Ebbesen, and J. Wenger, “Large molecular fluorescence enhancement by a nanoaperture with plasmonic corrugations,” Opt. Express19, 13056–13062 (2011).
    [CrossRef] [PubMed]
  15. O. Mahboub, S. Carretero Palacios, C. Genet, F. J. Garcia-Vidal, S. G. Rodrigo, L. Martin-Moreno, and T. W. Ebbesen, “Optimization of bulls eye structures for transmission enhancement,” Opt. Express18, 11292–11299 (2010).
    [CrossRef] [PubMed]
  16. H. Aouani, S. Itzhakov, D. Gachet, E. Devaux, T. W. Ebbesen, H. Rigneault, D. Oron, and J. Wenger, “Colloidal quantum dots as probes of excitation field enhancement in photonic antennas,” ACS Nano8, 4571–4578 (2010).
    [CrossRef]
  17. N. Djaker, R. Hostein, E. Devaux, T. W. Ebbesen, H. Rigneault, and J. Wenger, “Surface enhanced Raman Scattering on a single nanometric aperture,” J. Phys. Chem. C114, 16250–16256 (2010).
    [CrossRef]

2011 (5)

L. Novotny and N. van Hulst, “Antennas for light,” Nat. Photonics5, 83–90 (2011).
[CrossRef]

R. Hostein, H. Aouani, H. Rigneault, and J. Wenger, “Deciphering fluorescence signals by quantifying separately the excitation intensity from the number of emitters,” Opt. Lett.36, 3317–3319 (2011).
[CrossRef] [PubMed]

H. Aouani, O. Mahboub, N. Bonod, E. Devaux, E. Popov, H. Rigneault, T. W. Ebbesen, and J. Wenger, “Bright unidirectional fluorescence emission of molecules in a nanoaperture with plasmonic corrugations,” Nano Lett.11, 637–644 (2011).
[CrossRef] [PubMed]

Y. C. Jun, K. C. Y. Huang, and M. L. Brongersma, “Plasmonic beaming and active control over fluorescent emission,” Nature Commun.2, 283 (2011).
[CrossRef]

H. Aouani, O. Mahboub, E. Devaux, H. Rigneault, T. W. Ebbesen, and J. Wenger, “Large molecular fluorescence enhancement by a nanoaperture with plasmonic corrugations,” Opt. Express19, 13056–13062 (2011).
[CrossRef] [PubMed]

2010 (5)

O. Mahboub, S. Carretero Palacios, C. Genet, F. J. Garcia-Vidal, S. G. Rodrigo, L. Martin-Moreno, and T. W. Ebbesen, “Optimization of bulls eye structures for transmission enhancement,” Opt. Express18, 11292–11299 (2010).
[CrossRef] [PubMed]

H. Aouani, S. Itzhakov, D. Gachet, E. Devaux, T. W. Ebbesen, H. Rigneault, D. Oron, and J. Wenger, “Colloidal quantum dots as probes of excitation field enhancement in photonic antennas,” ACS Nano8, 4571–4578 (2010).
[CrossRef]

N. Djaker, R. Hostein, E. Devaux, T. W. Ebbesen, H. Rigneault, and J. Wenger, “Surface enhanced Raman Scattering on a single nanometric aperture,” J. Phys. Chem. C114, 16250–16256 (2010).
[CrossRef]

F. J. Garcia-Vidal, L. Martin-Moreno, T. W. Ebbesen, and L. Kuipers, “Light passing through subwavelength apertures,” Rev. Mod. Phys.82, 729–787 (2010).
[CrossRef]

J. A. Schuller, E. S. Barnard, W. S. Cai, Y. C. Jun, J. S. White, and M. L. Brongersma, “Plasmonics for extreme light concentration and manipulation,” Nature Mater.9, 193–204 (2010).
[CrossRef]

2009 (2)

A. Kinkhabwala, Z. F. Yu, S. H. Fan, Y. Avlasevich, K. Mullen, and W. E. Moerner, “Large single-molecule fluorescence enhancements produced by a bowtie nanoantenna,” Nat. Photonics3, 654–657 (2009).
[CrossRef]

Y. Fu and J. R. Lakowicz, “Modification of single molecule fluorescence near metallic nanostructures,” Laser Photon. Rev.3, 221–232 (2009).
[CrossRef]

2008 (2)

H. Ko, S. Singamaneni, and V. V. Tsukruk, “Nanostructured surfaces and assemblies as SERS media,” Small4, 1576–1599 (2008).
[CrossRef] [PubMed]

M. Yamanaka, S. Kawano, K. Fujita, N. I. Smith, and S. Kawata, “Beyond the diffraction-limit biological imaging by saturated excitation microscopy,” J. Biomed. Opt.13, 050507 (2008).
[CrossRef] [PubMed]

2007 (1)

K. Fujita, M. Kobayashi, S. Kawano, M. Yamanaka, and S. Kawata, “High-resolution confocal microscopy by saturated excitation of fluorescence,” Phys. Rev. Lett.99, 228105 (2007).
[CrossRef]

2005 (1)

P. Mühlschlegel, H. J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science308, 1607–1609 (2005).
[CrossRef] [PubMed]

2002 (1)

H. J. Lezec, A. Degiron, E. Devaux, R. A. Linke, L. Martin-Moreno, F. J. Garcia-Vidal, and T. W. Ebbesen, “Beaming light from a subwavelength aperture,” Science297, 820–822 (2002).
[CrossRef] [PubMed]

Aouani, H.

H. Aouani, O. Mahboub, N. Bonod, E. Devaux, E. Popov, H. Rigneault, T. W. Ebbesen, and J. Wenger, “Bright unidirectional fluorescence emission of molecules in a nanoaperture with plasmonic corrugations,” Nano Lett.11, 637–644 (2011).
[CrossRef] [PubMed]

H. Aouani, O. Mahboub, E. Devaux, H. Rigneault, T. W. Ebbesen, and J. Wenger, “Large molecular fluorescence enhancement by a nanoaperture with plasmonic corrugations,” Opt. Express19, 13056–13062 (2011).
[CrossRef] [PubMed]

R. Hostein, H. Aouani, H. Rigneault, and J. Wenger, “Deciphering fluorescence signals by quantifying separately the excitation intensity from the number of emitters,” Opt. Lett.36, 3317–3319 (2011).
[CrossRef] [PubMed]

H. Aouani, S. Itzhakov, D. Gachet, E. Devaux, T. W. Ebbesen, H. Rigneault, D. Oron, and J. Wenger, “Colloidal quantum dots as probes of excitation field enhancement in photonic antennas,” ACS Nano8, 4571–4578 (2010).
[CrossRef]

Avlasevich, Y.

A. Kinkhabwala, Z. F. Yu, S. H. Fan, Y. Avlasevich, K. Mullen, and W. E. Moerner, “Large single-molecule fluorescence enhancements produced by a bowtie nanoantenna,” Nat. Photonics3, 654–657 (2009).
[CrossRef]

Barnard, E. S.

J. A. Schuller, E. S. Barnard, W. S. Cai, Y. C. Jun, J. S. White, and M. L. Brongersma, “Plasmonics for extreme light concentration and manipulation,” Nature Mater.9, 193–204 (2010).
[CrossRef]

Bonod, N.

H. Aouani, O. Mahboub, N. Bonod, E. Devaux, E. Popov, H. Rigneault, T. W. Ebbesen, and J. Wenger, “Bright unidirectional fluorescence emission of molecules in a nanoaperture with plasmonic corrugations,” Nano Lett.11, 637–644 (2011).
[CrossRef] [PubMed]

Brongersma, M. L.

Y. C. Jun, K. C. Y. Huang, and M. L. Brongersma, “Plasmonic beaming and active control over fluorescent emission,” Nature Commun.2, 283 (2011).
[CrossRef]

J. A. Schuller, E. S. Barnard, W. S. Cai, Y. C. Jun, J. S. White, and M. L. Brongersma, “Plasmonics for extreme light concentration and manipulation,” Nature Mater.9, 193–204 (2010).
[CrossRef]

Cai, W. S.

J. A. Schuller, E. S. Barnard, W. S. Cai, Y. C. Jun, J. S. White, and M. L. Brongersma, “Plasmonics for extreme light concentration and manipulation,” Nature Mater.9, 193–204 (2010).
[CrossRef]

Carretero Palacios, S.

Degiron, A.

H. J. Lezec, A. Degiron, E. Devaux, R. A. Linke, L. Martin-Moreno, F. J. Garcia-Vidal, and T. W. Ebbesen, “Beaming light from a subwavelength aperture,” Science297, 820–822 (2002).
[CrossRef] [PubMed]

Devaux, E.

H. Aouani, O. Mahboub, N. Bonod, E. Devaux, E. Popov, H. Rigneault, T. W. Ebbesen, and J. Wenger, “Bright unidirectional fluorescence emission of molecules in a nanoaperture with plasmonic corrugations,” Nano Lett.11, 637–644 (2011).
[CrossRef] [PubMed]

H. Aouani, O. Mahboub, E. Devaux, H. Rigneault, T. W. Ebbesen, and J. Wenger, “Large molecular fluorescence enhancement by a nanoaperture with plasmonic corrugations,” Opt. Express19, 13056–13062 (2011).
[CrossRef] [PubMed]

H. Aouani, S. Itzhakov, D. Gachet, E. Devaux, T. W. Ebbesen, H. Rigneault, D. Oron, and J. Wenger, “Colloidal quantum dots as probes of excitation field enhancement in photonic antennas,” ACS Nano8, 4571–4578 (2010).
[CrossRef]

N. Djaker, R. Hostein, E. Devaux, T. W. Ebbesen, H. Rigneault, and J. Wenger, “Surface enhanced Raman Scattering on a single nanometric aperture,” J. Phys. Chem. C114, 16250–16256 (2010).
[CrossRef]

H. J. Lezec, A. Degiron, E. Devaux, R. A. Linke, L. Martin-Moreno, F. J. Garcia-Vidal, and T. W. Ebbesen, “Beaming light from a subwavelength aperture,” Science297, 820–822 (2002).
[CrossRef] [PubMed]

Djaker, N.

N. Djaker, R. Hostein, E. Devaux, T. W. Ebbesen, H. Rigneault, and J. Wenger, “Surface enhanced Raman Scattering on a single nanometric aperture,” J. Phys. Chem. C114, 16250–16256 (2010).
[CrossRef]

Ebbesen, T. W.

H. Aouani, O. Mahboub, E. Devaux, H. Rigneault, T. W. Ebbesen, and J. Wenger, “Large molecular fluorescence enhancement by a nanoaperture with plasmonic corrugations,” Opt. Express19, 13056–13062 (2011).
[CrossRef] [PubMed]

H. Aouani, O. Mahboub, N. Bonod, E. Devaux, E. Popov, H. Rigneault, T. W. Ebbesen, and J. Wenger, “Bright unidirectional fluorescence emission of molecules in a nanoaperture with plasmonic corrugations,” Nano Lett.11, 637–644 (2011).
[CrossRef] [PubMed]

H. Aouani, S. Itzhakov, D. Gachet, E. Devaux, T. W. Ebbesen, H. Rigneault, D. Oron, and J. Wenger, “Colloidal quantum dots as probes of excitation field enhancement in photonic antennas,” ACS Nano8, 4571–4578 (2010).
[CrossRef]

N. Djaker, R. Hostein, E. Devaux, T. W. Ebbesen, H. Rigneault, and J. Wenger, “Surface enhanced Raman Scattering on a single nanometric aperture,” J. Phys. Chem. C114, 16250–16256 (2010).
[CrossRef]

O. Mahboub, S. Carretero Palacios, C. Genet, F. J. Garcia-Vidal, S. G. Rodrigo, L. Martin-Moreno, and T. W. Ebbesen, “Optimization of bulls eye structures for transmission enhancement,” Opt. Express18, 11292–11299 (2010).
[CrossRef] [PubMed]

F. J. Garcia-Vidal, L. Martin-Moreno, T. W. Ebbesen, and L. Kuipers, “Light passing through subwavelength apertures,” Rev. Mod. Phys.82, 729–787 (2010).
[CrossRef]

H. J. Lezec, A. Degiron, E. Devaux, R. A. Linke, L. Martin-Moreno, F. J. Garcia-Vidal, and T. W. Ebbesen, “Beaming light from a subwavelength aperture,” Science297, 820–822 (2002).
[CrossRef] [PubMed]

Eisler, H. J.

P. Mühlschlegel, H. J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science308, 1607–1609 (2005).
[CrossRef] [PubMed]

Fan, S. H.

A. Kinkhabwala, Z. F. Yu, S. H. Fan, Y. Avlasevich, K. Mullen, and W. E. Moerner, “Large single-molecule fluorescence enhancements produced by a bowtie nanoantenna,” Nat. Photonics3, 654–657 (2009).
[CrossRef]

Fu, Y.

Y. Fu and J. R. Lakowicz, “Modification of single molecule fluorescence near metallic nanostructures,” Laser Photon. Rev.3, 221–232 (2009).
[CrossRef]

Fujita, K.

M. Yamanaka, S. Kawano, K. Fujita, N. I. Smith, and S. Kawata, “Beyond the diffraction-limit biological imaging by saturated excitation microscopy,” J. Biomed. Opt.13, 050507 (2008).
[CrossRef] [PubMed]

K. Fujita, M. Kobayashi, S. Kawano, M. Yamanaka, and S. Kawata, “High-resolution confocal microscopy by saturated excitation of fluorescence,” Phys. Rev. Lett.99, 228105 (2007).
[CrossRef]

Gachet, D.

H. Aouani, S. Itzhakov, D. Gachet, E. Devaux, T. W. Ebbesen, H. Rigneault, D. Oron, and J. Wenger, “Colloidal quantum dots as probes of excitation field enhancement in photonic antennas,” ACS Nano8, 4571–4578 (2010).
[CrossRef]

Garcia-Vidal, F. J.

F. J. Garcia-Vidal, L. Martin-Moreno, T. W. Ebbesen, and L. Kuipers, “Light passing through subwavelength apertures,” Rev. Mod. Phys.82, 729–787 (2010).
[CrossRef]

O. Mahboub, S. Carretero Palacios, C. Genet, F. J. Garcia-Vidal, S. G. Rodrigo, L. Martin-Moreno, and T. W. Ebbesen, “Optimization of bulls eye structures for transmission enhancement,” Opt. Express18, 11292–11299 (2010).
[CrossRef] [PubMed]

H. J. Lezec, A. Degiron, E. Devaux, R. A. Linke, L. Martin-Moreno, F. J. Garcia-Vidal, and T. W. Ebbesen, “Beaming light from a subwavelength aperture,” Science297, 820–822 (2002).
[CrossRef] [PubMed]

Genet, C.

Hecht, B.

P. Mühlschlegel, H. J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science308, 1607–1609 (2005).
[CrossRef] [PubMed]

Hostein, R.

R. Hostein, H. Aouani, H. Rigneault, and J. Wenger, “Deciphering fluorescence signals by quantifying separately the excitation intensity from the number of emitters,” Opt. Lett.36, 3317–3319 (2011).
[CrossRef] [PubMed]

N. Djaker, R. Hostein, E. Devaux, T. W. Ebbesen, H. Rigneault, and J. Wenger, “Surface enhanced Raman Scattering on a single nanometric aperture,” J. Phys. Chem. C114, 16250–16256 (2010).
[CrossRef]

Huang, K. C. Y.

Y. C. Jun, K. C. Y. Huang, and M. L. Brongersma, “Plasmonic beaming and active control over fluorescent emission,” Nature Commun.2, 283 (2011).
[CrossRef]

Itzhakov, S.

H. Aouani, S. Itzhakov, D. Gachet, E. Devaux, T. W. Ebbesen, H. Rigneault, D. Oron, and J. Wenger, “Colloidal quantum dots as probes of excitation field enhancement in photonic antennas,” ACS Nano8, 4571–4578 (2010).
[CrossRef]

Jun, Y. C.

Y. C. Jun, K. C. Y. Huang, and M. L. Brongersma, “Plasmonic beaming and active control over fluorescent emission,” Nature Commun.2, 283 (2011).
[CrossRef]

J. A. Schuller, E. S. Barnard, W. S. Cai, Y. C. Jun, J. S. White, and M. L. Brongersma, “Plasmonics for extreme light concentration and manipulation,” Nature Mater.9, 193–204 (2010).
[CrossRef]

Kawano, S.

M. Yamanaka, S. Kawano, K. Fujita, N. I. Smith, and S. Kawata, “Beyond the diffraction-limit biological imaging by saturated excitation microscopy,” J. Biomed. Opt.13, 050507 (2008).
[CrossRef] [PubMed]

K. Fujita, M. Kobayashi, S. Kawano, M. Yamanaka, and S. Kawata, “High-resolution confocal microscopy by saturated excitation of fluorescence,” Phys. Rev. Lett.99, 228105 (2007).
[CrossRef]

Kawata, S.

M. Yamanaka, S. Kawano, K. Fujita, N. I. Smith, and S. Kawata, “Beyond the diffraction-limit biological imaging by saturated excitation microscopy,” J. Biomed. Opt.13, 050507 (2008).
[CrossRef] [PubMed]

K. Fujita, M. Kobayashi, S. Kawano, M. Yamanaka, and S. Kawata, “High-resolution confocal microscopy by saturated excitation of fluorescence,” Phys. Rev. Lett.99, 228105 (2007).
[CrossRef]

Kinkhabwala, A.

A. Kinkhabwala, Z. F. Yu, S. H. Fan, Y. Avlasevich, K. Mullen, and W. E. Moerner, “Large single-molecule fluorescence enhancements produced by a bowtie nanoantenna,” Nat. Photonics3, 654–657 (2009).
[CrossRef]

Ko, H.

H. Ko, S. Singamaneni, and V. V. Tsukruk, “Nanostructured surfaces and assemblies as SERS media,” Small4, 1576–1599 (2008).
[CrossRef] [PubMed]

Kobayashi, M.

K. Fujita, M. Kobayashi, S. Kawano, M. Yamanaka, and S. Kawata, “High-resolution confocal microscopy by saturated excitation of fluorescence,” Phys. Rev. Lett.99, 228105 (2007).
[CrossRef]

Kuipers, L.

F. J. Garcia-Vidal, L. Martin-Moreno, T. W. Ebbesen, and L. Kuipers, “Light passing through subwavelength apertures,” Rev. Mod. Phys.82, 729–787 (2010).
[CrossRef]

Lakowicz, J. R.

Y. Fu and J. R. Lakowicz, “Modification of single molecule fluorescence near metallic nanostructures,” Laser Photon. Rev.3, 221–232 (2009).
[CrossRef]

Lezec, H. J.

H. J. Lezec, A. Degiron, E. Devaux, R. A. Linke, L. Martin-Moreno, F. J. Garcia-Vidal, and T. W. Ebbesen, “Beaming light from a subwavelength aperture,” Science297, 820–822 (2002).
[CrossRef] [PubMed]

Linke, R. A.

H. J. Lezec, A. Degiron, E. Devaux, R. A. Linke, L. Martin-Moreno, F. J. Garcia-Vidal, and T. W. Ebbesen, “Beaming light from a subwavelength aperture,” Science297, 820–822 (2002).
[CrossRef] [PubMed]

Mahboub, O.

Martin, O. J. F.

P. Mühlschlegel, H. J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science308, 1607–1609 (2005).
[CrossRef] [PubMed]

Martin-Moreno, L.

O. Mahboub, S. Carretero Palacios, C. Genet, F. J. Garcia-Vidal, S. G. Rodrigo, L. Martin-Moreno, and T. W. Ebbesen, “Optimization of bulls eye structures for transmission enhancement,” Opt. Express18, 11292–11299 (2010).
[CrossRef] [PubMed]

F. J. Garcia-Vidal, L. Martin-Moreno, T. W. Ebbesen, and L. Kuipers, “Light passing through subwavelength apertures,” Rev. Mod. Phys.82, 729–787 (2010).
[CrossRef]

H. J. Lezec, A. Degiron, E. Devaux, R. A. Linke, L. Martin-Moreno, F. J. Garcia-Vidal, and T. W. Ebbesen, “Beaming light from a subwavelength aperture,” Science297, 820–822 (2002).
[CrossRef] [PubMed]

Moerner, W. E.

A. Kinkhabwala, Z. F. Yu, S. H. Fan, Y. Avlasevich, K. Mullen, and W. E. Moerner, “Large single-molecule fluorescence enhancements produced by a bowtie nanoantenna,” Nat. Photonics3, 654–657 (2009).
[CrossRef]

Mühlschlegel, P.

P. Mühlschlegel, H. J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science308, 1607–1609 (2005).
[CrossRef] [PubMed]

Mullen, K.

A. Kinkhabwala, Z. F. Yu, S. H. Fan, Y. Avlasevich, K. Mullen, and W. E. Moerner, “Large single-molecule fluorescence enhancements produced by a bowtie nanoantenna,” Nat. Photonics3, 654–657 (2009).
[CrossRef]

Novotny, L.

L. Novotny and N. van Hulst, “Antennas for light,” Nat. Photonics5, 83–90 (2011).
[CrossRef]

Oron, D.

H. Aouani, S. Itzhakov, D. Gachet, E. Devaux, T. W. Ebbesen, H. Rigneault, D. Oron, and J. Wenger, “Colloidal quantum dots as probes of excitation field enhancement in photonic antennas,” ACS Nano8, 4571–4578 (2010).
[CrossRef]

Pohl, D. W.

P. Mühlschlegel, H. J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science308, 1607–1609 (2005).
[CrossRef] [PubMed]

Popov, E.

H. Aouani, O. Mahboub, N. Bonod, E. Devaux, E. Popov, H. Rigneault, T. W. Ebbesen, and J. Wenger, “Bright unidirectional fluorescence emission of molecules in a nanoaperture with plasmonic corrugations,” Nano Lett.11, 637–644 (2011).
[CrossRef] [PubMed]

Rigneault, H.

H. Aouani, O. Mahboub, N. Bonod, E. Devaux, E. Popov, H. Rigneault, T. W. Ebbesen, and J. Wenger, “Bright unidirectional fluorescence emission of molecules in a nanoaperture with plasmonic corrugations,” Nano Lett.11, 637–644 (2011).
[CrossRef] [PubMed]

H. Aouani, O. Mahboub, E. Devaux, H. Rigneault, T. W. Ebbesen, and J. Wenger, “Large molecular fluorescence enhancement by a nanoaperture with plasmonic corrugations,” Opt. Express19, 13056–13062 (2011).
[CrossRef] [PubMed]

R. Hostein, H. Aouani, H. Rigneault, and J. Wenger, “Deciphering fluorescence signals by quantifying separately the excitation intensity from the number of emitters,” Opt. Lett.36, 3317–3319 (2011).
[CrossRef] [PubMed]

N. Djaker, R. Hostein, E. Devaux, T. W. Ebbesen, H. Rigneault, and J. Wenger, “Surface enhanced Raman Scattering on a single nanometric aperture,” J. Phys. Chem. C114, 16250–16256 (2010).
[CrossRef]

H. Aouani, S. Itzhakov, D. Gachet, E. Devaux, T. W. Ebbesen, H. Rigneault, D. Oron, and J. Wenger, “Colloidal quantum dots as probes of excitation field enhancement in photonic antennas,” ACS Nano8, 4571–4578 (2010).
[CrossRef]

Rodrigo, S. G.

Schuller, J. A.

J. A. Schuller, E. S. Barnard, W. S. Cai, Y. C. Jun, J. S. White, and M. L. Brongersma, “Plasmonics for extreme light concentration and manipulation,” Nature Mater.9, 193–204 (2010).
[CrossRef]

Singamaneni, S.

H. Ko, S. Singamaneni, and V. V. Tsukruk, “Nanostructured surfaces and assemblies as SERS media,” Small4, 1576–1599 (2008).
[CrossRef] [PubMed]

Smith, N. I.

M. Yamanaka, S. Kawano, K. Fujita, N. I. Smith, and S. Kawata, “Beyond the diffraction-limit biological imaging by saturated excitation microscopy,” J. Biomed. Opt.13, 050507 (2008).
[CrossRef] [PubMed]

Tsukruk, V. V.

H. Ko, S. Singamaneni, and V. V. Tsukruk, “Nanostructured surfaces and assemblies as SERS media,” Small4, 1576–1599 (2008).
[CrossRef] [PubMed]

van Hulst, N.

L. Novotny and N. van Hulst, “Antennas for light,” Nat. Photonics5, 83–90 (2011).
[CrossRef]

Wenger, J.

H. Aouani, O. Mahboub, E. Devaux, H. Rigneault, T. W. Ebbesen, and J. Wenger, “Large molecular fluorescence enhancement by a nanoaperture with plasmonic corrugations,” Opt. Express19, 13056–13062 (2011).
[CrossRef] [PubMed]

H. Aouani, O. Mahboub, N. Bonod, E. Devaux, E. Popov, H. Rigneault, T. W. Ebbesen, and J. Wenger, “Bright unidirectional fluorescence emission of molecules in a nanoaperture with plasmonic corrugations,” Nano Lett.11, 637–644 (2011).
[CrossRef] [PubMed]

R. Hostein, H. Aouani, H. Rigneault, and J. Wenger, “Deciphering fluorescence signals by quantifying separately the excitation intensity from the number of emitters,” Opt. Lett.36, 3317–3319 (2011).
[CrossRef] [PubMed]

N. Djaker, R. Hostein, E. Devaux, T. W. Ebbesen, H. Rigneault, and J. Wenger, “Surface enhanced Raman Scattering on a single nanometric aperture,” J. Phys. Chem. C114, 16250–16256 (2010).
[CrossRef]

H. Aouani, S. Itzhakov, D. Gachet, E. Devaux, T. W. Ebbesen, H. Rigneault, D. Oron, and J. Wenger, “Colloidal quantum dots as probes of excitation field enhancement in photonic antennas,” ACS Nano8, 4571–4578 (2010).
[CrossRef]

White, J. S.

J. A. Schuller, E. S. Barnard, W. S. Cai, Y. C. Jun, J. S. White, and M. L. Brongersma, “Plasmonics for extreme light concentration and manipulation,” Nature Mater.9, 193–204 (2010).
[CrossRef]

Yamanaka, M.

M. Yamanaka, S. Kawano, K. Fujita, N. I. Smith, and S. Kawata, “Beyond the diffraction-limit biological imaging by saturated excitation microscopy,” J. Biomed. Opt.13, 050507 (2008).
[CrossRef] [PubMed]

K. Fujita, M. Kobayashi, S. Kawano, M. Yamanaka, and S. Kawata, “High-resolution confocal microscopy by saturated excitation of fluorescence,” Phys. Rev. Lett.99, 228105 (2007).
[CrossRef]

Yu, Z. F.

A. Kinkhabwala, Z. F. Yu, S. H. Fan, Y. Avlasevich, K. Mullen, and W. E. Moerner, “Large single-molecule fluorescence enhancements produced by a bowtie nanoantenna,” Nat. Photonics3, 654–657 (2009).
[CrossRef]

ACS Nano (1)

H. Aouani, S. Itzhakov, D. Gachet, E. Devaux, T. W. Ebbesen, H. Rigneault, D. Oron, and J. Wenger, “Colloidal quantum dots as probes of excitation field enhancement in photonic antennas,” ACS Nano8, 4571–4578 (2010).
[CrossRef]

J. Biomed. Opt. (1)

M. Yamanaka, S. Kawano, K. Fujita, N. I. Smith, and S. Kawata, “Beyond the diffraction-limit biological imaging by saturated excitation microscopy,” J. Biomed. Opt.13, 050507 (2008).
[CrossRef] [PubMed]

J. Phys. Chem. C (1)

N. Djaker, R. Hostein, E. Devaux, T. W. Ebbesen, H. Rigneault, and J. Wenger, “Surface enhanced Raman Scattering on a single nanometric aperture,” J. Phys. Chem. C114, 16250–16256 (2010).
[CrossRef]

Laser Photon. Rev. (1)

Y. Fu and J. R. Lakowicz, “Modification of single molecule fluorescence near metallic nanostructures,” Laser Photon. Rev.3, 221–232 (2009).
[CrossRef]

Nano Lett. (1)

H. Aouani, O. Mahboub, N. Bonod, E. Devaux, E. Popov, H. Rigneault, T. W. Ebbesen, and J. Wenger, “Bright unidirectional fluorescence emission of molecules in a nanoaperture with plasmonic corrugations,” Nano Lett.11, 637–644 (2011).
[CrossRef] [PubMed]

Nat. Photonics (2)

L. Novotny and N. van Hulst, “Antennas for light,” Nat. Photonics5, 83–90 (2011).
[CrossRef]

A. Kinkhabwala, Z. F. Yu, S. H. Fan, Y. Avlasevich, K. Mullen, and W. E. Moerner, “Large single-molecule fluorescence enhancements produced by a bowtie nanoantenna,” Nat. Photonics3, 654–657 (2009).
[CrossRef]

Nature Commun. (1)

Y. C. Jun, K. C. Y. Huang, and M. L. Brongersma, “Plasmonic beaming and active control over fluorescent emission,” Nature Commun.2, 283 (2011).
[CrossRef]

Nature Mater. (1)

J. A. Schuller, E. S. Barnard, W. S. Cai, Y. C. Jun, J. S. White, and M. L. Brongersma, “Plasmonics for extreme light concentration and manipulation,” Nature Mater.9, 193–204 (2010).
[CrossRef]

Opt. Express (2)

Opt. Lett. (1)

Phys. Rev. Lett. (1)

K. Fujita, M. Kobayashi, S. Kawano, M. Yamanaka, and S. Kawata, “High-resolution confocal microscopy by saturated excitation of fluorescence,” Phys. Rev. Lett.99, 228105 (2007).
[CrossRef]

Rev. Mod. Phys. (1)

F. J. Garcia-Vidal, L. Martin-Moreno, T. W. Ebbesen, and L. Kuipers, “Light passing through subwavelength apertures,” Rev. Mod. Phys.82, 729–787 (2010).
[CrossRef]

Science (2)

P. Mühlschlegel, H. J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science308, 1607–1609 (2005).
[CrossRef] [PubMed]

H. J. Lezec, A. Degiron, E. Devaux, R. A. Linke, L. Martin-Moreno, F. J. Garcia-Vidal, and T. W. Ebbesen, “Beaming light from a subwavelength aperture,” Science297, 820–822 (2002).
[CrossRef] [PubMed]

Small (1)

H. Ko, S. Singamaneni, and V. V. Tsukruk, “Nanostructured surfaces and assemblies as SERS media,” Small4, 1576–1599 (2008).
[CrossRef] [PubMed]

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Figures (3)

Fig. 1
Fig. 1

(a) Principle of saturated excitation of fluorescence: upon excitation intensity modulation at a frequency f, the deformed fluorescence signal contains the fundamental frequency f and also harmonics at higher frequencies (2f, 3f ...) which are recorded by lock-in detection. (b) Scanning electron microscope images of single aperture and corrugated aperture with five grooves of 440 nm period.

Fig. 2
Fig. 2

Demodulated fluorescence amplitudes at f = 5 kHz and 2 f = 10 kHz versus average excitation power for (a) the open solution, (b) a single 135 nm aperture and (c) a single aperture with a set of five circular corrugations. Lines are numerical fits based on Eq. (5).

Fig. 3
Fig. 3

(a) Fluorescence amplitudes ratio ρ = F2f/Ff for the different samples. (b) Excitation intensity enhancement deduced from the data set in (a) (filled bars), and compared to the results using fluorescence correlation spectroscopy (FCS, hatched bars) [12].

Equations (8)

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I e ( t ) = I ¯ e ( 1 + α cos ( 2 π f t ) )
F = N κ ϕ σ I e 1 + I e / I sat = N κ ϕ σ I ¯ e ( 1 + α cos ( 2 π f t ) ) 1 + ( I ¯ e / I sat ) ( 1 + α cos ( 2 π f t ) )
F ( t ) = F 0 + F f cos ( 2 π f t ) + F 2 f cos ( 4 π f t ) + F 3 f cos ( 6 π f t ) +
F i f = N κ k r 2 i 1 α i ( I ¯ e / I sat ) i ( 1 + I ¯ e / I sat ) i + 1
F f = N κ k r α I ¯ e / I sat ( 1 + I ¯ e / I sat ) 2 and F 2 f = N κ k r 2 α 2 ( I ¯ e / I sat ) 2 ( 1 + I ¯ e / I sat ) 3
ρ = F 2 f F f = α 2 I ¯ e I ¯ e + I sat
ρ = α 2 I ¯ e I sat
η ρ = ρ ant ρ sol = I ¯ e ant I ¯ e sol I sat sol I sat ant = η exc η I sat

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