Abstract

We demonstrate detailed simulations and experiments of near-field phase-response in a single silver nanoparticle. The plasmon-photon interaction is directly observed in the vicinity of silver nanoparticles through a near-field scanning optical microscope (NSOM). Our results manifest the correlation of phase-response and size-dependent optical enhancement. Detailed interference behaviors between optical excitation and plasmon mediated re-radiation are revealed on a single particle basis. This observation facilitates nano-applications in controlling the spatial distribution of surface plasmon (SP) modes by means of nanostructures.

©2008 Optical Society of America

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  1. U. Kreibig, B. Schmitz, and H. D. Breuer, “Separation of plasmon-polariton modes of small metal particles,” Phys. Rev. B 36, 5027 (1987).
    [Crossref]
  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]
  3. J. J. Mock, M. Barbic, D. R. Smith, D. A. Schultz, and S. Schultz, “Shape effects in plasmon resonance of individual colloidal silver nanoparticles,” J. Chem. Phys. 116, 6755–6759 (2002).
    [Crossref]
  4. R. P. Van Duyne, J. C. Hulteen, and D. A. Treichel, “Atomic force microscopy and surface-enhanced Raman spectroscopy. I. Ag island films and Ag film over polymer nanosphere surfaces supported on glass,” J. Chem. Phys. 99, 2101–2115 (1993).
    [Crossref]
  5. K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, “Ultrasensitive chemical analysis by Raman spectroscopy,” Chem. Rev. 99, 2957–2976 (1999).
    [Crossref]
  6. M. Moskovits, “Surface-enhanced spectroscopy,” Rev. Mod. Phys. 57, 783–826 (1985).
    [Crossref]
  7. V. P. Drachev, M. D. Thoreson, V. Nashine, E. N. Khaliullin, D. Ben-Amotz, V. J. Davisson, and V. M. Shalaev, “Adaptive silver films for surface-enhanced Raman spectroscopy of biomolecules,” J. Raman Spectrosc. 36, 648–656 (2005).
    [Crossref]
  8. Z. B. Wang et al., “Energy flow around a small particle investigated by classical Mie theory,” Phys. Rev. B 70, 035418 (2004).
    [Crossref]
  9. C. Bohren and D. Huffiman, Absorption and Scattering of Light by Small Particles (John Wiley &Sons, New York, 1982).
  10. S. R. Emory, W. E. Haskins, and S. Nie, “Direct observation of size-dependent optical enhancement in single metal nanoparticles,” J. Am. Chem. Soc. 120, 8009–8010 (1998).
    [Crossref]
  11. J. Prikulis et al., “Phase-sensitive near-field imaging of metal nanoparticles,” J. Appl. Phys. 92, 6211–6214 (2002).
    [Crossref]
  12. A. A. Mikhailovsky, M. A. Petruska, M. I. Stockman, and V. I. Klimov, “Broadband near-field interference spectroscopy of metal nanoparticles using a femtosecond white-light continuum,” Opt. Lett. 28, 1686–1688 (2003).
    [Crossref] [PubMed]
  13. B.-H. Choi, H.-H. Lee, S. Jin, S. Chun, and S.-H. Kim, “Characterization of the optical properties of silver nanoparticle films,” Nanotechnology 18, 075706 (2007).
    [Crossref] [PubMed]
  14. M. I. Stockman, S. V. Faleev, and D. J. Bergman, “Coherent control of femtosecond energy localization in nanosystems,” Phys. Rev. Lett. 88, 067402 (2002).
    [Crossref] [PubMed]
  15. J. F. Wolf, P. E. Hillner, R. Bilewicz, P. Kölsch, and J. P. Rabe, “Novel scanning near-field optical microscope (SNOM)/scanning confocal optical microscope based on normal force distance regulation and bent etched fiber tips,” Rev. Sci. Instrum. 70, 2751 (1999).
    [Crossref]

2007 (1)

B.-H. Choi, H.-H. Lee, S. Jin, S. Chun, and S.-H. Kim, “Characterization of the optical properties of silver nanoparticle films,” Nanotechnology 18, 075706 (2007).
[Crossref] [PubMed]

2005 (1)

V. P. Drachev, M. D. Thoreson, V. Nashine, E. N. Khaliullin, D. Ben-Amotz, V. J. Davisson, and V. M. Shalaev, “Adaptive silver films for surface-enhanced Raman spectroscopy of biomolecules,” J. Raman Spectrosc. 36, 648–656 (2005).
[Crossref]

2004 (1)

Z. B. Wang et al., “Energy flow around a small particle investigated by classical Mie theory,” Phys. Rev. B 70, 035418 (2004).
[Crossref]

2003 (1)

2002 (3)

J. Prikulis et al., “Phase-sensitive near-field imaging of metal nanoparticles,” J. Appl. Phys. 92, 6211–6214 (2002).
[Crossref]

M. I. Stockman, S. V. Faleev, and D. J. Bergman, “Coherent control of femtosecond energy localization in nanosystems,” Phys. Rev. Lett. 88, 067402 (2002).
[Crossref] [PubMed]

J. J. Mock, M. Barbic, D. R. Smith, D. A. Schultz, and S. Schultz, “Shape effects in plasmon resonance of individual colloidal silver nanoparticles,” J. Chem. Phys. 116, 6755–6759 (2002).
[Crossref]

1999 (2)

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, “Ultrasensitive chemical analysis by Raman spectroscopy,” Chem. Rev. 99, 2957–2976 (1999).
[Crossref]

J. F. Wolf, P. E. Hillner, R. Bilewicz, P. Kölsch, and J. P. Rabe, “Novel scanning near-field optical microscope (SNOM)/scanning confocal optical microscope based on normal force distance regulation and bent etched fiber tips,” Rev. Sci. Instrum. 70, 2751 (1999).
[Crossref]

1998 (1)

S. R. Emory, W. E. Haskins, and S. Nie, “Direct observation of size-dependent optical enhancement in single metal nanoparticles,” J. Am. Chem. Soc. 120, 8009–8010 (1998).
[Crossref]

1997 (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]

1993 (1)

R. P. Van Duyne, J. C. Hulteen, and D. A. Treichel, “Atomic force microscopy and surface-enhanced Raman spectroscopy. I. Ag island films and Ag film over polymer nanosphere surfaces supported on glass,” J. Chem. Phys. 99, 2101–2115 (1993).
[Crossref]

1987 (1)

U. Kreibig, B. Schmitz, and H. D. Breuer, “Separation of plasmon-polariton modes of small metal particles,” Phys. Rev. B 36, 5027 (1987).
[Crossref]

1985 (1)

M. Moskovits, “Surface-enhanced spectroscopy,” Rev. Mod. Phys. 57, 783–826 (1985).
[Crossref]

Barbic, M.

J. J. Mock, M. Barbic, D. R. Smith, D. A. Schultz, and S. Schultz, “Shape effects in plasmon resonance of individual colloidal silver nanoparticles,” J. Chem. Phys. 116, 6755–6759 (2002).
[Crossref]

Ben-Amotz, D.

V. P. Drachev, M. D. Thoreson, V. Nashine, E. N. Khaliullin, D. Ben-Amotz, V. J. Davisson, and V. M. Shalaev, “Adaptive silver films for surface-enhanced Raman spectroscopy of biomolecules,” J. Raman Spectrosc. 36, 648–656 (2005).
[Crossref]

Bergman, D. J.

M. I. Stockman, S. V. Faleev, and D. J. Bergman, “Coherent control of femtosecond energy localization in nanosystems,” Phys. Rev. Lett. 88, 067402 (2002).
[Crossref] [PubMed]

Bilewicz, R.

J. F. Wolf, P. E. Hillner, R. Bilewicz, P. Kölsch, and J. P. Rabe, “Novel scanning near-field optical microscope (SNOM)/scanning confocal optical microscope based on normal force distance regulation and bent etched fiber tips,” Rev. Sci. Instrum. 70, 2751 (1999).
[Crossref]

Bohren, C.

C. Bohren and D. Huffiman, Absorption and Scattering of Light by Small Particles (John Wiley &Sons, New York, 1982).

Breuer, H. D.

U. Kreibig, B. Schmitz, and H. D. Breuer, “Separation of plasmon-polariton modes of small metal particles,” Phys. Rev. B 36, 5027 (1987).
[Crossref]

Choi, B.-H.

B.-H. Choi, H.-H. Lee, S. Jin, S. Chun, and S.-H. Kim, “Characterization of the optical properties of silver nanoparticle films,” Nanotechnology 18, 075706 (2007).
[Crossref] [PubMed]

Chun, S.

B.-H. Choi, H.-H. Lee, S. Jin, S. Chun, and S.-H. Kim, “Characterization of the optical properties of silver nanoparticle films,” Nanotechnology 18, 075706 (2007).
[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. 99, 2957–2976 (1999).
[Crossref]

Davisson, V. J.

V. P. Drachev, M. D. Thoreson, V. Nashine, E. N. Khaliullin, D. Ben-Amotz, V. J. Davisson, and V. M. Shalaev, “Adaptive silver films for surface-enhanced Raman spectroscopy of biomolecules,” J. Raman Spectrosc. 36, 648–656 (2005).
[Crossref]

Drachev, V. P.

V. P. Drachev, M. D. Thoreson, V. Nashine, E. N. Khaliullin, D. Ben-Amotz, V. J. Davisson, and V. M. Shalaev, “Adaptive silver films for surface-enhanced Raman spectroscopy of biomolecules,” J. Raman Spectrosc. 36, 648–656 (2005).
[Crossref]

Emory, S. R.

S. R. Emory, W. E. Haskins, and S. Nie, “Direct observation of size-dependent optical enhancement in single metal nanoparticles,” J. Am. Chem. Soc. 120, 8009–8010 (1998).
[Crossref]

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

Faleev, S. V.

M. I. Stockman, S. V. Faleev, and D. J. Bergman, “Coherent control of femtosecond energy localization in nanosystems,” Phys. Rev. Lett. 88, 067402 (2002).
[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. 99, 2957–2976 (1999).
[Crossref]

Haskins, W. E.

S. R. Emory, W. E. Haskins, and S. Nie, “Direct observation of size-dependent optical enhancement in single metal nanoparticles,” J. Am. Chem. Soc. 120, 8009–8010 (1998).
[Crossref]

Hillner, P. E.

J. F. Wolf, P. E. Hillner, R. Bilewicz, P. Kölsch, and J. P. Rabe, “Novel scanning near-field optical microscope (SNOM)/scanning confocal optical microscope based on normal force distance regulation and bent etched fiber tips,” Rev. Sci. Instrum. 70, 2751 (1999).
[Crossref]

Huffiman, D.

C. Bohren and D. Huffiman, Absorption and Scattering of Light by Small Particles (John Wiley &Sons, New York, 1982).

Hulteen, J. C.

R. P. Van Duyne, J. C. Hulteen, and D. A. Treichel, “Atomic force microscopy and surface-enhanced Raman spectroscopy. I. Ag island films and Ag film over polymer nanosphere surfaces supported on glass,” J. Chem. Phys. 99, 2101–2115 (1993).
[Crossref]

Itzkan, I.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, “Ultrasensitive chemical analysis by Raman spectroscopy,” Chem. Rev. 99, 2957–2976 (1999).
[Crossref]

Jin, S.

B.-H. Choi, H.-H. Lee, S. Jin, S. Chun, and S.-H. Kim, “Characterization of the optical properties of silver nanoparticle films,” Nanotechnology 18, 075706 (2007).
[Crossref] [PubMed]

Khaliullin, E. N.

V. P. Drachev, M. D. Thoreson, V. Nashine, E. N. Khaliullin, D. Ben-Amotz, V. J. Davisson, and V. M. Shalaev, “Adaptive silver films for surface-enhanced Raman spectroscopy of biomolecules,” J. Raman Spectrosc. 36, 648–656 (2005).
[Crossref]

Kim, S.-H.

B.-H. Choi, H.-H. Lee, S. Jin, S. Chun, and S.-H. Kim, “Characterization of the optical properties of silver nanoparticle films,” Nanotechnology 18, 075706 (2007).
[Crossref] [PubMed]

Klimov, V. I.

Kneipp, H.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, “Ultrasensitive chemical analysis by Raman spectroscopy,” Chem. Rev. 99, 2957–2976 (1999).
[Crossref]

Kneipp, K.

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, “Ultrasensitive chemical analysis by Raman spectroscopy,” Chem. Rev. 99, 2957–2976 (1999).
[Crossref]

Kölsch, P.

J. F. Wolf, P. E. Hillner, R. Bilewicz, P. Kölsch, and J. P. Rabe, “Novel scanning near-field optical microscope (SNOM)/scanning confocal optical microscope based on normal force distance regulation and bent etched fiber tips,” Rev. Sci. Instrum. 70, 2751 (1999).
[Crossref]

Kreibig, U.

U. Kreibig, B. Schmitz, and H. D. Breuer, “Separation of plasmon-polariton modes of small metal particles,” Phys. Rev. B 36, 5027 (1987).
[Crossref]

Lee, H.-H.

B.-H. Choi, H.-H. Lee, S. Jin, S. Chun, and S.-H. Kim, “Characterization of the optical properties of silver nanoparticle films,” Nanotechnology 18, 075706 (2007).
[Crossref] [PubMed]

Mikhailovsky, A. A.

Mock, J. J.

J. J. Mock, M. Barbic, D. R. Smith, D. A. Schultz, and S. Schultz, “Shape effects in plasmon resonance of individual colloidal silver nanoparticles,” J. Chem. Phys. 116, 6755–6759 (2002).
[Crossref]

Moskovits, M.

M. Moskovits, “Surface-enhanced spectroscopy,” Rev. Mod. Phys. 57, 783–826 (1985).
[Crossref]

Nashine, V.

V. P. Drachev, M. D. Thoreson, V. Nashine, E. N. Khaliullin, D. Ben-Amotz, V. J. Davisson, and V. M. Shalaev, “Adaptive silver films for surface-enhanced Raman spectroscopy of biomolecules,” J. Raman Spectrosc. 36, 648–656 (2005).
[Crossref]

Nie, S.

S. R. Emory, W. E. Haskins, and S. Nie, “Direct observation of size-dependent optical enhancement in single metal nanoparticles,” J. Am. Chem. Soc. 120, 8009–8010 (1998).
[Crossref]

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

Petruska, M. A.

Prikulis, J.

J. Prikulis et al., “Phase-sensitive near-field imaging of metal nanoparticles,” J. Appl. Phys. 92, 6211–6214 (2002).
[Crossref]

Rabe, J. P.

J. F. Wolf, P. E. Hillner, R. Bilewicz, P. Kölsch, and J. P. Rabe, “Novel scanning near-field optical microscope (SNOM)/scanning confocal optical microscope based on normal force distance regulation and bent etched fiber tips,” Rev. Sci. Instrum. 70, 2751 (1999).
[Crossref]

Schmitz, B.

U. Kreibig, B. Schmitz, and H. D. Breuer, “Separation of plasmon-polariton modes of small metal particles,” Phys. Rev. B 36, 5027 (1987).
[Crossref]

Schultz, D. A.

J. J. Mock, M. Barbic, D. R. Smith, D. A. Schultz, and S. Schultz, “Shape effects in plasmon resonance of individual colloidal silver nanoparticles,” J. Chem. Phys. 116, 6755–6759 (2002).
[Crossref]

Schultz, S.

J. J. Mock, M. Barbic, D. R. Smith, D. A. Schultz, and S. Schultz, “Shape effects in plasmon resonance of individual colloidal silver nanoparticles,” J. Chem. Phys. 116, 6755–6759 (2002).
[Crossref]

Shalaev, V. M.

V. P. Drachev, M. D. Thoreson, V. Nashine, E. N. Khaliullin, D. Ben-Amotz, V. J. Davisson, and V. M. Shalaev, “Adaptive silver films for surface-enhanced Raman spectroscopy of biomolecules,” J. Raman Spectrosc. 36, 648–656 (2005).
[Crossref]

Smith, D. R.

J. J. Mock, M. Barbic, D. R. Smith, D. A. Schultz, and S. Schultz, “Shape effects in plasmon resonance of individual colloidal silver nanoparticles,” J. Chem. Phys. 116, 6755–6759 (2002).
[Crossref]

Stockman, M. I.

Thoreson, M. D.

V. P. Drachev, M. D. Thoreson, V. Nashine, E. N. Khaliullin, D. Ben-Amotz, V. J. Davisson, and V. M. Shalaev, “Adaptive silver films for surface-enhanced Raman spectroscopy of biomolecules,” J. Raman Spectrosc. 36, 648–656 (2005).
[Crossref]

Treichel, D. A.

R. P. Van Duyne, J. C. Hulteen, and D. A. Treichel, “Atomic force microscopy and surface-enhanced Raman spectroscopy. I. Ag island films and Ag film over polymer nanosphere surfaces supported on glass,” J. Chem. Phys. 99, 2101–2115 (1993).
[Crossref]

Van Duyne, R. P.

R. P. Van Duyne, J. C. Hulteen, and D. A. Treichel, “Atomic force microscopy and surface-enhanced Raman spectroscopy. I. Ag island films and Ag film over polymer nanosphere surfaces supported on glass,” J. Chem. Phys. 99, 2101–2115 (1993).
[Crossref]

Wang, Z. B.

Z. B. Wang et al., “Energy flow around a small particle investigated by classical Mie theory,” Phys. Rev. B 70, 035418 (2004).
[Crossref]

Wolf, J. F.

J. F. Wolf, P. E. Hillner, R. Bilewicz, P. Kölsch, and J. P. Rabe, “Novel scanning near-field optical microscope (SNOM)/scanning confocal optical microscope based on normal force distance regulation and bent etched fiber tips,” Rev. Sci. Instrum. 70, 2751 (1999).
[Crossref]

Chem. Rev. (1)

K. Kneipp, H. Kneipp, I. Itzkan, R. R. Dasari, and M. S. Feld, “Ultrasensitive chemical analysis by Raman spectroscopy,” Chem. Rev. 99, 2957–2976 (1999).
[Crossref]

J. Am. Chem. Soc. (1)

S. R. Emory, W. E. Haskins, and S. Nie, “Direct observation of size-dependent optical enhancement in single metal nanoparticles,” J. Am. Chem. Soc. 120, 8009–8010 (1998).
[Crossref]

J. Appl. Phys. (1)

J. Prikulis et al., “Phase-sensitive near-field imaging of metal nanoparticles,” J. Appl. Phys. 92, 6211–6214 (2002).
[Crossref]

J. Chem. Phys. (2)

J. J. Mock, M. Barbic, D. R. Smith, D. A. Schultz, and S. Schultz, “Shape effects in plasmon resonance of individual colloidal silver nanoparticles,” J. Chem. Phys. 116, 6755–6759 (2002).
[Crossref]

R. P. Van Duyne, J. C. Hulteen, and D. A. Treichel, “Atomic force microscopy and surface-enhanced Raman spectroscopy. I. Ag island films and Ag film over polymer nanosphere surfaces supported on glass,” J. Chem. Phys. 99, 2101–2115 (1993).
[Crossref]

J. Raman Spectrosc. (1)

V. P. Drachev, M. D. Thoreson, V. Nashine, E. N. Khaliullin, D. Ben-Amotz, V. J. Davisson, and V. M. Shalaev, “Adaptive silver films for surface-enhanced Raman spectroscopy of biomolecules,” J. Raman Spectrosc. 36, 648–656 (2005).
[Crossref]

Nanotechnology (1)

B.-H. Choi, H.-H. Lee, S. Jin, S. Chun, and S.-H. Kim, “Characterization of the optical properties of silver nanoparticle films,” Nanotechnology 18, 075706 (2007).
[Crossref] [PubMed]

Opt. Lett. (1)

Phys. Rev. B (2)

Z. B. Wang et al., “Energy flow around a small particle investigated by classical Mie theory,” Phys. Rev. B 70, 035418 (2004).
[Crossref]

U. Kreibig, B. Schmitz, and H. D. Breuer, “Separation of plasmon-polariton modes of small metal particles,” Phys. Rev. B 36, 5027 (1987).
[Crossref]

Phys. Rev. Lett. (1)

M. I. Stockman, S. V. Faleev, and D. J. Bergman, “Coherent control of femtosecond energy localization in nanosystems,” Phys. Rev. Lett. 88, 067402 (2002).
[Crossref] [PubMed]

Rev. Mod. Phys. (1)

M. Moskovits, “Surface-enhanced spectroscopy,” Rev. Mod. Phys. 57, 783–826 (1985).
[Crossref]

Rev. Sci. Instrum. (1)

J. F. Wolf, P. E. Hillner, R. Bilewicz, P. Kölsch, and J. P. Rabe, “Novel scanning near-field optical microscope (SNOM)/scanning confocal optical microscope based on normal force distance regulation and bent etched fiber tips,” Rev. Sci. Instrum. 70, 2751 (1999).
[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]

Other (1)

C. Bohren and D. Huffiman, Absorption and Scattering of Light by Small Particles (John Wiley &Sons, New York, 1982).

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Figures (4)

Fig. 1.
Fig. 1.

(a). NSOM setup. (b) The absorption spectrum of Ag nanoparticles. The spectral positions of the NSOM excitations are shown with RGB lines. Inset: SEM image of Ag nanoparticles.

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Fig. 2.
Fig. 2.

Simulation results of the far-field interference from Etip and Es with phase difference (a) ϕ=0, (b) ϕ=π/2, and (c) ϕ=π. (d) Their cross-sectional views are combined in (d), showing the dramatic difference between on- and off-resonance.

Download Full Size | PPT Slide | PDF

Fig. 3.
Fig. 3.

Measured NSOM images of a 50-nm nanoparticle with (a) λ=633 nm, (b) λ=532 nm, and (c) λ=488 nm. Their cross-sectional views are combined in (d).

Download Full Size | PPT Slide | PDF

Fig. 4.
Fig. 4.

Particle size spectra for RGB excitations. The tendency of shorter wavelength resonant with smaller silver nanoparticles is evident.

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Equations (4)

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

E tip ( r ) ∝ exp ⁡ [ i ( k r − ω t ) ] [ A k r + B exp ⁡ ( − r η ) ] ,
P = α E tip ,
α = ∣ α ∣ exp ⁡ ( i ϕ ) ,
E s ( r 1 ) ≈ [ Z 0 k 2 ( 4 π i k r 1 ) ] d P d t [ exp ⁡ ( − i k r 1 ) ] ,

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