Abstract

We study finite-size effects in surface-enhanced Raman scattering (SERS) from molecules adsorbed on small metal particles. Within an electromagnetic description of SERS, the enhancement of the Raman signal originates from the local field of the surface plasmon resonance in a nanoparticle. With decreasing particle sizes, this enhancement is reduced due to the size-dependent Landau damping of the surface plasmon. We show that, in small noble-metal particles, the reduction of interband screening in the surface layer leads to an additional increase in the local field acting on a molecule close to the metal surface. The overall size dependence of Raman signal enhancement is determined by the interplay between Landau damping and underscreening effects. Our calculations, based on a two-region model, show that the role of the surface layer increases for smaller nanoparticle sizes due to a larger volume fraction of the underscreened region.

© 2006 Optical Society of America

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  1. M. Fleischman, P. J. Hendra, and A. J. McQuillan, "Raman spectra of pyridine adsorbed at a silver electrode," Chem. Phys. Lett. 26, 163-166 (1974).
    [CrossRef]
  2. D. L. Jeanmaire and R. P. Van Duyne, "Surface Raman spectroelectrochemistry. Part I. Heterocyclic, aromatic, and aliphatic amines adsorbed on the anodized silver electrode," J. Electroanal. Chem. Interfacial Electrochem. 84, 1-20 (1977).
    [CrossRef]
  3. S. Nie and S. R. Emory, "Probing single molecules and single nanoparticles by surface-enhanced Raman scattering," Science 275, 1102-1106 (1997).
    [CrossRef] [PubMed]
  4. K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. R. Dasari, and M. S. Feld, "Single molecule detection using surface-enhanced Raman scattering (SERS)," Phys. Rev. Lett. 78, 1667-1670 (1997).
    [CrossRef]
  5. M. Moskovits, "Surface roughness and the enhanced intensity of Raman scattering by molecules adsorbed on metals," J. Chem. Phys. 69, 4159-4161 (1978).
    [CrossRef]
  6. M. Kerker, D.-S. Wang, and H. Chew, "Surface enhanced Raman scattering (SERS) by molecules adsorbed at spherical particles: errata," Appl. Opt. 19, 4159-4174 (1980).
    [PubMed]
  7. J. Gersten and A. Nitzan, "Electromagnetic theory of enhanced Raman scattering by molecules adsorbed on rough surfaces," J. Chem. Phys. 73, 3023-3037 (1980).
    [CrossRef]
  8. For a recent review, see G. S. Schatz and R. P. Van Duyne, in Handbook of Vibrational Spectroscopy, J.M.Chalmers and P.R.Griffiths, eds. (Wiley, 2002), p. 1.
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    [CrossRef]
  10. F. J. Adrian, "Charge transfer effects in surface-enhanced Raman scattering," J. Chem. Phys. 77, 5302-5314 (1982).
    [CrossRef]
  11. M. Moskovits, "Surface-enhanced spectroscopy," Rev. Mod. Phys. 57, 783-826 (1985).
    [CrossRef]
  12. A. Otto, I. Mrozek, H. Grabhorn, and W. J. Akermann, "Surface-enhanced Raman scattering," J. Phys.: Condens. Matter 4, 1143-1212 (1992), and references therein.
    [CrossRef]
  13. K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, "Ultrasensitive chemical analysis by Raman spectroscopy," Chem. Rev. (Washington, D.C.) 99, 2957-2976 (1999), and references therein.
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  14. M. Michaels, M. Nirmal, and L. E. Brus, "Surface enhanced Raman spectroscopy of individual rhodamine 6G molecules on large Ag nanocrystals," J. Am. Chem. Soc. 121, 9932-9939 (1999).
    [CrossRef]
  15. A. M. Michaels, J. Jiang, and L. E. Brus, "Ag nanocrystal junctions as the site for surface-enhanced Raman scattering of single rhodamine 6G molecules," J. Phys. Chem. B 104, 11965-11971 (2000).
    [CrossRef]
  16. M. Moskovits, L. Tay, J. Yang, and T. Haslett, "SERS and the single molecule," Top. Appl. Phys. 82, 215-226 (2002).
  17. Z. Wang, S. Pan, T. D. Krauss, H. Du, and L. J. Rothberg, "The structural basis for giant enhancement enabling single-molecule Raman scattering," Proc. Natl. Acad. Sci. U.S.A. 100, 8638-8643 (2004).
    [CrossRef]
  18. M. I. Stockman, L. N. Pandey, and T. F. George, "Inhomogeneous localization of polar eigenmodes in fractals," Phys. Rev. B 53, 2183-2186 (1996).
    [CrossRef]
  19. V. A. Markel, V. M. Shalaev, E. B. Stechel, W. Kim, and R. L. Armstrong, "Small-particle composites. I. Linear optical properties," Phys. Rev. B 53, 2425-2436 (1996).
    [CrossRef]
  20. H. Xu, E. J. Bjerneld, M. Käll, and L. Börjesson, "Spectroscopy of single hemoglobin molecules by surface enhanced Raman scattering," Phys. Rev. Lett. 83, 4357-4360 (1999).
    [CrossRef]
  21. H. Xu, J. Aizpurua, M. Käll, and P. Apell, "Electromagnetic contributions to single-molecule sensitivity in surface-enhanced Raman scattering," Phys. Rev. E 62, 4318-4324 (2000).
    [CrossRef]
  22. K. Li, M. I. Stockman, and D. J. Bergman, "Self-similar chain of metal nanospheres as an efficient nanolens," Phys. Rev. Lett. 91, 227402 (2003).
    [CrossRef] [PubMed]
  23. H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, "Unified treatment of fluorescence and Raman scattering processes near metal surfaces," Phys. Rev. Lett. 93, 243002 (2004).
    [CrossRef]
  24. B. Nikoobakht, J. Wang, and M. A. El-Sayed, "Surface-enhanced Raman scattering of molecules adsorbed on gold nanorods: off-surface plasmon resonance condition," Chem. Phys. Lett. 366, 17-23 (2002).
    [CrossRef]
  25. C. Sönnichsen, T. Franzl, T. Wilk, G. von Plessen, J. Feldmann, O. Wilson, and P. Mulvaney, "Drastic reduction of plasmon damping in gold nanorods," Phys. Rev. Lett. 88, 077402 (2002).
    [CrossRef] [PubMed]
  26. S. J. Oldenburg, S. L. Westcott, R. D. Averitt, and N. J. Halas, "Surface enhanced Raman scattering in the near infrared using metal nanoshell substrates," J. Chem. Phys. 111, 4729-4735 (1999).
    [CrossRef]
  27. J.-Y. Bigot, J. C. Merle, O. Cregut, and A. Daunois, "Electron dynamics in copper metallic nanoparticles probed with femtosecond optical pulses," Phys. Rev. Lett. 75, 4702-4705 (1995).
    [CrossRef] [PubMed]
  28. A. Kawabata and R. Kubo, "Electronic properties of fine metallic particles. II. Plasma resonance absorption," J. Phys. Soc. Jpn. 21, 1765-1772 (1966).
    [CrossRef]
  29. See, e.g., U. Kreibig and M. Vollmer, Optical Properties of Metal Clusters (Springer, 1995).
  30. L. Peyser-Capadona, J. Zheng, J. I. Gonzlez, T.-H. Lee, S. A. Patel, and R. M. Dickson, "Nanoparticle-free single molecule anti-Stokes Raman spectroscopy," Phys. Rev. Lett. 94, 058301 (2005).
    [CrossRef] [PubMed]
  31. B. N. J. Persson and E. Zaremba, "Electron-hole pair production at metal surfaces," Phys. Rev. B 31, 1863-1872 (1985).
    [CrossRef]
  32. A. Liebsch, "Surface-plasmon dispersion and size dependence of Mie resonance: silver versus simple metals," Phys. Rev. B 48, 11317-11328 (1993).
    [CrossRef]
  33. V. V. Kresin, "Collective resonances in silver clusters: role of d electrons and the polarization-free surface layer," Phys. Rev. B 51, 1844-1849 (1995).
    [CrossRef]
  34. A. Liebsch and W. L. Schaich, "Influence of a polarizable medium on the nonlocal optical response of a metal surface," Phys. Rev. B 52, 14219-14234 (1995).
    [CrossRef]
  35. C. Voisin, D. Christofilos, N. Del Fatti, F. Vallée, B. Prével, E. Cottancin, J. Lermé, M. Pellarin, and M. Broyer, "Size-dependent electron-electron interactions in metal nanoparticles," Phys. Rev. Lett. 85, 2200-2203 (2000).
    [CrossRef] [PubMed]
  36. C. Lopez-Bastidas, J. A. Maytorena, and A. Liebsch, "Hot-electron dynamics at noble metal surfaces," Phys. Rev. B 65, 035417 (2002).
    [CrossRef]
  37. N. Nilius, N. Ernst, and H.-J. Freund, "Photon emission spectroscopy of individual oxide-supported silver clusters in a scanning tunneling microscope," Phys. Rev. Lett. 84, 3994-3997 (2000).
    [CrossRef] [PubMed]
  38. A. A. Lushnikov, V. V. Maksimenko, and A. J. Simonov, "Surface plasmon oscillations in layer metal particles," Z. Phys. B 27, 321-324 (1977).
    [CrossRef]
  39. W. Ekardt, "Size-dependent photoabsorption and photoemission of small metal particles," Phys. Rev. B 31, 6360-6370 (1985).
    [CrossRef]
  40. V. N. Pustovit and T. V. Shahbazyan, "Microscopic theory of surface-enhanced Raman scattering in noble-metal nanoparticles," Phys. Rev. B 73, 085408 (2006).
    [CrossRef]
  41. See, e.g., D. A. Long, The Raman Effect (Wiley, 2002).
    [CrossRef]

2006 (1)

V. N. Pustovit and T. V. Shahbazyan, "Microscopic theory of surface-enhanced Raman scattering in noble-metal nanoparticles," Phys. Rev. B 73, 085408 (2006).
[CrossRef]

2005 (1)

L. Peyser-Capadona, J. Zheng, J. I. Gonzlez, T.-H. Lee, S. A. Patel, and R. M. Dickson, "Nanoparticle-free single molecule anti-Stokes Raman spectroscopy," Phys. Rev. Lett. 94, 058301 (2005).
[CrossRef] [PubMed]

2004 (2)

H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, "Unified treatment of fluorescence and Raman scattering processes near metal surfaces," Phys. Rev. Lett. 93, 243002 (2004).
[CrossRef]

Z. Wang, S. Pan, T. D. Krauss, H. Du, and L. J. Rothberg, "The structural basis for giant enhancement enabling single-molecule Raman scattering," Proc. Natl. Acad. Sci. U.S.A. 100, 8638-8643 (2004).
[CrossRef]

2003 (1)

K. Li, M. I. Stockman, and D. J. Bergman, "Self-similar chain of metal nanospheres as an efficient nanolens," Phys. Rev. Lett. 91, 227402 (2003).
[CrossRef] [PubMed]

2002 (4)

C. Lopez-Bastidas, J. A. Maytorena, and A. Liebsch, "Hot-electron dynamics at noble metal surfaces," Phys. Rev. B 65, 035417 (2002).
[CrossRef]

B. Nikoobakht, J. Wang, and M. A. El-Sayed, "Surface-enhanced Raman scattering of molecules adsorbed on gold nanorods: off-surface plasmon resonance condition," Chem. Phys. Lett. 366, 17-23 (2002).
[CrossRef]

C. Sönnichsen, T. Franzl, T. Wilk, G. von Plessen, J. Feldmann, O. Wilson, and P. Mulvaney, "Drastic reduction of plasmon damping in gold nanorods," Phys. Rev. Lett. 88, 077402 (2002).
[CrossRef] [PubMed]

M. Moskovits, L. Tay, J. Yang, and T. Haslett, "SERS and the single molecule," Top. Appl. Phys. 82, 215-226 (2002).

2000 (4)

A. M. Michaels, J. Jiang, and L. E. Brus, "Ag nanocrystal junctions as the site for surface-enhanced Raman scattering of single rhodamine 6G molecules," J. Phys. Chem. B 104, 11965-11971 (2000).
[CrossRef]

H. Xu, J. Aizpurua, M. Käll, and P. Apell, "Electromagnetic contributions to single-molecule sensitivity in surface-enhanced Raman scattering," Phys. Rev. E 62, 4318-4324 (2000).
[CrossRef]

N. Nilius, N. Ernst, and H.-J. Freund, "Photon emission spectroscopy of individual oxide-supported silver clusters in a scanning tunneling microscope," Phys. Rev. Lett. 84, 3994-3997 (2000).
[CrossRef] [PubMed]

C. Voisin, D. Christofilos, N. Del Fatti, F. Vallée, B. Prével, E. Cottancin, J. Lermé, M. Pellarin, and M. Broyer, "Size-dependent electron-electron interactions in metal nanoparticles," Phys. Rev. Lett. 85, 2200-2203 (2000).
[CrossRef] [PubMed]

1999 (4)

H. Xu, E. J. Bjerneld, M. Käll, and L. Börjesson, "Spectroscopy of single hemoglobin molecules by surface enhanced Raman scattering," Phys. Rev. Lett. 83, 4357-4360 (1999).
[CrossRef]

S. J. Oldenburg, S. L. Westcott, R. D. Averitt, and N. J. Halas, "Surface enhanced Raman scattering in the near infrared using metal nanoshell substrates," J. Chem. Phys. 111, 4729-4735 (1999).
[CrossRef]

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, "Ultrasensitive chemical analysis by Raman spectroscopy," Chem. Rev. (Washington, D.C.) 99, 2957-2976 (1999), and references therein.
[CrossRef]

M. Michaels, M. Nirmal, and L. E. Brus, "Surface enhanced Raman spectroscopy of individual rhodamine 6G molecules on large Ag nanocrystals," J. Am. Chem. Soc. 121, 9932-9939 (1999).
[CrossRef]

1997 (2)

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

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. R. Dasari, and M. S. Feld, "Single molecule detection using surface-enhanced Raman scattering (SERS)," Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

1996 (2)

M. I. Stockman, L. N. Pandey, and T. F. George, "Inhomogeneous localization of polar eigenmodes in fractals," Phys. Rev. B 53, 2183-2186 (1996).
[CrossRef]

V. A. Markel, V. M. Shalaev, E. B. Stechel, W. Kim, and R. L. Armstrong, "Small-particle composites. I. Linear optical properties," Phys. Rev. B 53, 2425-2436 (1996).
[CrossRef]

1995 (3)

J.-Y. Bigot, J. C. Merle, O. Cregut, and A. Daunois, "Electron dynamics in copper metallic nanoparticles probed with femtosecond optical pulses," Phys. Rev. Lett. 75, 4702-4705 (1995).
[CrossRef] [PubMed]

V. V. Kresin, "Collective resonances in silver clusters: role of d electrons and the polarization-free surface layer," Phys. Rev. B 51, 1844-1849 (1995).
[CrossRef]

A. Liebsch and W. L. Schaich, "Influence of a polarizable medium on the nonlocal optical response of a metal surface," Phys. Rev. B 52, 14219-14234 (1995).
[CrossRef]

1993 (1)

A. Liebsch, "Surface-plasmon dispersion and size dependence of Mie resonance: silver versus simple metals," Phys. Rev. B 48, 11317-11328 (1993).
[CrossRef]

1992 (1)

A. Otto, I. Mrozek, H. Grabhorn, and W. J. Akermann, "Surface-enhanced Raman scattering," J. Phys.: Condens. Matter 4, 1143-1212 (1992), and references therein.
[CrossRef]

1985 (3)

M. Moskovits, "Surface-enhanced spectroscopy," Rev. Mod. Phys. 57, 783-826 (1985).
[CrossRef]

W. Ekardt, "Size-dependent photoabsorption and photoemission of small metal particles," Phys. Rev. B 31, 6360-6370 (1985).
[CrossRef]

B. N. J. Persson and E. Zaremba, "Electron-hole pair production at metal surfaces," Phys. Rev. B 31, 1863-1872 (1985).
[CrossRef]

1982 (1)

F. J. Adrian, "Charge transfer effects in surface-enhanced Raman scattering," J. Chem. Phys. 77, 5302-5314 (1982).
[CrossRef]

1981 (1)

B. N. J. Persson, "On the theory of surface-enhanced Raman scattering," Chem. Phys. Lett. 82, 561-565 (1981).
[CrossRef]

1980 (2)

M. Kerker, D.-S. Wang, and H. Chew, "Surface enhanced Raman scattering (SERS) by molecules adsorbed at spherical particles: errata," Appl. Opt. 19, 4159-4174 (1980).
[PubMed]

J. Gersten and A. Nitzan, "Electromagnetic theory of enhanced Raman scattering by molecules adsorbed on rough surfaces," J. Chem. Phys. 73, 3023-3037 (1980).
[CrossRef]

1978 (1)

M. Moskovits, "Surface roughness and the enhanced intensity of Raman scattering by molecules adsorbed on metals," J. Chem. Phys. 69, 4159-4161 (1978).
[CrossRef]

1977 (2)

D. L. Jeanmaire and R. P. Van Duyne, "Surface Raman spectroelectrochemistry. Part I. Heterocyclic, aromatic, and aliphatic amines adsorbed on the anodized silver electrode," J. Electroanal. Chem. Interfacial Electrochem. 84, 1-20 (1977).
[CrossRef]

A. A. Lushnikov, V. V. Maksimenko, and A. J. Simonov, "Surface plasmon oscillations in layer metal particles," Z. Phys. B 27, 321-324 (1977).
[CrossRef]

1974 (1)

M. Fleischman, P. J. Hendra, and A. J. McQuillan, "Raman spectra of pyridine adsorbed at a silver electrode," Chem. Phys. Lett. 26, 163-166 (1974).
[CrossRef]

1966 (1)

A. Kawabata and R. Kubo, "Electronic properties of fine metallic particles. II. Plasma resonance absorption," J. Phys. Soc. Jpn. 21, 1765-1772 (1966).
[CrossRef]

Adrian, F. J.

F. J. Adrian, "Charge transfer effects in surface-enhanced Raman scattering," J. Chem. Phys. 77, 5302-5314 (1982).
[CrossRef]

Aizpurua, J.

H. Xu, J. Aizpurua, M. Käll, and P. Apell, "Electromagnetic contributions to single-molecule sensitivity in surface-enhanced Raman scattering," Phys. Rev. E 62, 4318-4324 (2000).
[CrossRef]

Akermann, W. J.

A. Otto, I. Mrozek, H. Grabhorn, and W. J. Akermann, "Surface-enhanced Raman scattering," J. Phys.: Condens. Matter 4, 1143-1212 (1992), and references therein.
[CrossRef]

Apell, P.

H. Xu, J. Aizpurua, M. Käll, and P. Apell, "Electromagnetic contributions to single-molecule sensitivity in surface-enhanced Raman scattering," Phys. Rev. E 62, 4318-4324 (2000).
[CrossRef]

Armstrong, R. L.

V. A. Markel, V. M. Shalaev, E. B. Stechel, W. Kim, and R. L. Armstrong, "Small-particle composites. I. Linear optical properties," Phys. Rev. B 53, 2425-2436 (1996).
[CrossRef]

Averitt, R. D.

S. J. Oldenburg, S. L. Westcott, R. D. Averitt, and N. J. Halas, "Surface enhanced Raman scattering in the near infrared using metal nanoshell substrates," J. Chem. Phys. 111, 4729-4735 (1999).
[CrossRef]

Bergman, D. J.

K. Li, M. I. Stockman, and D. J. Bergman, "Self-similar chain of metal nanospheres as an efficient nanolens," Phys. Rev. Lett. 91, 227402 (2003).
[CrossRef] [PubMed]

Bigot, J.-Y.

J.-Y. Bigot, J. C. Merle, O. Cregut, and A. Daunois, "Electron dynamics in copper metallic nanoparticles probed with femtosecond optical pulses," Phys. Rev. Lett. 75, 4702-4705 (1995).
[CrossRef] [PubMed]

Bjerneld, E. J.

H. Xu, E. J. Bjerneld, M. Käll, and L. Börjesson, "Spectroscopy of single hemoglobin molecules by surface enhanced Raman scattering," Phys. Rev. Lett. 83, 4357-4360 (1999).
[CrossRef]

Börjesson, L.

H. Xu, E. J. Bjerneld, M. Käll, and L. Börjesson, "Spectroscopy of single hemoglobin molecules by surface enhanced Raman scattering," Phys. Rev. Lett. 83, 4357-4360 (1999).
[CrossRef]

Broyer, M.

C. Voisin, D. Christofilos, N. Del Fatti, F. Vallée, B. Prével, E. Cottancin, J. Lermé, M. Pellarin, and M. Broyer, "Size-dependent electron-electron interactions in metal nanoparticles," Phys. Rev. Lett. 85, 2200-2203 (2000).
[CrossRef] [PubMed]

Brus, L. E.

A. M. Michaels, J. Jiang, and L. E. Brus, "Ag nanocrystal junctions as the site for surface-enhanced Raman scattering of single rhodamine 6G molecules," J. Phys. Chem. B 104, 11965-11971 (2000).
[CrossRef]

M. Michaels, M. Nirmal, and L. E. Brus, "Surface enhanced Raman spectroscopy of individual rhodamine 6G molecules on large Ag nanocrystals," J. Am. Chem. Soc. 121, 9932-9939 (1999).
[CrossRef]

Chew, H.

Christofilos, D.

C. Voisin, D. Christofilos, N. Del Fatti, F. Vallée, B. Prével, E. Cottancin, J. Lermé, M. Pellarin, and M. Broyer, "Size-dependent electron-electron interactions in metal nanoparticles," Phys. Rev. Lett. 85, 2200-2203 (2000).
[CrossRef] [PubMed]

Cottancin, E.

C. Voisin, D. Christofilos, N. Del Fatti, F. Vallée, B. Prével, E. Cottancin, J. Lermé, M. Pellarin, and M. Broyer, "Size-dependent electron-electron interactions in metal nanoparticles," Phys. Rev. Lett. 85, 2200-2203 (2000).
[CrossRef] [PubMed]

Cregut, O.

J.-Y. Bigot, J. C. Merle, O. Cregut, and A. Daunois, "Electron dynamics in copper metallic nanoparticles probed with femtosecond optical pulses," Phys. Rev. Lett. 75, 4702-4705 (1995).
[CrossRef] [PubMed]

Dasari, R. R.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, "Ultrasensitive chemical analysis by Raman spectroscopy," Chem. Rev. (Washington, D.C.) 99, 2957-2976 (1999), and references therein.
[CrossRef]

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. R. Dasari, and M. S. Feld, "Single molecule detection using surface-enhanced Raman scattering (SERS)," Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

Daunois, A.

J.-Y. Bigot, J. C. Merle, O. Cregut, and A. Daunois, "Electron dynamics in copper metallic nanoparticles probed with femtosecond optical pulses," Phys. Rev. Lett. 75, 4702-4705 (1995).
[CrossRef] [PubMed]

Del Fatti, N.

C. Voisin, D. Christofilos, N. Del Fatti, F. Vallée, B. Prével, E. Cottancin, J. Lermé, M. Pellarin, and M. Broyer, "Size-dependent electron-electron interactions in metal nanoparticles," Phys. Rev. Lett. 85, 2200-2203 (2000).
[CrossRef] [PubMed]

Dickson, R. M.

L. Peyser-Capadona, J. Zheng, J. I. Gonzlez, T.-H. Lee, S. A. Patel, and R. M. Dickson, "Nanoparticle-free single molecule anti-Stokes Raman spectroscopy," Phys. Rev. Lett. 94, 058301 (2005).
[CrossRef] [PubMed]

Du, H.

Z. Wang, S. Pan, T. D. Krauss, H. Du, and L. J. Rothberg, "The structural basis for giant enhancement enabling single-molecule Raman scattering," Proc. Natl. Acad. Sci. U.S.A. 100, 8638-8643 (2004).
[CrossRef]

Ekardt, W.

W. Ekardt, "Size-dependent photoabsorption and photoemission of small metal particles," Phys. Rev. B 31, 6360-6370 (1985).
[CrossRef]

El-Sayed, M. A.

B. Nikoobakht, J. Wang, and M. A. El-Sayed, "Surface-enhanced Raman scattering of molecules adsorbed on gold nanorods: off-surface plasmon resonance condition," Chem. Phys. Lett. 366, 17-23 (2002).
[CrossRef]

Emory, S. R.

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

Ernst, N.

N. Nilius, N. Ernst, and H.-J. Freund, "Photon emission spectroscopy of individual oxide-supported silver clusters in a scanning tunneling microscope," Phys. Rev. Lett. 84, 3994-3997 (2000).
[CrossRef] [PubMed]

Feld, M. S.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, "Ultrasensitive chemical analysis by Raman spectroscopy," Chem. Rev. (Washington, D.C.) 99, 2957-2976 (1999), and references therein.
[CrossRef]

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. R. Dasari, and M. S. Feld, "Single molecule detection using surface-enhanced Raman scattering (SERS)," Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

Feldmann, J.

C. Sönnichsen, T. Franzl, T. Wilk, G. von Plessen, J. Feldmann, O. Wilson, and P. Mulvaney, "Drastic reduction of plasmon damping in gold nanorods," Phys. Rev. Lett. 88, 077402 (2002).
[CrossRef] [PubMed]

Fleischman, M.

M. Fleischman, P. J. Hendra, and A. J. McQuillan, "Raman spectra of pyridine adsorbed at a silver electrode," Chem. Phys. Lett. 26, 163-166 (1974).
[CrossRef]

Franzl, T.

C. Sönnichsen, T. Franzl, T. Wilk, G. von Plessen, J. Feldmann, O. Wilson, and P. Mulvaney, "Drastic reduction of plasmon damping in gold nanorods," Phys. Rev. Lett. 88, 077402 (2002).
[CrossRef] [PubMed]

Freund, H.-J.

N. Nilius, N. Ernst, and H.-J. Freund, "Photon emission spectroscopy of individual oxide-supported silver clusters in a scanning tunneling microscope," Phys. Rev. Lett. 84, 3994-3997 (2000).
[CrossRef] [PubMed]

George, T. F.

M. I. Stockman, L. N. Pandey, and T. F. George, "Inhomogeneous localization of polar eigenmodes in fractals," Phys. Rev. B 53, 2183-2186 (1996).
[CrossRef]

Gersten, J.

J. Gersten and A. Nitzan, "Electromagnetic theory of enhanced Raman scattering by molecules adsorbed on rough surfaces," J. Chem. Phys. 73, 3023-3037 (1980).
[CrossRef]

Gonzlez, J. I.

L. Peyser-Capadona, J. Zheng, J. I. Gonzlez, T.-H. Lee, S. A. Patel, and R. M. Dickson, "Nanoparticle-free single molecule anti-Stokes Raman spectroscopy," Phys. Rev. Lett. 94, 058301 (2005).
[CrossRef] [PubMed]

Grabhorn, H.

A. Otto, I. Mrozek, H. Grabhorn, and W. J. Akermann, "Surface-enhanced Raman scattering," J. Phys.: Condens. Matter 4, 1143-1212 (1992), and references therein.
[CrossRef]

Halas, N. J.

S. J. Oldenburg, S. L. Westcott, R. D. Averitt, and N. J. Halas, "Surface enhanced Raman scattering in the near infrared using metal nanoshell substrates," J. Chem. Phys. 111, 4729-4735 (1999).
[CrossRef]

Haslett, T.

M. Moskovits, L. Tay, J. Yang, and T. Haslett, "SERS and the single molecule," Top. Appl. Phys. 82, 215-226 (2002).

Hendra, P. J.

M. Fleischman, P. J. Hendra, and A. J. McQuillan, "Raman spectra of pyridine adsorbed at a silver electrode," Chem. Phys. Lett. 26, 163-166 (1974).
[CrossRef]

Itzkan, I.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, "Ultrasensitive chemical analysis by Raman spectroscopy," Chem. Rev. (Washington, D.C.) 99, 2957-2976 (1999), and references therein.
[CrossRef]

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. R. Dasari, and M. S. Feld, "Single molecule detection using surface-enhanced Raman scattering (SERS)," Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

Jeanmaire, D. L.

D. L. Jeanmaire and R. P. Van Duyne, "Surface Raman spectroelectrochemistry. Part I. Heterocyclic, aromatic, and aliphatic amines adsorbed on the anodized silver electrode," J. Electroanal. Chem. Interfacial Electrochem. 84, 1-20 (1977).
[CrossRef]

Jiang, J.

A. M. Michaels, J. Jiang, and L. E. Brus, "Ag nanocrystal junctions as the site for surface-enhanced Raman scattering of single rhodamine 6G molecules," J. Phys. Chem. B 104, 11965-11971 (2000).
[CrossRef]

Johansson, P.

H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, "Unified treatment of fluorescence and Raman scattering processes near metal surfaces," Phys. Rev. Lett. 93, 243002 (2004).
[CrossRef]

Käll, M.

H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, "Unified treatment of fluorescence and Raman scattering processes near metal surfaces," Phys. Rev. Lett. 93, 243002 (2004).
[CrossRef]

H. Xu, J. Aizpurua, M. Käll, and P. Apell, "Electromagnetic contributions to single-molecule sensitivity in surface-enhanced Raman scattering," Phys. Rev. E 62, 4318-4324 (2000).
[CrossRef]

H. Xu, E. J. Bjerneld, M. Käll, and L. Börjesson, "Spectroscopy of single hemoglobin molecules by surface enhanced Raman scattering," Phys. Rev. Lett. 83, 4357-4360 (1999).
[CrossRef]

Kawabata, A.

A. Kawabata and R. Kubo, "Electronic properties of fine metallic particles. II. Plasma resonance absorption," J. Phys. Soc. Jpn. 21, 1765-1772 (1966).
[CrossRef]

Kerker, M.

Kim, W.

V. A. Markel, V. M. Shalaev, E. B. Stechel, W. Kim, and R. L. Armstrong, "Small-particle composites. I. Linear optical properties," Phys. Rev. B 53, 2425-2436 (1996).
[CrossRef]

Kneipp, H.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, "Ultrasensitive chemical analysis by Raman spectroscopy," Chem. Rev. (Washington, D.C.) 99, 2957-2976 (1999), and references therein.
[CrossRef]

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. R. Dasari, and M. S. Feld, "Single molecule detection using surface-enhanced Raman scattering (SERS)," Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

Kneipp, K.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, "Ultrasensitive chemical analysis by Raman spectroscopy," Chem. Rev. (Washington, D.C.) 99, 2957-2976 (1999), and references therein.
[CrossRef]

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. R. Dasari, and M. S. Feld, "Single molecule detection using surface-enhanced Raman scattering (SERS)," Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

Krauss, T. D.

Z. Wang, S. Pan, T. D. Krauss, H. Du, and L. J. Rothberg, "The structural basis for giant enhancement enabling single-molecule Raman scattering," Proc. Natl. Acad. Sci. U.S.A. 100, 8638-8643 (2004).
[CrossRef]

Kreibig, U.

See, e.g., U. Kreibig and M. Vollmer, Optical Properties of Metal Clusters (Springer, 1995).

Kresin, V. V.

V. V. Kresin, "Collective resonances in silver clusters: role of d electrons and the polarization-free surface layer," Phys. Rev. B 51, 1844-1849 (1995).
[CrossRef]

Kubo, R.

A. Kawabata and R. Kubo, "Electronic properties of fine metallic particles. II. Plasma resonance absorption," J. Phys. Soc. Jpn. 21, 1765-1772 (1966).
[CrossRef]

Lee, T.-H.

L. Peyser-Capadona, J. Zheng, J. I. Gonzlez, T.-H. Lee, S. A. Patel, and R. M. Dickson, "Nanoparticle-free single molecule anti-Stokes Raman spectroscopy," Phys. Rev. Lett. 94, 058301 (2005).
[CrossRef] [PubMed]

Lermé, J.

C. Voisin, D. Christofilos, N. Del Fatti, F. Vallée, B. Prével, E. Cottancin, J. Lermé, M. Pellarin, and M. Broyer, "Size-dependent electron-electron interactions in metal nanoparticles," Phys. Rev. Lett. 85, 2200-2203 (2000).
[CrossRef] [PubMed]

Li, K.

K. Li, M. I. Stockman, and D. J. Bergman, "Self-similar chain of metal nanospheres as an efficient nanolens," Phys. Rev. Lett. 91, 227402 (2003).
[CrossRef] [PubMed]

Liebsch, A.

C. Lopez-Bastidas, J. A. Maytorena, and A. Liebsch, "Hot-electron dynamics at noble metal surfaces," Phys. Rev. B 65, 035417 (2002).
[CrossRef]

A. Liebsch and W. L. Schaich, "Influence of a polarizable medium on the nonlocal optical response of a metal surface," Phys. Rev. B 52, 14219-14234 (1995).
[CrossRef]

A. Liebsch, "Surface-plasmon dispersion and size dependence of Mie resonance: silver versus simple metals," Phys. Rev. B 48, 11317-11328 (1993).
[CrossRef]

Long, D. A.

See, e.g., D. A. Long, The Raman Effect (Wiley, 2002).
[CrossRef]

Lopez-Bastidas, C.

C. Lopez-Bastidas, J. A. Maytorena, and A. Liebsch, "Hot-electron dynamics at noble metal surfaces," Phys. Rev. B 65, 035417 (2002).
[CrossRef]

Lushnikov, A. A.

A. A. Lushnikov, V. V. Maksimenko, and A. J. Simonov, "Surface plasmon oscillations in layer metal particles," Z. Phys. B 27, 321-324 (1977).
[CrossRef]

Maksimenko, V. V.

A. A. Lushnikov, V. V. Maksimenko, and A. J. Simonov, "Surface plasmon oscillations in layer metal particles," Z. Phys. B 27, 321-324 (1977).
[CrossRef]

Markel, V. A.

V. A. Markel, V. M. Shalaev, E. B. Stechel, W. Kim, and R. L. Armstrong, "Small-particle composites. I. Linear optical properties," Phys. Rev. B 53, 2425-2436 (1996).
[CrossRef]

Maytorena, J. A.

C. Lopez-Bastidas, J. A. Maytorena, and A. Liebsch, "Hot-electron dynamics at noble metal surfaces," Phys. Rev. B 65, 035417 (2002).
[CrossRef]

McQuillan, A. J.

M. Fleischman, P. J. Hendra, and A. J. McQuillan, "Raman spectra of pyridine adsorbed at a silver electrode," Chem. Phys. Lett. 26, 163-166 (1974).
[CrossRef]

Merle, J. C.

J.-Y. Bigot, J. C. Merle, O. Cregut, and A. Daunois, "Electron dynamics in copper metallic nanoparticles probed with femtosecond optical pulses," Phys. Rev. Lett. 75, 4702-4705 (1995).
[CrossRef] [PubMed]

Michaels, A. M.

A. M. Michaels, J. Jiang, and L. E. Brus, "Ag nanocrystal junctions as the site for surface-enhanced Raman scattering of single rhodamine 6G molecules," J. Phys. Chem. B 104, 11965-11971 (2000).
[CrossRef]

Michaels, M.

M. Michaels, M. Nirmal, and L. E. Brus, "Surface enhanced Raman spectroscopy of individual rhodamine 6G molecules on large Ag nanocrystals," J. Am. Chem. Soc. 121, 9932-9939 (1999).
[CrossRef]

Moskovits, M.

M. Moskovits, L. Tay, J. Yang, and T. Haslett, "SERS and the single molecule," Top. Appl. Phys. 82, 215-226 (2002).

M. Moskovits, "Surface-enhanced spectroscopy," Rev. Mod. Phys. 57, 783-826 (1985).
[CrossRef]

M. Moskovits, "Surface roughness and the enhanced intensity of Raman scattering by molecules adsorbed on metals," J. Chem. Phys. 69, 4159-4161 (1978).
[CrossRef]

Mrozek, I.

A. Otto, I. Mrozek, H. Grabhorn, and W. J. Akermann, "Surface-enhanced Raman scattering," J. Phys.: Condens. Matter 4, 1143-1212 (1992), and references therein.
[CrossRef]

Mulvaney, P.

C. Sönnichsen, T. Franzl, T. Wilk, G. von Plessen, J. Feldmann, O. Wilson, and P. Mulvaney, "Drastic reduction of plasmon damping in gold nanorods," Phys. Rev. Lett. 88, 077402 (2002).
[CrossRef] [PubMed]

Nie, S.

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

Nikoobakht, B.

B. Nikoobakht, J. Wang, and M. A. El-Sayed, "Surface-enhanced Raman scattering of molecules adsorbed on gold nanorods: off-surface plasmon resonance condition," Chem. Phys. Lett. 366, 17-23 (2002).
[CrossRef]

Nilius, N.

N. Nilius, N. Ernst, and H.-J. Freund, "Photon emission spectroscopy of individual oxide-supported silver clusters in a scanning tunneling microscope," Phys. Rev. Lett. 84, 3994-3997 (2000).
[CrossRef] [PubMed]

Nirmal, M.

M. Michaels, M. Nirmal, and L. E. Brus, "Surface enhanced Raman spectroscopy of individual rhodamine 6G molecules on large Ag nanocrystals," J. Am. Chem. Soc. 121, 9932-9939 (1999).
[CrossRef]

Nitzan, A.

J. Gersten and A. Nitzan, "Electromagnetic theory of enhanced Raman scattering by molecules adsorbed on rough surfaces," J. Chem. Phys. 73, 3023-3037 (1980).
[CrossRef]

Oldenburg, S. J.

S. J. Oldenburg, S. L. Westcott, R. D. Averitt, and N. J. Halas, "Surface enhanced Raman scattering in the near infrared using metal nanoshell substrates," J. Chem. Phys. 111, 4729-4735 (1999).
[CrossRef]

Otto, A.

A. Otto, I. Mrozek, H. Grabhorn, and W. J. Akermann, "Surface-enhanced Raman scattering," J. Phys.: Condens. Matter 4, 1143-1212 (1992), and references therein.
[CrossRef]

Pan, S.

Z. Wang, S. Pan, T. D. Krauss, H. Du, and L. J. Rothberg, "The structural basis for giant enhancement enabling single-molecule Raman scattering," Proc. Natl. Acad. Sci. U.S.A. 100, 8638-8643 (2004).
[CrossRef]

Pandey, L. N.

M. I. Stockman, L. N. Pandey, and T. F. George, "Inhomogeneous localization of polar eigenmodes in fractals," Phys. Rev. B 53, 2183-2186 (1996).
[CrossRef]

Patel, S. A.

L. Peyser-Capadona, J. Zheng, J. I. Gonzlez, T.-H. Lee, S. A. Patel, and R. M. Dickson, "Nanoparticle-free single molecule anti-Stokes Raman spectroscopy," Phys. Rev. Lett. 94, 058301 (2005).
[CrossRef] [PubMed]

Pellarin, M.

C. Voisin, D. Christofilos, N. Del Fatti, F. Vallée, B. Prével, E. Cottancin, J. Lermé, M. Pellarin, and M. Broyer, "Size-dependent electron-electron interactions in metal nanoparticles," Phys. Rev. Lett. 85, 2200-2203 (2000).
[CrossRef] [PubMed]

Perelman, L. T.

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. R. Dasari, and M. S. Feld, "Single molecule detection using surface-enhanced Raman scattering (SERS)," Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

Persson, B. N. J.

B. N. J. Persson and E. Zaremba, "Electron-hole pair production at metal surfaces," Phys. Rev. B 31, 1863-1872 (1985).
[CrossRef]

B. N. J. Persson, "On the theory of surface-enhanced Raman scattering," Chem. Phys. Lett. 82, 561-565 (1981).
[CrossRef]

Persson, M. P.

H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, "Unified treatment of fluorescence and Raman scattering processes near metal surfaces," Phys. Rev. Lett. 93, 243002 (2004).
[CrossRef]

Peyser-Capadona, L.

L. Peyser-Capadona, J. Zheng, J. I. Gonzlez, T.-H. Lee, S. A. Patel, and R. M. Dickson, "Nanoparticle-free single molecule anti-Stokes Raman spectroscopy," Phys. Rev. Lett. 94, 058301 (2005).
[CrossRef] [PubMed]

Prével, B.

C. Voisin, D. Christofilos, N. Del Fatti, F. Vallée, B. Prével, E. Cottancin, J. Lermé, M. Pellarin, and M. Broyer, "Size-dependent electron-electron interactions in metal nanoparticles," Phys. Rev. Lett. 85, 2200-2203 (2000).
[CrossRef] [PubMed]

Pustovit, V. N.

V. N. Pustovit and T. V. Shahbazyan, "Microscopic theory of surface-enhanced Raman scattering in noble-metal nanoparticles," Phys. Rev. B 73, 085408 (2006).
[CrossRef]

Rothberg, L. J.

Z. Wang, S. Pan, T. D. Krauss, H. Du, and L. J. Rothberg, "The structural basis for giant enhancement enabling single-molecule Raman scattering," Proc. Natl. Acad. Sci. U.S.A. 100, 8638-8643 (2004).
[CrossRef]

Schaich, W. L.

A. Liebsch and W. L. Schaich, "Influence of a polarizable medium on the nonlocal optical response of a metal surface," Phys. Rev. B 52, 14219-14234 (1995).
[CrossRef]

Schatz, G. S.

For a recent review, see G. S. Schatz and R. P. Van Duyne, in Handbook of Vibrational Spectroscopy, J.M.Chalmers and P.R.Griffiths, eds. (Wiley, 2002), p. 1.

Shahbazyan, T. V.

V. N. Pustovit and T. V. Shahbazyan, "Microscopic theory of surface-enhanced Raman scattering in noble-metal nanoparticles," Phys. Rev. B 73, 085408 (2006).
[CrossRef]

Shalaev, V. M.

V. A. Markel, V. M. Shalaev, E. B. Stechel, W. Kim, and R. L. Armstrong, "Small-particle composites. I. Linear optical properties," Phys. Rev. B 53, 2425-2436 (1996).
[CrossRef]

Simonov, A. J.

A. A. Lushnikov, V. V. Maksimenko, and A. J. Simonov, "Surface plasmon oscillations in layer metal particles," Z. Phys. B 27, 321-324 (1977).
[CrossRef]

Sönnichsen, C.

C. Sönnichsen, T. Franzl, T. Wilk, G. von Plessen, J. Feldmann, O. Wilson, and P. Mulvaney, "Drastic reduction of plasmon damping in gold nanorods," Phys. Rev. Lett. 88, 077402 (2002).
[CrossRef] [PubMed]

Stechel, E. B.

V. A. Markel, V. M. Shalaev, E. B. Stechel, W. Kim, and R. L. Armstrong, "Small-particle composites. I. Linear optical properties," Phys. Rev. B 53, 2425-2436 (1996).
[CrossRef]

Stockman, M. I.

K. Li, M. I. Stockman, and D. J. Bergman, "Self-similar chain of metal nanospheres as an efficient nanolens," Phys. Rev. Lett. 91, 227402 (2003).
[CrossRef] [PubMed]

M. I. Stockman, L. N. Pandey, and T. F. George, "Inhomogeneous localization of polar eigenmodes in fractals," Phys. Rev. B 53, 2183-2186 (1996).
[CrossRef]

Tay, L.

M. Moskovits, L. Tay, J. Yang, and T. Haslett, "SERS and the single molecule," Top. Appl. Phys. 82, 215-226 (2002).

Vallée, F.

C. Voisin, D. Christofilos, N. Del Fatti, F. Vallée, B. Prével, E. Cottancin, J. Lermé, M. Pellarin, and M. Broyer, "Size-dependent electron-electron interactions in metal nanoparticles," Phys. Rev. Lett. 85, 2200-2203 (2000).
[CrossRef] [PubMed]

Van Duyne, R. P.

D. L. Jeanmaire and R. P. Van Duyne, "Surface Raman spectroelectrochemistry. Part I. Heterocyclic, aromatic, and aliphatic amines adsorbed on the anodized silver electrode," J. Electroanal. Chem. Interfacial Electrochem. 84, 1-20 (1977).
[CrossRef]

For a recent review, see G. S. Schatz and R. P. Van Duyne, in Handbook of Vibrational Spectroscopy, J.M.Chalmers and P.R.Griffiths, eds. (Wiley, 2002), p. 1.

Voisin, C.

C. Voisin, D. Christofilos, N. Del Fatti, F. Vallée, B. Prével, E. Cottancin, J. Lermé, M. Pellarin, and M. Broyer, "Size-dependent electron-electron interactions in metal nanoparticles," Phys. Rev. Lett. 85, 2200-2203 (2000).
[CrossRef] [PubMed]

Vollmer, M.

See, e.g., U. Kreibig and M. Vollmer, Optical Properties of Metal Clusters (Springer, 1995).

von Plessen, G.

C. Sönnichsen, T. Franzl, T. Wilk, G. von Plessen, J. Feldmann, O. Wilson, and P. Mulvaney, "Drastic reduction of plasmon damping in gold nanorods," Phys. Rev. Lett. 88, 077402 (2002).
[CrossRef] [PubMed]

Wang, D.-S.

Wang, J.

B. Nikoobakht, J. Wang, and M. A. El-Sayed, "Surface-enhanced Raman scattering of molecules adsorbed on gold nanorods: off-surface plasmon resonance condition," Chem. Phys. Lett. 366, 17-23 (2002).
[CrossRef]

Wang, X.-H.

H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, "Unified treatment of fluorescence and Raman scattering processes near metal surfaces," Phys. Rev. Lett. 93, 243002 (2004).
[CrossRef]

Wang, Y.

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. R. Dasari, and M. S. Feld, "Single molecule detection using surface-enhanced Raman scattering (SERS)," Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

Wang, Z.

Z. Wang, S. Pan, T. D. Krauss, H. Du, and L. J. Rothberg, "The structural basis for giant enhancement enabling single-molecule Raman scattering," Proc. Natl. Acad. Sci. U.S.A. 100, 8638-8643 (2004).
[CrossRef]

Westcott, S. L.

S. J. Oldenburg, S. L. Westcott, R. D. Averitt, and N. J. Halas, "Surface enhanced Raman scattering in the near infrared using metal nanoshell substrates," J. Chem. Phys. 111, 4729-4735 (1999).
[CrossRef]

Wilk, T.

C. Sönnichsen, T. Franzl, T. Wilk, G. von Plessen, J. Feldmann, O. Wilson, and P. Mulvaney, "Drastic reduction of plasmon damping in gold nanorods," Phys. Rev. Lett. 88, 077402 (2002).
[CrossRef] [PubMed]

Wilson, O.

C. Sönnichsen, T. Franzl, T. Wilk, G. von Plessen, J. Feldmann, O. Wilson, and P. Mulvaney, "Drastic reduction of plasmon damping in gold nanorods," Phys. Rev. Lett. 88, 077402 (2002).
[CrossRef] [PubMed]

Xu, H.

H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, "Unified treatment of fluorescence and Raman scattering processes near metal surfaces," Phys. Rev. Lett. 93, 243002 (2004).
[CrossRef]

H. Xu, J. Aizpurua, M. Käll, and P. Apell, "Electromagnetic contributions to single-molecule sensitivity in surface-enhanced Raman scattering," Phys. Rev. E 62, 4318-4324 (2000).
[CrossRef]

H. Xu, E. J. Bjerneld, M. Käll, and L. Börjesson, "Spectroscopy of single hemoglobin molecules by surface enhanced Raman scattering," Phys. Rev. Lett. 83, 4357-4360 (1999).
[CrossRef]

Xu, H. Q.

H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, "Unified treatment of fluorescence and Raman scattering processes near metal surfaces," Phys. Rev. Lett. 93, 243002 (2004).
[CrossRef]

Yang, J.

M. Moskovits, L. Tay, J. Yang, and T. Haslett, "SERS and the single molecule," Top. Appl. Phys. 82, 215-226 (2002).

Zaremba, E.

B. N. J. Persson and E. Zaremba, "Electron-hole pair production at metal surfaces," Phys. Rev. B 31, 1863-1872 (1985).
[CrossRef]

Zheng, J.

L. Peyser-Capadona, J. Zheng, J. I. Gonzlez, T.-H. Lee, S. A. Patel, and R. M. Dickson, "Nanoparticle-free single molecule anti-Stokes Raman spectroscopy," Phys. Rev. Lett. 94, 058301 (2005).
[CrossRef] [PubMed]

Appl. Opt. (1)

Chem. Phys. Lett. (3)

B. N. J. Persson, "On the theory of surface-enhanced Raman scattering," Chem. Phys. Lett. 82, 561-565 (1981).
[CrossRef]

M. Fleischman, P. J. Hendra, and A. J. McQuillan, "Raman spectra of pyridine adsorbed at a silver electrode," Chem. Phys. Lett. 26, 163-166 (1974).
[CrossRef]

B. Nikoobakht, J. Wang, and M. A. El-Sayed, "Surface-enhanced Raman scattering of molecules adsorbed on gold nanorods: off-surface plasmon resonance condition," Chem. Phys. Lett. 366, 17-23 (2002).
[CrossRef]

Chem. Rev. (Washington, D.C.) (1)

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, "Ultrasensitive chemical analysis by Raman spectroscopy," Chem. Rev. (Washington, D.C.) 99, 2957-2976 (1999), and references therein.
[CrossRef]

J. Am. Chem. Soc. (1)

M. Michaels, M. Nirmal, and L. E. Brus, "Surface enhanced Raman spectroscopy of individual rhodamine 6G molecules on large Ag nanocrystals," J. Am. Chem. Soc. 121, 9932-9939 (1999).
[CrossRef]

J. Chem. Phys. (4)

M. Moskovits, "Surface roughness and the enhanced intensity of Raman scattering by molecules adsorbed on metals," J. Chem. Phys. 69, 4159-4161 (1978).
[CrossRef]

F. J. Adrian, "Charge transfer effects in surface-enhanced Raman scattering," J. Chem. Phys. 77, 5302-5314 (1982).
[CrossRef]

J. Gersten and A. Nitzan, "Electromagnetic theory of enhanced Raman scattering by molecules adsorbed on rough surfaces," J. Chem. Phys. 73, 3023-3037 (1980).
[CrossRef]

S. J. Oldenburg, S. L. Westcott, R. D. Averitt, and N. J. Halas, "Surface enhanced Raman scattering in the near infrared using metal nanoshell substrates," J. Chem. Phys. 111, 4729-4735 (1999).
[CrossRef]

J. Electroanal. Chem. Interfacial Electrochem. (1)

D. L. Jeanmaire and R. P. Van Duyne, "Surface Raman spectroelectrochemistry. Part I. Heterocyclic, aromatic, and aliphatic amines adsorbed on the anodized silver electrode," J. Electroanal. Chem. Interfacial Electrochem. 84, 1-20 (1977).
[CrossRef]

J. Phys. Chem. B (1)

A. M. Michaels, J. Jiang, and L. E. Brus, "Ag nanocrystal junctions as the site for surface-enhanced Raman scattering of single rhodamine 6G molecules," J. Phys. Chem. B 104, 11965-11971 (2000).
[CrossRef]

J. Phys. Soc. Jpn. (1)

A. Kawabata and R. Kubo, "Electronic properties of fine metallic particles. II. Plasma resonance absorption," J. Phys. Soc. Jpn. 21, 1765-1772 (1966).
[CrossRef]

J. Phys.: Condens. Matter (1)

A. Otto, I. Mrozek, H. Grabhorn, and W. J. Akermann, "Surface-enhanced Raman scattering," J. Phys.: Condens. Matter 4, 1143-1212 (1992), and references therein.
[CrossRef]

Phys. Rev. B (9)

M. I. Stockman, L. N. Pandey, and T. F. George, "Inhomogeneous localization of polar eigenmodes in fractals," Phys. Rev. B 53, 2183-2186 (1996).
[CrossRef]

V. A. Markel, V. M. Shalaev, E. B. Stechel, W. Kim, and R. L. Armstrong, "Small-particle composites. I. Linear optical properties," Phys. Rev. B 53, 2425-2436 (1996).
[CrossRef]

B. N. J. Persson and E. Zaremba, "Electron-hole pair production at metal surfaces," Phys. Rev. B 31, 1863-1872 (1985).
[CrossRef]

A. Liebsch, "Surface-plasmon dispersion and size dependence of Mie resonance: silver versus simple metals," Phys. Rev. B 48, 11317-11328 (1993).
[CrossRef]

V. V. Kresin, "Collective resonances in silver clusters: role of d electrons and the polarization-free surface layer," Phys. Rev. B 51, 1844-1849 (1995).
[CrossRef]

A. Liebsch and W. L. Schaich, "Influence of a polarizable medium on the nonlocal optical response of a metal surface," Phys. Rev. B 52, 14219-14234 (1995).
[CrossRef]

C. Lopez-Bastidas, J. A. Maytorena, and A. Liebsch, "Hot-electron dynamics at noble metal surfaces," Phys. Rev. B 65, 035417 (2002).
[CrossRef]

W. Ekardt, "Size-dependent photoabsorption and photoemission of small metal particles," Phys. Rev. B 31, 6360-6370 (1985).
[CrossRef]

V. N. Pustovit and T. V. Shahbazyan, "Microscopic theory of surface-enhanced Raman scattering in noble-metal nanoparticles," Phys. Rev. B 73, 085408 (2006).
[CrossRef]

Phys. Rev. E (1)

H. Xu, J. Aizpurua, M. Käll, and P. Apell, "Electromagnetic contributions to single-molecule sensitivity in surface-enhanced Raman scattering," Phys. Rev. E 62, 4318-4324 (2000).
[CrossRef]

Phys. Rev. Lett. (9)

K. Li, M. I. Stockman, and D. J. Bergman, "Self-similar chain of metal nanospheres as an efficient nanolens," Phys. Rev. Lett. 91, 227402 (2003).
[CrossRef] [PubMed]

H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, "Unified treatment of fluorescence and Raman scattering processes near metal surfaces," Phys. Rev. Lett. 93, 243002 (2004).
[CrossRef]

C. Sönnichsen, T. Franzl, T. Wilk, G. von Plessen, J. Feldmann, O. Wilson, and P. Mulvaney, "Drastic reduction of plasmon damping in gold nanorods," Phys. Rev. Lett. 88, 077402 (2002).
[CrossRef] [PubMed]

J.-Y. Bigot, J. C. Merle, O. Cregut, and A. Daunois, "Electron dynamics in copper metallic nanoparticles probed with femtosecond optical pulses," Phys. Rev. Lett. 75, 4702-4705 (1995).
[CrossRef] [PubMed]

N. Nilius, N. Ernst, and H.-J. Freund, "Photon emission spectroscopy of individual oxide-supported silver clusters in a scanning tunneling microscope," Phys. Rev. Lett. 84, 3994-3997 (2000).
[CrossRef] [PubMed]

C. Voisin, D. Christofilos, N. Del Fatti, F. Vallée, B. Prével, E. Cottancin, J. Lermé, M. Pellarin, and M. Broyer, "Size-dependent electron-electron interactions in metal nanoparticles," Phys. Rev. Lett. 85, 2200-2203 (2000).
[CrossRef] [PubMed]

H. Xu, E. J. Bjerneld, M. Käll, and L. Börjesson, "Spectroscopy of single hemoglobin molecules by surface enhanced Raman scattering," Phys. Rev. Lett. 83, 4357-4360 (1999).
[CrossRef]

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. R. Dasari, and M. S. Feld, "Single molecule detection using surface-enhanced Raman scattering (SERS)," Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

L. Peyser-Capadona, J. Zheng, J. I. Gonzlez, T.-H. Lee, S. A. Patel, and R. M. Dickson, "Nanoparticle-free single molecule anti-Stokes Raman spectroscopy," Phys. Rev. Lett. 94, 058301 (2005).
[CrossRef] [PubMed]

Proc. Natl. Acad. Sci. U.S.A. (1)

Z. Wang, S. Pan, T. D. Krauss, H. Du, and L. J. Rothberg, "The structural basis for giant enhancement enabling single-molecule Raman scattering," Proc. Natl. Acad. Sci. U.S.A. 100, 8638-8643 (2004).
[CrossRef]

Rev. Mod. Phys. (1)

M. Moskovits, "Surface-enhanced spectroscopy," Rev. Mod. Phys. 57, 783-826 (1985).
[CrossRef]

Science (1)

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

Top. Appl. Phys. (1)

M. Moskovits, L. Tay, J. Yang, and T. Haslett, "SERS and the single molecule," Top. Appl. Phys. 82, 215-226 (2002).

Z. Phys. B (1)

A. A. Lushnikov, V. V. Maksimenko, and A. J. Simonov, "Surface plasmon oscillations in layer metal particles," Z. Phys. B 27, 321-324 (1977).
[CrossRef]

Other (3)

See, e.g., D. A. Long, The Raman Effect (Wiley, 2002).
[CrossRef]

See, e.g., U. Kreibig and M. Vollmer, Optical Properties of Metal Clusters (Springer, 1995).

For a recent review, see G. S. Schatz and R. P. Van Duyne, in Handbook of Vibrational Spectroscopy, J.M.Chalmers and P.R.Griffiths, eds. (Wiley, 2002), p. 1.

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Figures (4)

Fig. 1
Fig. 1

Schematic representation of SERS from a molecule adsorbed on a metal nanoparticle.

Fig. 2
Fig. 2

Absorption spectra of an Ag nanoparticle calculated for R = 3.0 nm and several values of surface layer thickness Δ.

Fig. 3
Fig. 3

Local field at sp energy as a function of distance from the particle boundary calculated for R = 3.0 nm and several values of surface layer thickness Δ.

Fig. 4
Fig. 4

Size dependence of the Raman enhancement factor calculated for particle–molecule distance d = 0.1 nm and several values of surface layer thickness Δ.

Equations (24)

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ϵ s ( ω ) = 1 ω p 2 ω ( ω + i γ ) ,
γ s v F R ,
Φ ( ω , r ) = ϕ 0 ( r ) + d 3 r δ N ( ω , r ) r r ,
δ N ( r ) = δ N s ( r ) + δ N d ( r ) + δ N m ( r ) + δ N 0 ( r ) ,
δ N ( r ) = P ( r ) = ( P d + P s + P m + P 0 ) ,
P d ( r ) = ϵ d 1 4 π θ ( R d r ) Φ ( r ) ,
P s ( r ) = ϵ s 1 4 π θ ( R r ) Φ ( r ) ,
P m ( r ) = ϵ m 1 4 π θ ( r R ) Φ ( r ) ,
P 0 ( r ) = δ ( r r 0 ) α 0 Φ ( r 0 ) ,
ϵ ( r ) Φ ( r ) = ϕ 0 ( r ) 0 1 r r 0 α 0 0 Φ ( r 0 ) + d 3 r 1 r r [ χ d θ ( R d r ) + χ s θ ( R r ) + χ m θ ( r R ) ] Φ ( r ) ,
ϵ ( r ) Φ ( r ) = ϕ 0 ( r ) ϵ d 1 3 β ( r R d ) Φ ( R d ) + ϵ m ϵ s 3 β ( r R ) Φ ( R ) 4 π α 0 3 r 0 2 β ( r r 0 ) Φ ( r 0 ) r 0 ,
β ( x ) = x 2 θ ( x 1 ) 2 x θ ( 1 x ) .
ϕ = φ 0 + δ φ , φ 0 = ϕ 0 ϵ ( r ) = e E i r ϵ ( r ) ,
δ φ ( r ) = 1 ϵ ( r ) [ β ( r R d ) ϕ 0 ( R d ) λ d ( 1 2 λ m ) 1 2 a 3 λ d λ m + β ( r R ) Φ 0 ( R ) λ m ( 1 a 3 λ d ) 1 2 a 3 λ d λ m ] ,
λ d = ϵ d 1 ϵ d + 3 ϵ s 1 , λ m = ϵ m ϵ s 2 ϵ m + ϵ s .
δ φ ( r ) = E i α ϵ m r 2 , r > R ,
α ( ω ) = R 3 a 3 λ d ( 1 λ m ) λ m 1 2 a 3 λ d λ m .
α 0 = R 3 ϵ s + ϵ d 1 ϵ m ϵ s + ϵ d 1 + 2 ϵ m ,
E ( r 0 ) = ϕ r 0 = E i ϵ m ( 1 + 2 g ) , g ( ω ) = α ( ω ) r 0 3 .
ϵ ( r ) ϕ R ( r ) = ϕ 0 R ( r ) ϵ d 1 3 β ( r R d ) ϕ R ( R d ) + ϵ m ϵ s 3 β ( r R ) ϕ R ( R ) ,
ϕ 0 R ( r ) = 4 π α 0 3 r 0 2 E ( r 0 ) [ r 0 2 r 2 θ ( r r 0 ) 2 r r 0 θ ( r 0 r ) ]
φ 0 R = ϕ 0 R ϵ ( r ) , δ ϕ R ( r ) = 8 π α 0 3 r 0 3 E ( r 0 ) δ φ ( r ) ,
ϕ R ( r ) = 4 π α 0 E i 3 ϵ m r 2 [ 1 + 2 g ( ω ) ] [ 1 + 2 g ( ω s ) ]
A ( ω , ω s ) = 1 + 2 g ( ω ) + 2 g ( ω s ) + 4 g ( ω ) g ( ω s ) 2 .

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