Abstract

We simulate the remarkable changes that occur to the decay rates of a fluorescent molecule as a conical metal tip approaches. A new and simple model is developed to reveal and quantify which decay channels are responsible. Our analysis, which is independent of the method of molecular excitation, shows some universal characteristics. As the tip-apex enters the molecule’s near-field, the creation of surface plasmon polaritons can become extraordinarily efficient, leading to an increase in the nonradiative rate and, by proportional radiative-damping, in the radiative rate. Enhancements reaching 3 orders of magnitude have been found, which can improve the apparent brightness of a molecule. At distances less than ~5nm, short-ranged energy transfer to the nano-scale apex quickly becomes dominant and is entirely nonradiative.

© 2007 Optical Society of America

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2007 (2)

F. D. Stefani, K. Vasilev, N. Bocchio, F. Gaul, A. Pomozzi, and M. Kreiter, “Photonic mode density effects on single-molecule fluorescence blinking, ” New J. Phys. 9, 21 (2007).
[Crossref]

N. A. Issa and R. Guckenberger, “Optical nanofocusig on tapered metallic waveguides,” Plasmonics 2, 31–37 (2007).
[Crossref]

2006 (6)

F. M. Huang and D. Richards, “Fluorescence enhancement and energy transfer in apertureless scanning near-field optical microscopy,” J. Opt. A 8, S234–S238 (2006).
[Crossref]

A. Downes, D. Salter, and A. Elfick, “Finite element simulations of tip-enhanced Raman and fluorescence spectroscopy,” J. Phys. Chem. B 110, 6692–6698 (2006).
[Crossref] [PubMed]

R. Carminati, J. J. Greffet, C. Henkel, and J. M. Vigoureux, “Radiative and non-radiative decay of a single molecule close to a metallic nanoparticle,” Opt. Commun. 261, 368–375 (2006).
[Crossref]

J. R. Lakowicz, “Plasmonics in biology and plasmon-controlled fluorescence,” Plasmonics 1, 5–33 (2006).
[Crossref] [PubMed]

P. Anger, P. Bharadwaj, and L. Novotny, “Enhancement and quenching of single-molecule fluorescence,” Phys. Rev. Lett. 96, 4 (2006).
[Crossref]

F. Cannone, G. Chirico, A. R. Bizzarri, and S. Cannistraro, “Quenching and blinking of fluorescence of a single dye molecule bound to gold nanoparticles,” J. Phys. Chem. B 110, 16491–16498 (2006).
[Crossref] [PubMed]

2005 (2)

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, (2005).
[Crossref] [PubMed]

E. Dulkeith, M. Ringler, T. A. Klar, J. Feldmann, A. M. Javier, and W. J. Parak, “Gold nanoparticles quench fluorescence by phase induced radiative rate suppression,” Nano Lett. 5, 585–589 (2005).
[Crossref] [PubMed]

2004 (2)

M. Thomas, J. J. Greffet, R. Carminati, and J. R. Arias-Gonzalez, “Single-molecule spontaneous emission close to absorbing nanostructures,” Appl. Phys. Lett. 85, 3863–3865 (2004).
[Crossref]

H. G. Frey, S. Witt, K. Felderer, and R. Guckenberger, “High-resolution imaging of single fluorescent molecules with the optical near-field of a metal tip,” Phys. Rev. Lett. 93, 200801 (2004).
[Crossref] [PubMed]

2002 (1)

A. Kramer, W. Trabesinger, B. Hecht, and U. P. Wild, “Optical near-field enhancement at a metal tip probed by a single fluorophore,” Appl. Phys. Lett. 80, 1652–1654 (2002).
[Crossref]

2001 (2)

H. Gersen, M. F. Garcia-Parajo, L. Novotny, J. A. Veerman, L. Kuipers, and N. F. Van Hulst, “Near-field effects in single molecule emission,” J. Microsc. 202, 374–378 (2001).
[Crossref] [PubMed]

A. Rahmani, P. C. Chaumet, and F. de Fornel, “Environment-induced modification of spontaneous emission: Single-molecule near-field probe,” Phys. Rev. A 63, 023819 (2001).
[Crossref]

2000 (1)

T. J. Yang, G. A. Lessard, and S. R. Quake, “An apertureless near-field microscope for fluorescence imaging,” Appl. Phys. Lett. 76, 378–380 (2000).
[Crossref]

1999 (2)

N. Hayazawa, 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]

E. J. Sanchez, 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]

1998 (1)

W. L. Barnes, “Fluorescence near interfaces: the role of photonic mode density,” J. Mod. Opt. 45, 661–699 (1998).
[Crossref]

1997 (1)

1996 (1)

L. Novotny, “Single molecule fluorescence in inhomogeneous environments,” Appl. Phys. Lett. 69, 3806–3808 (1996).
[Crossref]

1995 (2)

C. Girard, O. J. F. Martin, and A. Dereux, “Molecular lifetime changes induced by nanometer-scale optical-fields,” Phys. Rev. Lett. 75, 3098–3101 (1995).
[Crossref] [PubMed]

R. X. Bian, R. C. Dunn, and X. S. Xie, “Single molecule emission characteristics in near-field microscopy,” Phys. Rev. Lett. 75, 4772–4775 (1995).
[Crossref] [PubMed]

1994 (1)

L. Novotny and C. Hafner, “Light propagation in a cylindrical waveguide with a complex, metallic, dielectric function,” Phys. Rev. E 50, 4094–4106 (1994).
[Crossref]

1984 (2)

P. Avouris and B. N. J. Persson, “Excited-states at metal-surfaces and their nonradiative relaxation,” J. Phys. Chem. 88, 837–848 (1984).
[Crossref]

G. W. Ford and W. H. Weber, “Electromagnetic-interactions of molecules with metal-surfaces,” Phys. Rep. 113, 195–287 (1984).
[Crossref]

1982 (1)

P. M. Whitmore, H. J. Robota, and C. B. Harris, “Mechanisms for electronic-energy transfer between molecules and metal-surfaces - a comparison of silver and nickel,” J. Chem. Phys. 77, 1560–1568 (1982).
[Crossref]

1978 (1)

R. R. Chance, A. Prock, and R. Silbey, “Molecular fluorescence and energy transfer near interfaces,” Adv. Chem. Phys. 37, 1–65 (1978).
[Crossref]

1972 (1)

P. B. Johnson and R. W. Chirsty, “Optical constants of the noble metals,” Phys. Rev. B 6, 4370–4379 (1972).
[Crossref]

Anger, P.

P. Anger, P. Bharadwaj, and L. Novotny, “Enhancement and quenching of single-molecule fluorescence,” Phys. Rev. Lett. 96, 4 (2006).
[Crossref]

Arias-Gonzalez, J. R.

M. Thomas, J. J. Greffet, R. Carminati, and J. R. Arias-Gonzalez, “Single-molecule spontaneous emission close to absorbing nanostructures,” Appl. Phys. Lett. 85, 3863–3865 (2004).
[Crossref]

Aslan, K.

Y. X. Zhang, K. Aslan, M. J. R. Previte, and C. D. Geddes, “Metal-enhanced fluorescence: Surface plasmons can radiate a fluorophore’s structured emission,” Appl. Phys. Lett.90, (2007).

Avouris, P.

P. Avouris and B. N. J. Persson, “Excited-states at metal-surfaces and their nonradiative relaxation,” J. Phys. Chem. 88, 837–848 (1984).
[Crossref]

Barnes, W. L.

W. L. Barnes, “Fluorescence near interfaces: the role of photonic mode density,” J. Mod. Opt. 45, 661–699 (1998).
[Crossref]

G. Winter and W. L. Barnes, “Emission of light through thin silver films via near-field coupling to surface plasmon polaritons,” Appl. Phys. Lett.88, (2006).
[Crossref]

Bharadwaj, P.

P. Anger, P. Bharadwaj, and L. Novotny, “Enhancement and quenching of single-molecule fluorescence,” Phys. Rev. Lett. 96, 4 (2006).
[Crossref]

Bian, R. X.

R. X. Bian, R. C. Dunn, and X. S. Xie, “Single molecule emission characteristics in near-field microscopy,” Phys. Rev. Lett. 75, 4772–4775 (1995).
[Crossref] [PubMed]

Bizzarri, A. R.

F. Cannone, G. Chirico, A. R. Bizzarri, and S. Cannistraro, “Quenching and blinking of fluorescence of a single dye molecule bound to gold nanoparticles,” J. Phys. Chem. B 110, 16491–16498 (2006).
[Crossref] [PubMed]

Bocchio, N.

F. D. Stefani, K. Vasilev, N. Bocchio, F. Gaul, A. Pomozzi, and M. Kreiter, “Photonic mode density effects on single-molecule fluorescence blinking, ” New J. Phys. 9, 21 (2007).
[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, (2005).
[Crossref] [PubMed]

Cannistraro, S.

F. Cannone, G. Chirico, A. R. Bizzarri, and S. Cannistraro, “Quenching and blinking of fluorescence of a single dye molecule bound to gold nanoparticles,” J. Phys. Chem. B 110, 16491–16498 (2006).
[Crossref] [PubMed]

Cannone, F.

F. Cannone, G. Chirico, A. R. Bizzarri, and S. Cannistraro, “Quenching and blinking of fluorescence of a single dye molecule bound to gold nanoparticles,” J. Phys. Chem. B 110, 16491–16498 (2006).
[Crossref] [PubMed]

Carminati, R.

R. Carminati, J. J. Greffet, C. Henkel, and J. M. Vigoureux, “Radiative and non-radiative decay of a single molecule close to a metallic nanoparticle,” Opt. Commun. 261, 368–375 (2006).
[Crossref]

M. Thomas, J. J. Greffet, R. Carminati, and J. R. Arias-Gonzalez, “Single-molecule spontaneous emission close to absorbing nanostructures,” Appl. Phys. Lett. 85, 3863–3865 (2004).
[Crossref]

Chance, R. R.

R. R. Chance, A. Prock, and R. Silbey, “Molecular fluorescence and energy transfer near interfaces,” Adv. Chem. Phys. 37, 1–65 (1978).
[Crossref]

Chaumet, P. C.

A. Rahmani, P. C. Chaumet, and F. de Fornel, “Environment-induced modification of spontaneous emission: Single-molecule near-field probe,” Phys. Rev. A 63, 023819 (2001).
[Crossref]

Chirico, G.

F. Cannone, G. Chirico, A. R. Bizzarri, and S. Cannistraro, “Quenching and blinking of fluorescence of a single dye molecule bound to gold nanoparticles,” J. Phys. Chem. B 110, 16491–16498 (2006).
[Crossref] [PubMed]

Chirsty, R. W.

P. B. Johnson and R. W. Chirsty, “Optical constants of the noble metals,” Phys. Rev. B 6, 4370–4379 (1972).
[Crossref]

Dereux, A.

C. Girard, O. J. F. Martin, and A. Dereux, “Molecular lifetime changes induced by nanometer-scale optical-fields,” Phys. Rev. Lett. 75, 3098–3101 (1995).
[Crossref] [PubMed]

Downes, A.

A. Downes, D. Salter, and A. Elfick, “Finite element simulations of tip-enhanced Raman and fluorescence spectroscopy,” J. Phys. Chem. B 110, 6692–6698 (2006).
[Crossref] [PubMed]

Dulkeith, E.

E. Dulkeith, M. Ringler, T. A. Klar, J. Feldmann, A. M. Javier, and W. J. Parak, “Gold nanoparticles quench fluorescence by phase induced radiative rate suppression,” Nano Lett. 5, 585–589 (2005).
[Crossref] [PubMed]

Dunn, R. C.

R. X. Bian, R. C. Dunn, and X. S. Xie, “Single molecule emission characteristics in near-field microscopy,” Phys. Rev. Lett. 75, 4772–4775 (1995).
[Crossref] [PubMed]

Eisler, H. J.

J. N. Farahani, D. W. Pohl, H. J. Eisler, and B. Hecht, “Single quantum dot coupled to a scanning optical antenna: A tunable superemitter,” Phys. Rev. Lett.95, (2005).
[Crossref] [PubMed]

Elfick, A.

A. Downes, D. Salter, and A. Elfick, “Finite element simulations of tip-enhanced Raman and fluorescence spectroscopy,” J. Phys. Chem. B 110, 6692–6698 (2006).
[Crossref] [PubMed]

Farahani, J. N.

J. N. Farahani, D. W. Pohl, H. J. Eisler, and B. Hecht, “Single quantum dot coupled to a scanning optical antenna: A tunable superemitter,” Phys. Rev. Lett.95, (2005).
[Crossref] [PubMed]

Felderer, K.

H. G. Frey, S. Witt, K. Felderer, and R. Guckenberger, “High-resolution imaging of single fluorescent molecules with the optical near-field of a metal tip,” Phys. Rev. Lett. 93, 200801 (2004).
[Crossref] [PubMed]

Feldmann, J.

E. Dulkeith, M. Ringler, T. A. Klar, J. Feldmann, A. M. Javier, and W. J. Parak, “Gold nanoparticles quench fluorescence by phase induced radiative rate suppression,” Nano Lett. 5, 585–589 (2005).
[Crossref] [PubMed]

Festy, F.

F. M. Huang, F. Festy, and D. Richards, “Tip-enhanced fluorescence imaging of quantum dots,” Appl. Phys. Lett.87, (2005).
[Crossref]

Ford, G. W.

G. W. Ford and W. H. Weber, “Electromagnetic-interactions of molecules with metal-surfaces,” Phys. Rep. 113, 195–287 (1984).
[Crossref]

Fornel, F. de

A. Rahmani, P. C. Chaumet, and F. de Fornel, “Environment-induced modification of spontaneous emission: Single-molecule near-field probe,” Phys. Rev. A 63, 023819 (2001).
[Crossref]

Frey, H. G.

H. G. Frey, S. Witt, K. Felderer, and R. Guckenberger, “High-resolution imaging of single fluorescent molecules with the optical near-field of a metal tip,” Phys. Rev. Lett. 93, 200801 (2004).
[Crossref] [PubMed]

Garcia-Parajo, M. F.

H. Gersen, M. F. Garcia-Parajo, L. Novotny, J. A. Veerman, L. Kuipers, and N. F. Van Hulst, “Near-field effects in single molecule emission,” J. Microsc. 202, 374–378 (2001).
[Crossref] [PubMed]

Gaul, F.

F. D. Stefani, K. Vasilev, N. Bocchio, F. Gaul, A. Pomozzi, and M. Kreiter, “Photonic mode density effects on single-molecule fluorescence blinking, ” New J. Phys. 9, 21 (2007).
[Crossref]

Geddes, C. D.

Y. X. Zhang, K. Aslan, M. J. R. Previte, and C. D. Geddes, “Metal-enhanced fluorescence: Surface plasmons can radiate a fluorophore’s structured emission,” Appl. Phys. Lett.90, (2007).

Gersen, H.

H. Gersen, M. F. Garcia-Parajo, L. Novotny, J. A. Veerman, L. Kuipers, and N. F. Van Hulst, “Near-field effects in single molecule emission,” J. Microsc. 202, 374–378 (2001).
[Crossref] [PubMed]

Girard, C.

C. Girard, O. J. F. Martin, and A. Dereux, “Molecular lifetime changes induced by nanometer-scale optical-fields,” Phys. Rev. Lett. 75, 3098–3101 (1995).
[Crossref] [PubMed]

Greffet, J. J.

R. Carminati, J. J. Greffet, C. Henkel, and J. M. Vigoureux, “Radiative and non-radiative decay of a single molecule close to a metallic nanoparticle,” Opt. Commun. 261, 368–375 (2006).
[Crossref]

M. Thomas, J. J. Greffet, R. Carminati, and J. R. Arias-Gonzalez, “Single-molecule spontaneous emission close to absorbing nanostructures,” Appl. Phys. Lett. 85, 3863–3865 (2004).
[Crossref]

Guckenberger, R.

N. A. Issa and R. Guckenberger, “Optical nanofocusig on tapered metallic waveguides,” Plasmonics 2, 31–37 (2007).
[Crossref]

H. G. Frey, S. Witt, K. Felderer, and R. Guckenberger, “High-resolution imaging of single fluorescent molecules with the optical near-field of a metal tip,” Phys. Rev. Lett. 93, 200801 (2004).
[Crossref] [PubMed]

Hafner, C.

L. Novotny and C. Hafner, “Light propagation in a cylindrical waveguide with a complex, metallic, dielectric function,” Phys. Rev. E 50, 4094–4106 (1994).
[Crossref]

Hakanson, U.

S. Kuhn, U. Hakanson, L. Rogobete, and V. Sandoghdar, “Enhancement of single-molecule fluorescence using a gold nanoparticle as an optical nanoantenna,” Phys. Rev. Lett.97, (2006).
[Crossref] [PubMed]

Harris, C. B.

P. M. Whitmore, H. J. Robota, and C. B. Harris, “Mechanisms for electronic-energy transfer between molecules and metal-surfaces - a comparison of silver and nickel,” J. Chem. Phys. 77, 1560–1568 (1982).
[Crossref]

Hayazawa, N.

N. Hayazawa, 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]

Hecht, B.

A. Kramer, W. Trabesinger, B. Hecht, and U. P. Wild, “Optical near-field enhancement at a metal tip probed by a single fluorophore,” Appl. Phys. Lett. 80, 1652–1654 (2002).
[Crossref]

J. N. Farahani, D. W. Pohl, H. J. Eisler, and B. Hecht, “Single quantum dot coupled to a scanning optical antenna: A tunable superemitter,” Phys. Rev. Lett.95, (2005).
[Crossref] [PubMed]

Henkel, C.

R. Carminati, J. J. Greffet, C. Henkel, and J. M. Vigoureux, “Radiative and non-radiative decay of a single molecule close to a metallic nanoparticle,” Opt. Commun. 261, 368–375 (2006).
[Crossref]

Huang, F. M.

F. M. Huang and D. Richards, “Fluorescence enhancement and energy transfer in apertureless scanning near-field optical microscopy,” J. Opt. A 8, S234–S238 (2006).
[Crossref]

F. M. Huang, F. Festy, and D. Richards, “Tip-enhanced fluorescence imaging of quantum dots,” Appl. Phys. Lett.87, (2005).
[Crossref]

Inouye, Y.

N. Hayazawa, 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]

Issa, N. A.

N. A. Issa and R. Guckenberger, “Optical nanofocusig on tapered metallic waveguides,” Plasmonics 2, 31–37 (2007).
[Crossref]

Javier, A. M.

E. Dulkeith, M. Ringler, T. A. Klar, J. Feldmann, A. M. Javier, and W. J. Parak, “Gold nanoparticles quench fluorescence by phase induced radiative rate suppression,” Nano Lett. 5, 585–589 (2005).
[Crossref] [PubMed]

Johnson, P. B.

P. B. Johnson and R. W. Chirsty, “Optical constants of the noble metals,” Phys. Rev. B 6, 4370–4379 (1972).
[Crossref]

Kawata, S.

N. Hayazawa, 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]

Klar, T. A.

E. Dulkeith, M. Ringler, T. A. Klar, J. Feldmann, A. M. Javier, and W. J. Parak, “Gold nanoparticles quench fluorescence by phase induced radiative rate suppression,” Nano Lett. 5, 585–589 (2005).
[Crossref] [PubMed]

Kobayashi, T.

Kramer, A.

A. Kramer, W. Trabesinger, B. Hecht, and U. P. Wild, “Optical near-field enhancement at a metal tip probed by a single fluorophore,” Appl. Phys. Lett. 80, 1652–1654 (2002).
[Crossref]

Kreiter, M.

F. D. Stefani, K. Vasilev, N. Bocchio, F. Gaul, A. Pomozzi, and M. Kreiter, “Photonic mode density effects on single-molecule fluorescence blinking, ” New J. Phys. 9, 21 (2007).
[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, (2005).
[Crossref] [PubMed]

Krug II, J. T.

J. T. Krug II, E. J. Sanchez, and X. S. Xie, “Fluorescence quenching in tip-enhanced nonlinear optical microscopy,” Appl. Phys. Lett.86, (2005).

Kuhn, S.

S. Kuhn, U. Hakanson, L. Rogobete, and V. Sandoghdar, “Enhancement of single-molecule fluorescence using a gold nanoparticle as an optical nanoantenna,” Phys. Rev. Lett.97, (2006).
[Crossref] [PubMed]

Kuipers, L.

H. Gersen, M. F. Garcia-Parajo, L. Novotny, J. A. Veerman, L. Kuipers, and N. F. Van Hulst, “Near-field effects in single molecule emission,” J. Microsc. 202, 374–378 (2001).
[Crossref] [PubMed]

Lakowicz, J. R.

J. R. Lakowicz, “Plasmonics in biology and plasmon-controlled fluorescence,” Plasmonics 1, 5–33 (2006).
[Crossref] [PubMed]

Lessard, G. A.

T. J. Yang, G. A. Lessard, and S. R. Quake, “An apertureless near-field microscope for fluorescence imaging,” Appl. Phys. Lett. 76, 378–380 (2000).
[Crossref]

Love, J. D.

A. W. Snyder and J. D. Love, Optical waveguide theory (Chapman and Hall, New York, 1983).

Martin, O. J. F.

C. Girard, O. J. F. Martin, and A. Dereux, “Molecular lifetime changes induced by nanometer-scale optical-fields,” Phys. Rev. Lett. 75, 3098–3101 (1995).
[Crossref] [PubMed]

Morimoto, A.

Novotny, L.

P. Anger, P. Bharadwaj, and L. Novotny, “Enhancement and quenching of single-molecule fluorescence,” Phys. Rev. Lett. 96, 4 (2006).
[Crossref]

H. Gersen, M. F. Garcia-Parajo, L. Novotny, J. A. Veerman, L. Kuipers, and N. F. Van Hulst, “Near-field effects in single molecule emission,” J. Microsc. 202, 374–378 (2001).
[Crossref] [PubMed]

E. J. Sanchez, 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]

L. Novotny, “Single molecule fluorescence in inhomogeneous environments,” Appl. Phys. Lett. 69, 3806–3808 (1996).
[Crossref]

L. Novotny and C. Hafner, “Light propagation in a cylindrical waveguide with a complex, metallic, dielectric function,” Phys. Rev. E 50, 4094–4106 (1994).
[Crossref]

Parak, W. J.

E. Dulkeith, M. Ringler, T. A. Klar, J. Feldmann, A. M. Javier, and W. J. Parak, “Gold nanoparticles quench fluorescence by phase induced radiative rate suppression,” Nano Lett. 5, 585–589 (2005).
[Crossref] [PubMed]

Persson, B. N. J.

P. Avouris and B. N. J. Persson, “Excited-states at metal-surfaces and their nonradiative relaxation,” J. Phys. Chem. 88, 837–848 (1984).
[Crossref]

Pohl, D. W.

J. N. Farahani, D. W. Pohl, H. J. Eisler, and B. Hecht, “Single quantum dot coupled to a scanning optical antenna: A tunable superemitter,” Phys. Rev. Lett.95, (2005).
[Crossref] [PubMed]

Pomozzi, A.

F. D. Stefani, K. Vasilev, N. Bocchio, F. Gaul, A. Pomozzi, and M. Kreiter, “Photonic mode density effects on single-molecule fluorescence blinking, ” New J. Phys. 9, 21 (2007).
[Crossref]

Previte, M. J. R.

Y. X. Zhang, K. Aslan, M. J. R. Previte, and C. D. Geddes, “Metal-enhanced fluorescence: Surface plasmons can radiate a fluorophore’s structured emission,” Appl. Phys. Lett.90, (2007).

Prock, A.

R. R. Chance, A. Prock, and R. Silbey, “Molecular fluorescence and energy transfer near interfaces,” Adv. Chem. Phys. 37, 1–65 (1978).
[Crossref]

Quake, S. R.

T. J. Yang, G. A. Lessard, and S. R. Quake, “An apertureless near-field microscope for fluorescence imaging,” Appl. Phys. Lett. 76, 378–380 (2000).
[Crossref]

Rahmani, A.

A. Rahmani, P. C. Chaumet, and F. de Fornel, “Environment-induced modification of spontaneous emission: Single-molecule near-field probe,” Phys. Rev. A 63, 023819 (2001).
[Crossref]

Richards, D.

F. M. Huang and D. Richards, “Fluorescence enhancement and energy transfer in apertureless scanning near-field optical microscopy,” J. Opt. A 8, S234–S238 (2006).
[Crossref]

F. M. Huang, F. Festy, and D. Richards, “Tip-enhanced fluorescence imaging of quantum dots,” Appl. Phys. Lett.87, (2005).
[Crossref]

Ringler, M.

E. Dulkeith, M. Ringler, T. A. Klar, J. Feldmann, A. M. Javier, and W. J. Parak, “Gold nanoparticles quench fluorescence by phase induced radiative rate suppression,” Nano Lett. 5, 585–589 (2005).
[Crossref] [PubMed]

Robota, H. J.

P. M. Whitmore, H. J. Robota, and C. B. Harris, “Mechanisms for electronic-energy transfer between molecules and metal-surfaces - a comparison of silver and nickel,” J. Chem. Phys. 77, 1560–1568 (1982).
[Crossref]

Rogobete, L.

S. Kuhn, U. Hakanson, L. Rogobete, and V. Sandoghdar, “Enhancement of single-molecule fluorescence using a gold nanoparticle as an optical nanoantenna,” Phys. Rev. Lett.97, (2006).
[Crossref] [PubMed]

Salter, D.

A. Downes, D. Salter, and A. Elfick, “Finite element simulations of tip-enhanced Raman and fluorescence spectroscopy,” J. Phys. Chem. B 110, 6692–6698 (2006).
[Crossref] [PubMed]

Sanchez, E. J.

E. J. Sanchez, 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]

J. T. Krug II, E. J. Sanchez, and X. S. Xie, “Fluorescence quenching in tip-enhanced nonlinear optical microscopy,” Appl. Phys. Lett.86, (2005).

Sandoghdar, V.

S. Kuhn, U. Hakanson, L. Rogobete, and V. Sandoghdar, “Enhancement of single-molecule fluorescence using a gold nanoparticle as an optical nanoantenna,” Phys. Rev. Lett.97, (2006).
[Crossref] [PubMed]

Silbey, R.

R. R. Chance, A. Prock, and R. Silbey, “Molecular fluorescence and energy transfer near interfaces,” Adv. Chem. Phys. 37, 1–65 (1978).
[Crossref]

Snyder, A. W.

A. W. Snyder and J. D. Love, Optical waveguide theory (Chapman and Hall, New York, 1983).

Stefani, F. D.

F. D. Stefani, K. Vasilev, N. Bocchio, F. Gaul, A. Pomozzi, and M. Kreiter, “Photonic mode density effects on single-molecule fluorescence blinking, ” New J. Phys. 9, 21 (2007).
[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, (2005).
[Crossref] [PubMed]

Stoyanova, N.

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, (2005).
[Crossref] [PubMed]

Takahara, J.

Taki, H.

Thomas, M.

M. Thomas, J. J. Greffet, R. Carminati, and J. R. Arias-Gonzalez, “Single-molecule spontaneous emission close to absorbing nanostructures,” Appl. Phys. Lett. 85, 3863–3865 (2004).
[Crossref]

Trabesinger, W.

A. Kramer, W. Trabesinger, B. Hecht, and U. P. Wild, “Optical near-field enhancement at a metal tip probed by a single fluorophore,” Appl. Phys. Lett. 80, 1652–1654 (2002).
[Crossref]

Van Hulst, N. F.

H. Gersen, M. F. Garcia-Parajo, L. Novotny, J. A. Veerman, L. Kuipers, and N. F. Van Hulst, “Near-field effects in single molecule emission,” J. Microsc. 202, 374–378 (2001).
[Crossref] [PubMed]

Vasilev, K.

F. D. Stefani, K. Vasilev, N. Bocchio, F. Gaul, A. Pomozzi, and M. Kreiter, “Photonic mode density effects on single-molecule fluorescence blinking, ” New J. Phys. 9, 21 (2007).
[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, (2005).
[Crossref] [PubMed]

Veerman, J. A.

H. Gersen, M. F. Garcia-Parajo, L. Novotny, J. A. Veerman, L. Kuipers, and N. F. Van Hulst, “Near-field effects in single molecule emission,” J. Microsc. 202, 374–378 (2001).
[Crossref] [PubMed]

Vigoureux, J. M.

R. Carminati, J. J. Greffet, C. Henkel, and J. M. Vigoureux, “Radiative and non-radiative decay of a single molecule close to a metallic nanoparticle,” Opt. Commun. 261, 368–375 (2006).
[Crossref]

Weber, W. H.

G. W. Ford and W. H. Weber, “Electromagnetic-interactions of molecules with metal-surfaces,” Phys. Rep. 113, 195–287 (1984).
[Crossref]

Whitmore, P. M.

P. M. Whitmore, H. J. Robota, and C. B. Harris, “Mechanisms for electronic-energy transfer between molecules and metal-surfaces - a comparison of silver and nickel,” J. Chem. Phys. 77, 1560–1568 (1982).
[Crossref]

Wild, U. P.

A. Kramer, W. Trabesinger, B. Hecht, and U. P. Wild, “Optical near-field enhancement at a metal tip probed by a single fluorophore,” Appl. Phys. Lett. 80, 1652–1654 (2002).
[Crossref]

Winter, G.

G. Winter and W. L. Barnes, “Emission of light through thin silver films via near-field coupling to surface plasmon polaritons,” Appl. Phys. Lett.88, (2006).
[Crossref]

Witt, S.

H. G. Frey, S. Witt, K. Felderer, and R. Guckenberger, “High-resolution imaging of single fluorescent molecules with the optical near-field of a metal tip,” Phys. Rev. Lett. 93, 200801 (2004).
[Crossref] [PubMed]

Xie, X. S.

E. J. Sanchez, 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]

R. X. Bian, R. C. Dunn, and X. S. Xie, “Single molecule emission characteristics in near-field microscopy,” Phys. Rev. Lett. 75, 4772–4775 (1995).
[Crossref] [PubMed]

J. T. Krug II, E. J. Sanchez, and X. S. Xie, “Fluorescence quenching in tip-enhanced nonlinear optical microscopy,” Appl. Phys. Lett.86, (2005).

Yamagishi, S.

Yang, T. J.

T. J. Yang, G. A. Lessard, and S. R. Quake, “An apertureless near-field microscope for fluorescence imaging,” Appl. Phys. Lett. 76, 378–380 (2000).
[Crossref]

Zhang, Y. X.

Y. X. Zhang, K. Aslan, M. J. R. Previte, and C. D. Geddes, “Metal-enhanced fluorescence: Surface plasmons can radiate a fluorophore’s structured emission,” Appl. Phys. Lett.90, (2007).

Adv. Chem. Phys. (1)

R. R. Chance, A. Prock, and R. Silbey, “Molecular fluorescence and energy transfer near interfaces,” Adv. Chem. Phys. 37, 1–65 (1978).
[Crossref]

Appl. Phys. Lett. (4)

T. J. Yang, G. A. Lessard, and S. R. Quake, “An apertureless near-field microscope for fluorescence imaging,” Appl. Phys. Lett. 76, 378–380 (2000).
[Crossref]

A. Kramer, W. Trabesinger, B. Hecht, and U. P. Wild, “Optical near-field enhancement at a metal tip probed by a single fluorophore,” Appl. Phys. Lett. 80, 1652–1654 (2002).
[Crossref]

M. Thomas, J. J. Greffet, R. Carminati, and J. R. Arias-Gonzalez, “Single-molecule spontaneous emission close to absorbing nanostructures,” Appl. Phys. Lett. 85, 3863–3865 (2004).
[Crossref]

L. Novotny, “Single molecule fluorescence in inhomogeneous environments,” Appl. Phys. Lett. 69, 3806–3808 (1996).
[Crossref]

J. Chem. Phys. (1)

P. M. Whitmore, H. J. Robota, and C. B. Harris, “Mechanisms for electronic-energy transfer between molecules and metal-surfaces - a comparison of silver and nickel,” J. Chem. Phys. 77, 1560–1568 (1982).
[Crossref]

J. Microsc. (2)

N. Hayazawa, 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]

H. Gersen, M. F. Garcia-Parajo, L. Novotny, J. A. Veerman, L. Kuipers, and N. F. Van Hulst, “Near-field effects in single molecule emission,” J. Microsc. 202, 374–378 (2001).
[Crossref] [PubMed]

J. Mod. Opt. (1)

W. L. Barnes, “Fluorescence near interfaces: the role of photonic mode density,” J. Mod. Opt. 45, 661–699 (1998).
[Crossref]

J. Opt. A (1)

F. M. Huang and D. Richards, “Fluorescence enhancement and energy transfer in apertureless scanning near-field optical microscopy,” J. Opt. A 8, S234–S238 (2006).
[Crossref]

J. Phys. Chem. (1)

P. Avouris and B. N. J. Persson, “Excited-states at metal-surfaces and their nonradiative relaxation,” J. Phys. Chem. 88, 837–848 (1984).
[Crossref]

J. Phys. Chem. B (2)

A. Downes, D. Salter, and A. Elfick, “Finite element simulations of tip-enhanced Raman and fluorescence spectroscopy,” J. Phys. Chem. B 110, 6692–6698 (2006).
[Crossref] [PubMed]

F. Cannone, G. Chirico, A. R. Bizzarri, and S. Cannistraro, “Quenching and blinking of fluorescence of a single dye molecule bound to gold nanoparticles,” J. Phys. Chem. B 110, 16491–16498 (2006).
[Crossref] [PubMed]

Nano Lett. (1)

E. Dulkeith, M. Ringler, T. A. Klar, J. Feldmann, A. M. Javier, and W. J. Parak, “Gold nanoparticles quench fluorescence by phase induced radiative rate suppression,” Nano Lett. 5, 585–589 (2005).
[Crossref] [PubMed]

New J. Phys. (1)

F. D. Stefani, K. Vasilev, N. Bocchio, F. Gaul, A. Pomozzi, and M. Kreiter, “Photonic mode density effects on single-molecule fluorescence blinking, ” New J. Phys. 9, 21 (2007).
[Crossref]

Opt. Commun. (1)

R. Carminati, J. J. Greffet, C. Henkel, and J. M. Vigoureux, “Radiative and non-radiative decay of a single molecule close to a metallic nanoparticle,” Opt. Commun. 261, 368–375 (2006).
[Crossref]

Opt. Lett. (1)

Phys. Rep. (1)

G. W. Ford and W. H. Weber, “Electromagnetic-interactions of molecules with metal-surfaces,” Phys. Rep. 113, 195–287 (1984).
[Crossref]

Phys. Rev. A (1)

A. Rahmani, P. C. Chaumet, and F. de Fornel, “Environment-induced modification of spontaneous emission: Single-molecule near-field probe,” Phys. Rev. A 63, 023819 (2001).
[Crossref]

Phys. Rev. B (1)

P. B. Johnson and R. W. Chirsty, “Optical constants of the noble metals,” Phys. Rev. B 6, 4370–4379 (1972).
[Crossref]

Phys. Rev. E (1)

L. Novotny and C. Hafner, “Light propagation in a cylindrical waveguide with a complex, metallic, dielectric function,” Phys. Rev. E 50, 4094–4106 (1994).
[Crossref]

Phys. Rev. Lett. (6)

C. Girard, O. J. F. Martin, and A. Dereux, “Molecular lifetime changes induced by nanometer-scale optical-fields,” Phys. Rev. Lett. 75, 3098–3101 (1995).
[Crossref] [PubMed]

R. X. Bian, R. C. Dunn, and X. S. Xie, “Single molecule emission characteristics in near-field microscopy,” Phys. Rev. Lett. 75, 4772–4775 (1995).
[Crossref] [PubMed]

H. G. Frey, S. Witt, K. Felderer, and R. Guckenberger, “High-resolution imaging of single fluorescent molecules with the optical near-field of a metal tip,” Phys. Rev. Lett. 93, 200801 (2004).
[Crossref] [PubMed]

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, (2005).
[Crossref] [PubMed]

P. Anger, P. Bharadwaj, and L. Novotny, “Enhancement and quenching of single-molecule fluorescence,” Phys. Rev. Lett. 96, 4 (2006).
[Crossref]

E. J. Sanchez, 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]

Plasmonics (2)

J. R. Lakowicz, “Plasmonics in biology and plasmon-controlled fluorescence,” Plasmonics 1, 5–33 (2006).
[Crossref] [PubMed]

N. A. Issa and R. Guckenberger, “Optical nanofocusig on tapered metallic waveguides,” Plasmonics 2, 31–37 (2007).
[Crossref]

Other (8)

J. T. Krug II, E. J. Sanchez, and X. S. Xie, “Fluorescence quenching in tip-enhanced nonlinear optical microscopy,” Appl. Phys. Lett.86, (2005).

A. W. Snyder and J. D. Love, Optical waveguide theory (Chapman and Hall, New York, 1983).

D. R. Lide, ed. CRC handbook of chemistry and physics (CRC press, London, 1996).

Y. X. Zhang, K. Aslan, M. J. R. Previte, and C. D. Geddes, “Metal-enhanced fluorescence: Surface plasmons can radiate a fluorophore’s structured emission,” Appl. Phys. Lett.90, (2007).

G. Winter and W. L. Barnes, “Emission of light through thin silver films via near-field coupling to surface plasmon polaritons,” Appl. Phys. Lett.88, (2006).
[Crossref]

S. Kuhn, U. Hakanson, L. Rogobete, and V. Sandoghdar, “Enhancement of single-molecule fluorescence using a gold nanoparticle as an optical nanoantenna,” Phys. Rev. Lett.97, (2006).
[Crossref] [PubMed]

J. N. Farahani, D. W. Pohl, H. J. Eisler, and B. Hecht, “Single quantum dot coupled to a scanning optical antenna: A tunable superemitter,” Phys. Rev. Lett.95, (2005).
[Crossref] [PubMed]

F. M. Huang, F. Festy, and D. Richards, “Tip-enhanced fluorescence imaging of quantum dots,” Appl. Phys. Lett.87, (2005).
[Crossref]

Supplementary Material (1)

» Media 1: MOV (3743 KB)     

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Figures (9)

Fig. 1.
Fig. 1.

(a). Example solution, Re(H ϕ), with diagram overlay of the model geometry. This cross-section view is symmetric about indicated axis of rotation. In this figure, the tip (silver) is at a distance D=100nm from the dipole and λ=550nm. The metal tip supports a propagating SPP that is clearly visible. The power in propagating SPPs remaining at the top of the tip is measured prior to the top PML, and is counted as nonradiative. (b) Example FEM meshing near the tip showing adaptation and fine mesh near nano-scale features: D=10nm. (c) Diagram illustrating different parts of the tip where the integrated resistive losses are attributed to SPP losses (volume 1) and local energy transfer (volume 2).

Fig. 2.
Fig. 2.

Comparison of the numerical solution of γ LET/γ̃o with the analytic solution [Eq. (6)] that neglects retardation effects. The numerical solution is for a silver tip using the geometry of Fig. 1(a) (without glass substrate) and λ=550nm. The analytic solution assumes the molecule is at distance D from a flat silver substrate (no tip). For comparison, the normalized total nonradiative rate γ nr/γ̃o is shown.

Fig. 3.
Fig. 3.

Numerical solution for a silver tip using the geometry of Fig. 1(a). (a). All calculated rates shown. γ LET approximates well Eq. (6) when D<~10nm. Γsc is defined in Section 6. (b). Validation of the tip portioning: γ prop/γ SPP≅ constant when D<~20nm and γ SPP/γ nr≠constant.

Fig. 4.
Fig. 4.

Relationship between the radiative rate and the nonradiative-SPP rate. A chance the emission spatial distribution is observed.

Fig. 5.
Fig. 5.

Comparison of efficiencies for two different initial quantum efficiencies. The curves are nearly identical for D<~10nm (see text).

Fig. 6.
Fig. 6.

A hypothetical silver tip without loss

Fig. 7.
Fig. 7.

Simulations for exploring the influence of metal dielectric constant. γ LET approximates well Eq. (6) when D<~10nm for both metals.

Fig. 8.
Fig. 8.

Animation showing the approach of a gold tip (λ=565nm). |Re(H)| is plotted, which has been normalized at each frame (excitation is distance independent). The value of D is stated above. The prevalence of the radiative, SPP and LET rates at different distances is distinct. File size: 3.7 Mb. [Media 1]

Fig. 9.
Fig. 9.

Spectra for gold tips in air and water surrounding medium, with fixed D=30nm.

Tables (1)

Tables Icon

Appendix B: Table of terms

Equations (14)

Equations on this page are rendered with MathJax. Learn more.

γ = γ r + γ i + γ nr .
γ nr = 1 ω tip 1 2 Re ( j * · E ) dV .
γ nr = γ SPP + γ LET .
q = γ r γ = γ r γ r + γ nr + ( 1 q o 1 ) γ o .
x LET < x < x SPP .
γ LET γ ˜ o 3 8 1 ε medium Im { ε metal ε medium ε metal + ε medium } c 3 ω 3 1 D 3 ,
P ( 2 ) = 1 2 ( 2 ) Re ( j * · E ) dV .
γ SPP = γ ( 1 ) + γ prop .
Γ sc = 1 2 ω tip Re ( E s × H s * ) · n ̂ dS γ prop .
σ = ( D 10 nm ) γ r γ SPP + γ r .
P ( 1 ) = 1 2 ( 1 ) Re ( j * · E ) dV .
a = 1 2 S ( E ¯ × H ) · z ̂ dr ,
P prop 2 π R o a 2 P ¯
P ¯ = 1 2 ( E ¯ × H ¯ * ) · z ̂ ' dr ' ,

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