Abstract

Surface-enhanced Raman scattering (SERS) from Rhodamine 6G (R6G) homogenously adsorbed on fractal shaped 170-nm-period square arrays formed by 50-nm-high gold nanoparticles (diameters of 80, 100, or 120 nm are constant within each array), fabricated on a smooth gold film by electron-beam lithography, is characterized using high-resolution Raman microscopy with polarized excitation. Linear reflection spectroscopy verifies that all nanostructures exhibit resonances close to the 532 nm excitation wavelength used for Raman microscopy. The SERS images feature diffraction-limited (0.35μm) bright spots corresponding to local SERS enhancements of up to 120 (relative to that from a smooth gold film), which are influenced by array boundaries, particle diameter, excitation polarization, and detected wavelength. We use six main Raman lines of the R6G spectrum for characterization of multiresonant local-field enhancements that are related to constructive interference of surface plasmon polaritons partially reflected inside the array boundaries.

© 2009 Optical Society of America

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  2. G. T. Boyd, Th. Rasing, J. R. R. Leite, and Y. R. Shen, “Local-field enhancement on rough surfaces of metals, semimetals, and semiconductors with the use of optical second-harmonic generation,” Phys. Rev. B 30, 519-526 (1984).
    [CrossRef]
  3. 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]
  4. K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, “Surface-enhanced Raman scattering and biophysics,” J. Phys. Condens. Matter 14, R597-R624 (2002).
    [CrossRef]
  5. P. J. Schuck, D. P. Fromm, A. Sundaramurthy, G. S. Kino, and W. E. Moerner, “Improving the mismatch between light and nanoscale objects with gold bowtie nanoantennas,” Phys. Rev. Lett. 94, 017402 (2005).
    [CrossRef] [PubMed]
  6. P. Mühlschlegel, H.-J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science 308, 1607-1609 (2005).
    [CrossRef] [PubMed]
  7. A. Hohenau, J. R. Krenn, S. G. Rodrigo, L. Martin-Moreno, F. Garcia-Vidal, J. Beermann, and S. I. Bozhevolnyi, “Spectroscopy and nonlinear microscopy of gold nanoparticle arrays on gold films,” Phys. Rev. B 75, 085104 (2007).
    [CrossRef]
  8. A. K. Sarychev and V. M. Shalaev, “Electromagnetic field fluctuations and optical nonlinearities in metal-dielectric composites,” Phys. Rep. 335, 275-371 (2000).
    [CrossRef]
  9. S. I. Bozhevolnyi, J. Beermann, and V. Coello, “Direct observation of localized second-harmonic enhancement in random metal nanostructures,” Phys. Rev. Lett. 90, 197403 (2003).
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  10. A. Gopinath, S. V. Boriskina, B. M. Reinhard, and L. Dal Negro, “Deterministic aperiodic arrays of metal nanoparticles for surface-enhanced Raman scattering (SERS),” Opt. Express 17, 3741-3753 (2009).
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    [CrossRef]
  12. A. Mooradian, “Photoluminescence of metals,” Phys. Rev. Lett. 22, 185-187 (1969).
    [CrossRef]
  13. G. T. Boyd, Z. H. Yu, and Y. R. Shen, “Photoinduced luminescence from the noble metals and its enhancement on roughened surfaces,” Phys. Rev. B 33, 7923-7936 (1986).
    [CrossRef]
  14. M. R. Beversluis, A. Bouhelier, and L. Novotny, “Continuum generation from single gold nanostructures through near-field mediated intraband transitions,” Phys. Rev. B 68, 115433 (2003).
    [CrossRef]
  15. J. Beermann and S. I. Bozhevolnyi, “Two-photon luminescence microscopy of field enhancement at gold nanoparticles,” Phys. Status Solidi C 2, 3983-3987 (2005).
    [CrossRef]
  16. J. Beermann, I. P. Radko, A. Boltasseva, and S. I. Bozhevolnyi, “Localized field enhancements in fractal shaped periodic metal nanostructures,” Opt. Express 15, 15234-15241 (2007).
    [CrossRef] [PubMed]
  17. J. Beermann, A. B. Evlyukhin, A. Boltasseva, and S. I. Bozhevolnyi, “Nonlinear microscopy of localized field enhancements in fractal shaped periodic metal nanostructures,” J. Opt. Soc. Am. B 25, 1585-1592 (2008).
    [CrossRef]
  18. J. Beermann, S. M. Novikov, K. Leosson, and S. I. Bozhevolnyi, “Surface enhanced Raman microscopy with metal nanoparticle arrays,” J. Opt. A, Pure Appl. Opt. 11, 075004 (2009).
    [CrossRef]
  19. J. Beermann, S. M. Novikov, K. Leosson, and S. I. Bozhevolnyi, “Surface enhanced Raman imaging: periodic arrays and individual metal nanoparticles,” Opt. Express 17, 12698-12705 (2009).
    [CrossRef] [PubMed]
  20. K. Falconer, Fractal Geometry: Mathematical Foundations and Application, 2nd ed. (Wiley, 2003).
    [CrossRef]
  21. J. Beermann and S. I. Bozhevolnyi, “Microscopy of localized second-harmonic enhancement in random metal nanostructures,” Phys. Rev. B 69, 155429 (2004).
    [CrossRef]
  22. T. Søndergaard, J. Beermann, A. E. Boltasseva, and S. I. Bozhevolnyi, “Slow-plasmon resonant-nanostrip antennas: analysis and demonstration,” Phys. Rev. B 77, 115420 (2008).
    [CrossRef]
  23. J. Beermann, S. M. Novikov, T. Søndergaard, A. E. Boltasseva, and S. I. Bozhevolnyi, “Two-photon mapping of localized field enhancements in thin nanostrip antennas,” Opt. Express 16, 17302-17309 (2008).
    [CrossRef] [PubMed]
  24. J. Zhao, L. Jensen, J. Sung, S. Zou, G. C. Schatz, and R. P. Van Duyne, “Interaction of plasmon and molecular resonances for Rhodamine 6G adsorbed on silver nanoparticles,” J. Am. Chem. Soc. 129, 7647-7656 (2007).
    [CrossRef] [PubMed]
  25. I. P. Radko, S. I. Bozhevolnyi, A. B. Evlyukhin, and A. Boltasseva, “Surface plasmon polariton beam focusing with parabolic nanoparticle chains,” Opt. Express 15, 6576-6582 (2007).
    [CrossRef] [PubMed]
  26. S. A. Maier, M. D. Friedman, P. E. Barclay, and O. Painter, “Experimental demonstration of fiber-accessible metal nanoparticle plasmon waveguides for planar energy guiding and sensing,” Appl. Phys. Lett. 86, 071103 (2005).
    [CrossRef]
  27. C. Bai and C. Wang, Single Molecule Chemistry and Physics (Springer, 2006).
  28. E. C. Le Ru and P. G. Etchegoin, “Rigorous justification of the |E|4 enhancement factor in surface enhanced Raman spectroscopy,” Chem. Phys. Lett. 423, 63-66 (2006).
    [CrossRef]
  29. A. Otto, “Surface-enhanced Raman scattering of adsorbates,” J. Raman Spectrosc. 22, 743-752 (1991).
    [CrossRef]
  30. D. P. Fromm, A. Sundaramurthy, A. Kinkhabwala, P. J. Schuck, G. S. Kino, and W. E. Moerner, “Exploring the chemical enhancement for surface-enhanced Raman scattering with Au bowtie nanoantennas,” J. Chem. Phys. 124, 061101 (2006).
    [CrossRef]

2009

2008

2007

A. Hohenau, J. R. Krenn, S. G. Rodrigo, L. Martin-Moreno, F. Garcia-Vidal, J. Beermann, and S. I. Bozhevolnyi, “Spectroscopy and nonlinear microscopy of gold nanoparticle arrays on gold films,” Phys. Rev. B 75, 085104 (2007).
[CrossRef]

J. Zhao, L. Jensen, J. Sung, S. Zou, G. C. Schatz, and R. P. Van Duyne, “Interaction of plasmon and molecular resonances for Rhodamine 6G adsorbed on silver nanoparticles,” J. Am. Chem. Soc. 129, 7647-7656 (2007).
[CrossRef] [PubMed]

I. P. Radko, S. I. Bozhevolnyi, A. B. Evlyukhin, and A. Boltasseva, “Surface plasmon polariton beam focusing with parabolic nanoparticle chains,” Opt. Express 15, 6576-6582 (2007).
[CrossRef] [PubMed]

J. Beermann, I. P. Radko, A. Boltasseva, and S. I. Bozhevolnyi, “Localized field enhancements in fractal shaped periodic metal nanostructures,” Opt. Express 15, 15234-15241 (2007).
[CrossRef] [PubMed]

2006

E. C. Le Ru and P. G. Etchegoin, “Rigorous justification of the |E|4 enhancement factor in surface enhanced Raman spectroscopy,” Chem. Phys. Lett. 423, 63-66 (2006).
[CrossRef]

D. P. Fromm, A. Sundaramurthy, A. Kinkhabwala, P. J. Schuck, G. S. Kino, and W. E. Moerner, “Exploring the chemical enhancement for surface-enhanced Raman scattering with Au bowtie nanoantennas,” J. Chem. Phys. 124, 061101 (2006).
[CrossRef]

2005

P. J. Schuck, D. P. Fromm, A. Sundaramurthy, G. S. Kino, and W. E. Moerner, “Improving the mismatch between light and nanoscale objects with gold bowtie nanoantennas,” Phys. Rev. Lett. 94, 017402 (2005).
[CrossRef] [PubMed]

P. Mühlschlegel, H.-J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science 308, 1607-1609 (2005).
[CrossRef] [PubMed]

S. A. Maier, M. D. Friedman, P. E. Barclay, and O. Painter, “Experimental demonstration of fiber-accessible metal nanoparticle plasmon waveguides for planar energy guiding and sensing,” Appl. Phys. Lett. 86, 071103 (2005).
[CrossRef]

J. Beermann and S. I. Bozhevolnyi, “Two-photon luminescence microscopy of field enhancement at gold nanoparticles,” Phys. Status Solidi C 2, 3983-3987 (2005).
[CrossRef]

2004

J. Beermann and S. I. Bozhevolnyi, “Microscopy of localized second-harmonic enhancement in random metal nanostructures,” Phys. Rev. B 69, 155429 (2004).
[CrossRef]

2003

M. R. Beversluis, A. Bouhelier, and L. Novotny, “Continuum generation from single gold nanostructures through near-field mediated intraband transitions,” Phys. Rev. B 68, 115433 (2003).
[CrossRef]

S. I. Bozhevolnyi, J. Beermann, and V. Coello, “Direct observation of localized second-harmonic enhancement in random metal nanostructures,” Phys. Rev. Lett. 90, 197403 (2003).
[CrossRef] [PubMed]

2002

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, “Surface-enhanced Raman scattering and biophysics,” J. Phys. Condens. Matter 14, R597-R624 (2002).
[CrossRef]

2000

A. K. Sarychev and V. M. Shalaev, “Electromagnetic field fluctuations and optical nonlinearities in metal-dielectric composites,” Phys. Rep. 335, 275-371 (2000).
[CrossRef]

1999

C. Even, S. Russ, V. Repain, P. Pieranski, and B. Sapoval, “Localizations in fractal drums: an experimental study,” Phys. Rev. Lett. 83, 726-729 (1999).
[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]

1991

A. Otto, “Surface-enhanced Raman scattering of adsorbates,” J. Raman Spectrosc. 22, 743-752 (1991).
[CrossRef]

1986

G. T. Boyd, Z. H. Yu, and Y. R. Shen, “Photoinduced luminescence from the noble metals and its enhancement on roughened surfaces,” Phys. Rev. B 33, 7923-7936 (1986).
[CrossRef]

1984

G. T. Boyd, Th. Rasing, J. R. R. Leite, and Y. R. Shen, “Local-field enhancement on rough surfaces of metals, semimetals, and semiconductors with the use of optical second-harmonic generation,” Phys. Rev. B 30, 519-526 (1984).
[CrossRef]

1969

A. Mooradian, “Photoluminescence of metals,” Phys. Rev. Lett. 22, 185-187 (1969).
[CrossRef]

Bai, C.

C. Bai and C. Wang, Single Molecule Chemistry and Physics (Springer, 2006).

Barclay, P. E.

S. A. Maier, M. D. Friedman, P. E. Barclay, and O. Painter, “Experimental demonstration of fiber-accessible metal nanoparticle plasmon waveguides for planar energy guiding and sensing,” Appl. Phys. Lett. 86, 071103 (2005).
[CrossRef]

Beermann, J.

J. Beermann, S. M. Novikov, K. Leosson, and S. I. Bozhevolnyi, “Surface enhanced Raman imaging: periodic arrays and individual metal nanoparticles,” Opt. Express 17, 12698-12705 (2009).
[CrossRef] [PubMed]

J. Beermann, S. M. Novikov, K. Leosson, and S. I. Bozhevolnyi, “Surface enhanced Raman microscopy with metal nanoparticle arrays,” J. Opt. A, Pure Appl. Opt. 11, 075004 (2009).
[CrossRef]

J. Beermann, A. B. Evlyukhin, A. Boltasseva, and S. I. Bozhevolnyi, “Nonlinear microscopy of localized field enhancements in fractal shaped periodic metal nanostructures,” J. Opt. Soc. Am. B 25, 1585-1592 (2008).
[CrossRef]

J. Beermann, S. M. Novikov, T. Søndergaard, A. E. Boltasseva, and S. I. Bozhevolnyi, “Two-photon mapping of localized field enhancements in thin nanostrip antennas,” Opt. Express 16, 17302-17309 (2008).
[CrossRef] [PubMed]

T. Søndergaard, J. Beermann, A. E. Boltasseva, and S. I. Bozhevolnyi, “Slow-plasmon resonant-nanostrip antennas: analysis and demonstration,” Phys. Rev. B 77, 115420 (2008).
[CrossRef]

A. Hohenau, J. R. Krenn, S. G. Rodrigo, L. Martin-Moreno, F. Garcia-Vidal, J. Beermann, and S. I. Bozhevolnyi, “Spectroscopy and nonlinear microscopy of gold nanoparticle arrays on gold films,” Phys. Rev. B 75, 085104 (2007).
[CrossRef]

J. Beermann, I. P. Radko, A. Boltasseva, and S. I. Bozhevolnyi, “Localized field enhancements in fractal shaped periodic metal nanostructures,” Opt. Express 15, 15234-15241 (2007).
[CrossRef] [PubMed]

J. Beermann and S. I. Bozhevolnyi, “Two-photon luminescence microscopy of field enhancement at gold nanoparticles,” Phys. Status Solidi C 2, 3983-3987 (2005).
[CrossRef]

J. Beermann and S. I. Bozhevolnyi, “Microscopy of localized second-harmonic enhancement in random metal nanostructures,” Phys. Rev. B 69, 155429 (2004).
[CrossRef]

S. I. Bozhevolnyi, J. Beermann, and V. Coello, “Direct observation of localized second-harmonic enhancement in random metal nanostructures,” Phys. Rev. Lett. 90, 197403 (2003).
[CrossRef] [PubMed]

Beversluis, M. R.

M. R. Beversluis, A. Bouhelier, and L. Novotny, “Continuum generation from single gold nanostructures through near-field mediated intraband transitions,” Phys. Rev. B 68, 115433 (2003).
[CrossRef]

Boltasseva, A.

Boltasseva, A. E.

J. Beermann, S. M. Novikov, T. Søndergaard, A. E. Boltasseva, and S. I. Bozhevolnyi, “Two-photon mapping of localized field enhancements in thin nanostrip antennas,” Opt. Express 16, 17302-17309 (2008).
[CrossRef] [PubMed]

T. Søndergaard, J. Beermann, A. E. Boltasseva, and S. I. Bozhevolnyi, “Slow-plasmon resonant-nanostrip antennas: analysis and demonstration,” Phys. Rev. B 77, 115420 (2008).
[CrossRef]

Boriskina, S. V.

Bouhelier, A.

M. R. Beversluis, A. Bouhelier, and L. Novotny, “Continuum generation from single gold nanostructures through near-field mediated intraband transitions,” Phys. Rev. B 68, 115433 (2003).
[CrossRef]

Boyd, G. T.

G. T. Boyd, Z. H. Yu, and Y. R. Shen, “Photoinduced luminescence from the noble metals and its enhancement on roughened surfaces,” Phys. Rev. B 33, 7923-7936 (1986).
[CrossRef]

G. T. Boyd, Th. Rasing, J. R. R. Leite, and Y. R. Shen, “Local-field enhancement on rough surfaces of metals, semimetals, and semiconductors with the use of optical second-harmonic generation,” Phys. Rev. B 30, 519-526 (1984).
[CrossRef]

Bozhevolnyi, S. I.

J. Beermann, S. M. Novikov, K. Leosson, and S. I. Bozhevolnyi, “Surface enhanced Raman imaging: periodic arrays and individual metal nanoparticles,” Opt. Express 17, 12698-12705 (2009).
[CrossRef] [PubMed]

J. Beermann, S. M. Novikov, K. Leosson, and S. I. Bozhevolnyi, “Surface enhanced Raman microscopy with metal nanoparticle arrays,” J. Opt. A, Pure Appl. Opt. 11, 075004 (2009).
[CrossRef]

J. Beermann, A. B. Evlyukhin, A. Boltasseva, and S. I. Bozhevolnyi, “Nonlinear microscopy of localized field enhancements in fractal shaped periodic metal nanostructures,” J. Opt. Soc. Am. B 25, 1585-1592 (2008).
[CrossRef]

J. Beermann, S. M. Novikov, T. Søndergaard, A. E. Boltasseva, and S. I. Bozhevolnyi, “Two-photon mapping of localized field enhancements in thin nanostrip antennas,” Opt. Express 16, 17302-17309 (2008).
[CrossRef] [PubMed]

T. Søndergaard, J. Beermann, A. E. Boltasseva, and S. I. Bozhevolnyi, “Slow-plasmon resonant-nanostrip antennas: analysis and demonstration,” Phys. Rev. B 77, 115420 (2008).
[CrossRef]

A. Hohenau, J. R. Krenn, S. G. Rodrigo, L. Martin-Moreno, F. Garcia-Vidal, J. Beermann, and S. I. Bozhevolnyi, “Spectroscopy and nonlinear microscopy of gold nanoparticle arrays on gold films,” Phys. Rev. B 75, 085104 (2007).
[CrossRef]

J. Beermann, I. P. Radko, A. Boltasseva, and S. I. Bozhevolnyi, “Localized field enhancements in fractal shaped periodic metal nanostructures,” Opt. Express 15, 15234-15241 (2007).
[CrossRef] [PubMed]

I. P. Radko, S. I. Bozhevolnyi, A. B. Evlyukhin, and A. Boltasseva, “Surface plasmon polariton beam focusing with parabolic nanoparticle chains,” Opt. Express 15, 6576-6582 (2007).
[CrossRef] [PubMed]

J. Beermann and S. I. Bozhevolnyi, “Two-photon luminescence microscopy of field enhancement at gold nanoparticles,” Phys. Status Solidi C 2, 3983-3987 (2005).
[CrossRef]

J. Beermann and S. I. Bozhevolnyi, “Microscopy of localized second-harmonic enhancement in random metal nanostructures,” Phys. Rev. B 69, 155429 (2004).
[CrossRef]

S. I. Bozhevolnyi, J. Beermann, and V. Coello, “Direct observation of localized second-harmonic enhancement in random metal nanostructures,” Phys. Rev. Lett. 90, 197403 (2003).
[CrossRef] [PubMed]

Coello, V.

S. I. Bozhevolnyi, J. Beermann, and V. Coello, “Direct observation of localized second-harmonic enhancement in random metal nanostructures,” Phys. Rev. Lett. 90, 197403 (2003).
[CrossRef] [PubMed]

Dal Negro, L.

Dasari, R. R.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, “Surface-enhanced Raman scattering and biophysics,” J. Phys. Condens. Matter 14, R597-R624 (2002).
[CrossRef]

Eisler, H. -J.

P. Mühlschlegel, H.-J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science 308, 1607-1609 (2005).
[CrossRef] [PubMed]

Etchegoin, P. G.

E. C. Le Ru and P. G. Etchegoin, “Rigorous justification of the |E|4 enhancement factor in surface enhanced Raman spectroscopy,” Chem. Phys. Lett. 423, 63-66 (2006).
[CrossRef]

Even, C.

C. Even, S. Russ, V. Repain, P. Pieranski, and B. Sapoval, “Localizations in fractal drums: an experimental study,” Phys. Rev. Lett. 83, 726-729 (1999).
[CrossRef]

Evlyukhin, A. B.

Falconer, K.

K. Falconer, Fractal Geometry: Mathematical Foundations and Application, 2nd ed. (Wiley, 2003).
[CrossRef]

Feld, M. S.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, “Surface-enhanced Raman scattering and biophysics,” J. Phys. Condens. Matter 14, R597-R624 (2002).
[CrossRef]

Friedman, M. D.

S. A. Maier, M. D. Friedman, P. E. Barclay, and O. Painter, “Experimental demonstration of fiber-accessible metal nanoparticle plasmon waveguides for planar energy guiding and sensing,” Appl. Phys. Lett. 86, 071103 (2005).
[CrossRef]

Fromm, D. P.

D. P. Fromm, A. Sundaramurthy, A. Kinkhabwala, P. J. Schuck, G. S. Kino, and W. E. Moerner, “Exploring the chemical enhancement for surface-enhanced Raman scattering with Au bowtie nanoantennas,” J. Chem. Phys. 124, 061101 (2006).
[CrossRef]

P. J. Schuck, D. P. Fromm, A. Sundaramurthy, G. S. Kino, and W. E. Moerner, “Improving the mismatch between light and nanoscale objects with gold bowtie nanoantennas,” Phys. Rev. Lett. 94, 017402 (2005).
[CrossRef] [PubMed]

Garcia-Vidal, F.

A. Hohenau, J. R. Krenn, S. G. Rodrigo, L. Martin-Moreno, F. Garcia-Vidal, J. Beermann, and S. I. Bozhevolnyi, “Spectroscopy and nonlinear microscopy of gold nanoparticle arrays on gold films,” Phys. Rev. B 75, 085104 (2007).
[CrossRef]

George, T. F.

V. M. Markel and T. F. George, Optics of Nanostructured Materials (Wiley, 2001).

Gopinath, A.

Hecht, B.

P. Mühlschlegel, H.-J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science 308, 1607-1609 (2005).
[CrossRef] [PubMed]

Hohenau, A.

A. Hohenau, J. R. Krenn, S. G. Rodrigo, L. Martin-Moreno, F. Garcia-Vidal, J. Beermann, and S. I. Bozhevolnyi, “Spectroscopy and nonlinear microscopy of gold nanoparticle arrays on gold films,” Phys. Rev. B 75, 085104 (2007).
[CrossRef]

Itzkan, I.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, “Surface-enhanced Raman scattering and biophysics,” J. Phys. Condens. Matter 14, R597-R624 (2002).
[CrossRef]

Jensen, L.

J. Zhao, L. Jensen, J. Sung, S. Zou, G. C. Schatz, and R. P. Van Duyne, “Interaction of plasmon and molecular resonances for Rhodamine 6G adsorbed on silver nanoparticles,” J. Am. Chem. Soc. 129, 7647-7656 (2007).
[CrossRef] [PubMed]

Kinkhabwala, A.

D. P. Fromm, A. Sundaramurthy, A. Kinkhabwala, P. J. Schuck, G. S. Kino, and W. E. Moerner, “Exploring the chemical enhancement for surface-enhanced Raman scattering with Au bowtie nanoantennas,” J. Chem. Phys. 124, 061101 (2006).
[CrossRef]

Kino, G. S.

D. P. Fromm, A. Sundaramurthy, A. Kinkhabwala, P. J. Schuck, G. S. Kino, and W. E. Moerner, “Exploring the chemical enhancement for surface-enhanced Raman scattering with Au bowtie nanoantennas,” J. Chem. Phys. 124, 061101 (2006).
[CrossRef]

P. J. Schuck, D. P. Fromm, A. Sundaramurthy, G. S. Kino, and W. E. Moerner, “Improving the mismatch between light and nanoscale objects with gold bowtie nanoantennas,” Phys. Rev. Lett. 94, 017402 (2005).
[CrossRef] [PubMed]

Kneipp, H.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, “Surface-enhanced Raman scattering and biophysics,” J. Phys. Condens. Matter 14, R597-R624 (2002).
[CrossRef]

Kneipp, K.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, “Surface-enhanced Raman scattering and biophysics,” J. Phys. Condens. Matter 14, R597-R624 (2002).
[CrossRef]

Krenn, J. R.

A. Hohenau, J. R. Krenn, S. G. Rodrigo, L. Martin-Moreno, F. Garcia-Vidal, J. Beermann, and S. I. Bozhevolnyi, “Spectroscopy and nonlinear microscopy of gold nanoparticle arrays on gold films,” Phys. Rev. B 75, 085104 (2007).
[CrossRef]

Le Ru, E. C.

E. C. Le Ru and P. G. Etchegoin, “Rigorous justification of the |E|4 enhancement factor in surface enhanced Raman spectroscopy,” Chem. Phys. Lett. 423, 63-66 (2006).
[CrossRef]

Leite, J. R. R.

G. T. Boyd, Th. Rasing, J. R. R. Leite, and Y. R. Shen, “Local-field enhancement on rough surfaces of metals, semimetals, and semiconductors with the use of optical second-harmonic generation,” Phys. Rev. B 30, 519-526 (1984).
[CrossRef]

Leosson, K.

J. Beermann, S. M. Novikov, K. Leosson, and S. I. Bozhevolnyi, “Surface enhanced Raman imaging: periodic arrays and individual metal nanoparticles,” Opt. Express 17, 12698-12705 (2009).
[CrossRef] [PubMed]

J. Beermann, S. M. Novikov, K. Leosson, and S. I. Bozhevolnyi, “Surface enhanced Raman microscopy with metal nanoparticle arrays,” J. Opt. A, Pure Appl. Opt. 11, 075004 (2009).
[CrossRef]

Maier, S. A.

S. A. Maier, M. D. Friedman, P. E. Barclay, and O. Painter, “Experimental demonstration of fiber-accessible metal nanoparticle plasmon waveguides for planar energy guiding and sensing,” Appl. Phys. Lett. 86, 071103 (2005).
[CrossRef]

Markel, V. M.

V. M. Markel and T. F. George, Optics of Nanostructured Materials (Wiley, 2001).

Martin, O. J. F.

P. Mühlschlegel, H.-J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science 308, 1607-1609 (2005).
[CrossRef] [PubMed]

Martin-Moreno, L.

A. Hohenau, J. R. Krenn, S. G. Rodrigo, L. Martin-Moreno, F. Garcia-Vidal, J. Beermann, and S. I. Bozhevolnyi, “Spectroscopy and nonlinear microscopy of gold nanoparticle arrays on gold films,” Phys. Rev. B 75, 085104 (2007).
[CrossRef]

Moerner, W. E.

D. P. Fromm, A. Sundaramurthy, A. Kinkhabwala, P. J. Schuck, G. S. Kino, and W. E. Moerner, “Exploring the chemical enhancement for surface-enhanced Raman scattering with Au bowtie nanoantennas,” J. Chem. Phys. 124, 061101 (2006).
[CrossRef]

P. J. Schuck, D. P. Fromm, A. Sundaramurthy, G. S. Kino, and W. E. Moerner, “Improving the mismatch between light and nanoscale objects with gold bowtie nanoantennas,” Phys. Rev. Lett. 94, 017402 (2005).
[CrossRef] [PubMed]

Mooradian, A.

A. Mooradian, “Photoluminescence of metals,” Phys. Rev. Lett. 22, 185-187 (1969).
[CrossRef]

Mühlschlegel, P.

P. Mühlschlegel, H.-J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science 308, 1607-1609 (2005).
[CrossRef] [PubMed]

Novikov, S. M.

Novotny, L.

M. R. Beversluis, A. Bouhelier, and L. Novotny, “Continuum generation from single gold nanostructures through near-field mediated intraband transitions,” Phys. Rev. B 68, 115433 (2003).
[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]

Otto, A.

A. Otto, “Surface-enhanced Raman scattering of adsorbates,” J. Raman Spectrosc. 22, 743-752 (1991).
[CrossRef]

Painter, O.

S. A. Maier, M. D. Friedman, P. E. Barclay, and O. Painter, “Experimental demonstration of fiber-accessible metal nanoparticle plasmon waveguides for planar energy guiding and sensing,” Appl. Phys. Lett. 86, 071103 (2005).
[CrossRef]

Pieranski, P.

C. Even, S. Russ, V. Repain, P. Pieranski, and B. Sapoval, “Localizations in fractal drums: an experimental study,” Phys. Rev. Lett. 83, 726-729 (1999).
[CrossRef]

Pohl, D. W.

P. Mühlschlegel, H.-J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science 308, 1607-1609 (2005).
[CrossRef] [PubMed]

Radko, I. P.

Rasing, Th.

G. T. Boyd, Th. Rasing, J. R. R. Leite, and Y. R. Shen, “Local-field enhancement on rough surfaces of metals, semimetals, and semiconductors with the use of optical second-harmonic generation,” Phys. Rev. B 30, 519-526 (1984).
[CrossRef]

Reinhard, B. M.

Repain, V.

C. Even, S. Russ, V. Repain, P. Pieranski, and B. Sapoval, “Localizations in fractal drums: an experimental study,” Phys. Rev. Lett. 83, 726-729 (1999).
[CrossRef]

Rodrigo, S. G.

A. Hohenau, J. R. Krenn, S. G. Rodrigo, L. Martin-Moreno, F. Garcia-Vidal, J. Beermann, and S. I. Bozhevolnyi, “Spectroscopy and nonlinear microscopy of gold nanoparticle arrays on gold films,” Phys. Rev. B 75, 085104 (2007).
[CrossRef]

Russ, S.

C. Even, S. Russ, V. Repain, P. Pieranski, and B. Sapoval, “Localizations in fractal drums: an experimental study,” Phys. Rev. Lett. 83, 726-729 (1999).
[CrossRef]

Sánchez, E. J.

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]

Sapoval, B.

C. Even, S. Russ, V. Repain, P. Pieranski, and B. Sapoval, “Localizations in fractal drums: an experimental study,” Phys. Rev. Lett. 83, 726-729 (1999).
[CrossRef]

Sarychev, A. K.

A. K. Sarychev and V. M. Shalaev, “Electromagnetic field fluctuations and optical nonlinearities in metal-dielectric composites,” Phys. Rep. 335, 275-371 (2000).
[CrossRef]

Schatz, G. C.

J. Zhao, L. Jensen, J. Sung, S. Zou, G. C. Schatz, and R. P. Van Duyne, “Interaction of plasmon and molecular resonances for Rhodamine 6G adsorbed on silver nanoparticles,” J. Am. Chem. Soc. 129, 7647-7656 (2007).
[CrossRef] [PubMed]

Schuck, P. J.

D. P. Fromm, A. Sundaramurthy, A. Kinkhabwala, P. J. Schuck, G. S. Kino, and W. E. Moerner, “Exploring the chemical enhancement for surface-enhanced Raman scattering with Au bowtie nanoantennas,” J. Chem. Phys. 124, 061101 (2006).
[CrossRef]

P. J. Schuck, D. P. Fromm, A. Sundaramurthy, G. S. Kino, and W. E. Moerner, “Improving the mismatch between light and nanoscale objects with gold bowtie nanoantennas,” Phys. Rev. Lett. 94, 017402 (2005).
[CrossRef] [PubMed]

Shalaev, V. M.

A. K. Sarychev and V. M. Shalaev, “Electromagnetic field fluctuations and optical nonlinearities in metal-dielectric composites,” Phys. Rep. 335, 275-371 (2000).
[CrossRef]

Shen, Y. R.

G. T. Boyd, Z. H. Yu, and Y. R. Shen, “Photoinduced luminescence from the noble metals and its enhancement on roughened surfaces,” Phys. Rev. B 33, 7923-7936 (1986).
[CrossRef]

G. T. Boyd, Th. Rasing, J. R. R. Leite, and Y. R. Shen, “Local-field enhancement on rough surfaces of metals, semimetals, and semiconductors with the use of optical second-harmonic generation,” Phys. Rev. B 30, 519-526 (1984).
[CrossRef]

Søndergaard, T.

J. Beermann, S. M. Novikov, T. Søndergaard, A. E. Boltasseva, and S. I. Bozhevolnyi, “Two-photon mapping of localized field enhancements in thin nanostrip antennas,” Opt. Express 16, 17302-17309 (2008).
[CrossRef] [PubMed]

T. Søndergaard, J. Beermann, A. E. Boltasseva, and S. I. Bozhevolnyi, “Slow-plasmon resonant-nanostrip antennas: analysis and demonstration,” Phys. Rev. B 77, 115420 (2008).
[CrossRef]

Sundaramurthy, A.

D. P. Fromm, A. Sundaramurthy, A. Kinkhabwala, P. J. Schuck, G. S. Kino, and W. E. Moerner, “Exploring the chemical enhancement for surface-enhanced Raman scattering with Au bowtie nanoantennas,” J. Chem. Phys. 124, 061101 (2006).
[CrossRef]

P. J. Schuck, D. P. Fromm, A. Sundaramurthy, G. S. Kino, and W. E. Moerner, “Improving the mismatch between light and nanoscale objects with gold bowtie nanoantennas,” Phys. Rev. Lett. 94, 017402 (2005).
[CrossRef] [PubMed]

Sung, J.

J. Zhao, L. Jensen, J. Sung, S. Zou, G. C. Schatz, and R. P. Van Duyne, “Interaction of plasmon and molecular resonances for Rhodamine 6G adsorbed on silver nanoparticles,” J. Am. Chem. Soc. 129, 7647-7656 (2007).
[CrossRef] [PubMed]

Van Duyne, R. P.

J. Zhao, L. Jensen, J. Sung, S. Zou, G. C. Schatz, and R. P. Van Duyne, “Interaction of plasmon and molecular resonances for Rhodamine 6G adsorbed on silver nanoparticles,” J. Am. Chem. Soc. 129, 7647-7656 (2007).
[CrossRef] [PubMed]

Wang, C.

C. Bai and C. Wang, Single Molecule Chemistry and Physics (Springer, 2006).

Xie, X. S.

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]

Yu, Z. H.

G. T. Boyd, Z. H. Yu, and Y. R. Shen, “Photoinduced luminescence from the noble metals and its enhancement on roughened surfaces,” Phys. Rev. B 33, 7923-7936 (1986).
[CrossRef]

Zhao, J.

J. Zhao, L. Jensen, J. Sung, S. Zou, G. C. Schatz, and R. P. Van Duyne, “Interaction of plasmon and molecular resonances for Rhodamine 6G adsorbed on silver nanoparticles,” J. Am. Chem. Soc. 129, 7647-7656 (2007).
[CrossRef] [PubMed]

Zou, S.

J. Zhao, L. Jensen, J. Sung, S. Zou, G. C. Schatz, and R. P. Van Duyne, “Interaction of plasmon and molecular resonances for Rhodamine 6G adsorbed on silver nanoparticles,” J. Am. Chem. Soc. 129, 7647-7656 (2007).
[CrossRef] [PubMed]

Appl. Phys. Lett.

S. A. Maier, M. D. Friedman, P. E. Barclay, and O. Painter, “Experimental demonstration of fiber-accessible metal nanoparticle plasmon waveguides for planar energy guiding and sensing,” Appl. Phys. Lett. 86, 071103 (2005).
[CrossRef]

Chem. Phys. Lett.

E. C. Le Ru and P. G. Etchegoin, “Rigorous justification of the |E|4 enhancement factor in surface enhanced Raman spectroscopy,” Chem. Phys. Lett. 423, 63-66 (2006).
[CrossRef]

J. Am. Chem. Soc.

J. Zhao, L. Jensen, J. Sung, S. Zou, G. C. Schatz, and R. P. Van Duyne, “Interaction of plasmon and molecular resonances for Rhodamine 6G adsorbed on silver nanoparticles,” J. Am. Chem. Soc. 129, 7647-7656 (2007).
[CrossRef] [PubMed]

J. Chem. Phys.

D. P. Fromm, A. Sundaramurthy, A. Kinkhabwala, P. J. Schuck, G. S. Kino, and W. E. Moerner, “Exploring the chemical enhancement for surface-enhanced Raman scattering with Au bowtie nanoantennas,” J. Chem. Phys. 124, 061101 (2006).
[CrossRef]

J. Opt. A, Pure Appl. Opt.

J. Beermann, S. M. Novikov, K. Leosson, and S. I. Bozhevolnyi, “Surface enhanced Raman microscopy with metal nanoparticle arrays,” J. Opt. A, Pure Appl. Opt. 11, 075004 (2009).
[CrossRef]

J. Opt. Soc. Am. B

J. Phys. Condens. Matter

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, “Surface-enhanced Raman scattering and biophysics,” J. Phys. Condens. Matter 14, R597-R624 (2002).
[CrossRef]

J. Raman Spectrosc.

A. Otto, “Surface-enhanced Raman scattering of adsorbates,” J. Raman Spectrosc. 22, 743-752 (1991).
[CrossRef]

Opt. Express

Phys. Rep.

A. K. Sarychev and V. M. Shalaev, “Electromagnetic field fluctuations and optical nonlinearities in metal-dielectric composites,” Phys. Rep. 335, 275-371 (2000).
[CrossRef]

Phys. Rev. B

G. T. Boyd, Th. Rasing, J. R. R. Leite, and Y. R. Shen, “Local-field enhancement on rough surfaces of metals, semimetals, and semiconductors with the use of optical second-harmonic generation,” Phys. Rev. B 30, 519-526 (1984).
[CrossRef]

G. T. Boyd, Z. H. Yu, and Y. R. Shen, “Photoinduced luminescence from the noble metals and its enhancement on roughened surfaces,” Phys. Rev. B 33, 7923-7936 (1986).
[CrossRef]

M. R. Beversluis, A. Bouhelier, and L. Novotny, “Continuum generation from single gold nanostructures through near-field mediated intraband transitions,” Phys. Rev. B 68, 115433 (2003).
[CrossRef]

A. Hohenau, J. R. Krenn, S. G. Rodrigo, L. Martin-Moreno, F. Garcia-Vidal, J. Beermann, and S. I. Bozhevolnyi, “Spectroscopy and nonlinear microscopy of gold nanoparticle arrays on gold films,” Phys. Rev. B 75, 085104 (2007).
[CrossRef]

J. Beermann and S. I. Bozhevolnyi, “Microscopy of localized second-harmonic enhancement in random metal nanostructures,” Phys. Rev. B 69, 155429 (2004).
[CrossRef]

T. Søndergaard, J. Beermann, A. E. Boltasseva, and S. I. Bozhevolnyi, “Slow-plasmon resonant-nanostrip antennas: analysis and demonstration,” Phys. Rev. B 77, 115420 (2008).
[CrossRef]

Phys. Rev. Lett.

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]

P. J. Schuck, D. P. Fromm, A. Sundaramurthy, G. S. Kino, and W. E. Moerner, “Improving the mismatch between light and nanoscale objects with gold bowtie nanoantennas,” Phys. Rev. Lett. 94, 017402 (2005).
[CrossRef] [PubMed]

S. I. Bozhevolnyi, J. Beermann, and V. Coello, “Direct observation of localized second-harmonic enhancement in random metal nanostructures,” Phys. Rev. Lett. 90, 197403 (2003).
[CrossRef] [PubMed]

C. Even, S. Russ, V. Repain, P. Pieranski, and B. Sapoval, “Localizations in fractal drums: an experimental study,” Phys. Rev. Lett. 83, 726-729 (1999).
[CrossRef]

A. Mooradian, “Photoluminescence of metals,” Phys. Rev. Lett. 22, 185-187 (1969).
[CrossRef]

Phys. Status Solidi C

J. Beermann and S. I. Bozhevolnyi, “Two-photon luminescence microscopy of field enhancement at gold nanoparticles,” Phys. Status Solidi C 2, 3983-3987 (2005).
[CrossRef]

Science

P. Mühlschlegel, H.-J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science 308, 1607-1609 (2005).
[CrossRef] [PubMed]

Other

K. Falconer, Fractal Geometry: Mathematical Foundations and Application, 2nd ed. (Wiley, 2003).
[CrossRef]

V. M. Markel and T. F. George, Optics of Nanostructured Materials (Wiley, 2001).

C. Bai and C. Wang, Single Molecule Chemistry and Physics (Springer, 2006).

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Figures (7)

Fig. 1
Fig. 1

(a) DF image ( 170 × 170 μ m 2 ) of fractal shaped with 100-nm-diameter particles and period 170 nm. The dashed circle indicates the area where the reflection spectra were obtained, while the solid-line rectangle and letters (A–E) point out the areas imaged by Raman microscopy and shown in Figs. 3, 6, respectively. (b) Example of SEM image obtained at the dashed rectangle position in (a) but for the fractal with 80-nm-diameter particles.

Fig. 2
Fig. 2

Relative reflection spectra obtained for fractals with the particle diameters 80, 100, and 120 nm without R6G (solid lines) and with R6G (dotted lines).

Fig. 3
Fig. 3

Raman images ( 20 × 18 μ m 2 ) obtained by mapping the Raman intensity integrated over (a) 606 623 cm 1 and (b) 1468 1614 cm 1 from R6G adsorbed on the fractal array with 100-nm-diameter particles at the area indicated by the solid-line rectangle in Fig. 1a. The white circles indicate positions corresponding to the spectra labeled (a) 1st and (b) 2nd spot in Fig. 4b.

Fig. 4
Fig. 4

(a) Typical Raman spectra obtained from the fractal with 100-nm-diameter particles at positions away from bright spots and a reference spectrum obtained at the smooth gold substrate outside the fractal. (b) Raman spectra obtained at the positions of the first and the second spot indicated in Fig. 3.

Fig. 5
Fig. 5

Relative Raman enhancement estimated by comparing levels at each Raman peak with the levels obtained in the reference spectrum.

Fig. 6
Fig. 6

Raman images obtained by mapping the Raman intensity integrated over 1468 1614 cm 1 from R6G adsorbed on the fractal array with 100-nm-diameter particles. The areas in Figs. 6a, 6b, 6c, 6d, 6e can be recognized at the capital letters A–E in Fig. 1a.

Fig. 7
Fig. 7

(a) Raman image ( 8 × 8 μ m 2 ) obtained by mapping the Raman intensity integrated over 1468 1614 cm 1 from R6G adsorbed on a test sample with 100-nm-diameter particles and a regular 170-nm-periodic square shaped array. (b) Reflection spectrum obtained from the test sample along with (c) Raman spectra obtained from different test-sample areas. (d) Relative Raman enhancement estimated by comparing levels at each Raman peak with the levels obtained in the reference spectrum.

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