Abstract

We present a comparative study on the enhancement of photoluminescence and Raman processes by a single metal nanoparticle. Taking an analytical approach, we show the physics behind strikingly different orders of magnitude in enhancement that have been observed, provide fundamental explanation for not observing quenching of Raman processes, and outline the path to optimization of both photoluminescence and Raman enhancement.

© 2012 Optical Society of America

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  1. M. Fleischmann, P. J. Hendra, and A. J. McQuillan, Chem. Phys. Lett. 26, 163 (1974).
    [CrossRef]
  2. S. Nie and S. R. Emory, Science 275, 1102 (1997).
    [CrossRef]
  3. M. Bakker, V. P. Drachev, Z. Liu, H.-K. Yuan, R. H. Pedersen, A. Boltasseva, J. Chen, J. Irudayaraj, A. V. Kildishev, and V. M. Shalaev, New J. Phys. 10, 125022 (2008).
    [CrossRef]
  4. D. A. Weitz, S. Garoff, J. I. Gersten, and A. Nitzan, J. Chem. Phys. 78, 5324 (1983).
    [CrossRef]
  5. B. Pettinger, J. Chem. Phys. 85, 7442 (1986).
    [CrossRef]
  6. P. Bharadwaj, B. Deutsch, and L. Novotny, Adv. Opt. Photon. 1, 438 (2009).
    [CrossRef]
  7. H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, Phys. Rev. Lett. 93, 243002 (2004).
    [CrossRef]
  8. E. Dulkeith, A. C. Morteani, T. Niedereichholz, T. A. Klar, and J. Feldmann, Phys. Rev. Lett. 89, 203002 (2002).
    [CrossRef]
  9. G. Sun, J. B. Khurgin, and A. Bratkovsky, Phys. Rev. B 84, 045415 (2011).
    [CrossRef]
  10. G. Sun, J. B. Khurgin, and C. C. Yang, Appl. Phys. Lett. 95, 171103 (2009).
    [CrossRef]
  11. P. B. Johnson and R. W. Christy, Phys. Rev. B 6, 4370 (1972).
    [CrossRef]

2011 (1)

G. Sun, J. B. Khurgin, and A. Bratkovsky, Phys. Rev. B 84, 045415 (2011).
[CrossRef]

2009 (2)

G. Sun, J. B. Khurgin, and C. C. Yang, Appl. Phys. Lett. 95, 171103 (2009).
[CrossRef]

P. Bharadwaj, B. Deutsch, and L. Novotny, Adv. Opt. Photon. 1, 438 (2009).
[CrossRef]

2008 (1)

M. Bakker, V. P. Drachev, Z. Liu, H.-K. Yuan, R. H. Pedersen, A. Boltasseva, J. Chen, J. Irudayaraj, A. V. Kildishev, and V. M. Shalaev, New J. Phys. 10, 125022 (2008).
[CrossRef]

2004 (1)

H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, Phys. Rev. Lett. 93, 243002 (2004).
[CrossRef]

2002 (1)

E. Dulkeith, A. C. Morteani, T. Niedereichholz, T. A. Klar, and J. Feldmann, Phys. Rev. Lett. 89, 203002 (2002).
[CrossRef]

1997 (1)

S. Nie and S. R. Emory, Science 275, 1102 (1997).
[CrossRef]

1986 (1)

B. Pettinger, J. Chem. Phys. 85, 7442 (1986).
[CrossRef]

1983 (1)

D. A. Weitz, S. Garoff, J. I. Gersten, and A. Nitzan, J. Chem. Phys. 78, 5324 (1983).
[CrossRef]

1974 (1)

M. Fleischmann, P. J. Hendra, and A. J. McQuillan, Chem. Phys. Lett. 26, 163 (1974).
[CrossRef]

1972 (1)

P. B. Johnson and R. W. Christy, Phys. Rev. B 6, 4370 (1972).
[CrossRef]

Bakker, M.

M. Bakker, V. P. Drachev, Z. Liu, H.-K. Yuan, R. H. Pedersen, A. Boltasseva, J. Chen, J. Irudayaraj, A. V. Kildishev, and V. M. Shalaev, New J. Phys. 10, 125022 (2008).
[CrossRef]

Bharadwaj, P.

Boltasseva, A.

M. Bakker, V. P. Drachev, Z. Liu, H.-K. Yuan, R. H. Pedersen, A. Boltasseva, J. Chen, J. Irudayaraj, A. V. Kildishev, and V. M. Shalaev, New J. Phys. 10, 125022 (2008).
[CrossRef]

Bratkovsky, A.

G. Sun, J. B. Khurgin, and A. Bratkovsky, Phys. Rev. B 84, 045415 (2011).
[CrossRef]

Chen, J.

M. Bakker, V. P. Drachev, Z. Liu, H.-K. Yuan, R. H. Pedersen, A. Boltasseva, J. Chen, J. Irudayaraj, A. V. Kildishev, and V. M. Shalaev, New J. Phys. 10, 125022 (2008).
[CrossRef]

Christy, R. W.

P. B. Johnson and R. W. Christy, Phys. Rev. B 6, 4370 (1972).
[CrossRef]

Deutsch, B.

Drachev, V. P.

M. Bakker, V. P. Drachev, Z. Liu, H.-K. Yuan, R. H. Pedersen, A. Boltasseva, J. Chen, J. Irudayaraj, A. V. Kildishev, and V. M. Shalaev, New J. Phys. 10, 125022 (2008).
[CrossRef]

Dulkeith, E.

E. Dulkeith, A. C. Morteani, T. Niedereichholz, T. A. Klar, and J. Feldmann, Phys. Rev. Lett. 89, 203002 (2002).
[CrossRef]

Emory, S. R.

S. Nie and S. R. Emory, Science 275, 1102 (1997).
[CrossRef]

Feldmann, J.

E. Dulkeith, A. C. Morteani, T. Niedereichholz, T. A. Klar, and J. Feldmann, Phys. Rev. Lett. 89, 203002 (2002).
[CrossRef]

Fleischmann, M.

M. Fleischmann, P. J. Hendra, and A. J. McQuillan, Chem. Phys. Lett. 26, 163 (1974).
[CrossRef]

Garoff, S.

D. A. Weitz, S. Garoff, J. I. Gersten, and A. Nitzan, J. Chem. Phys. 78, 5324 (1983).
[CrossRef]

Gersten, J. I.

D. A. Weitz, S. Garoff, J. I. Gersten, and A. Nitzan, J. Chem. Phys. 78, 5324 (1983).
[CrossRef]

Hendra, P. J.

M. Fleischmann, P. J. Hendra, and A. J. McQuillan, Chem. Phys. Lett. 26, 163 (1974).
[CrossRef]

Irudayaraj, J.

M. Bakker, V. P. Drachev, Z. Liu, H.-K. Yuan, R. H. Pedersen, A. Boltasseva, J. Chen, J. Irudayaraj, A. V. Kildishev, and V. M. Shalaev, New J. Phys. 10, 125022 (2008).
[CrossRef]

Johansson, P.

H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, Phys. Rev. Lett. 93, 243002 (2004).
[CrossRef]

Johnson, P. B.

P. B. Johnson and R. W. Christy, Phys. Rev. B 6, 4370 (1972).
[CrossRef]

Käll, M.

H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, Phys. Rev. Lett. 93, 243002 (2004).
[CrossRef]

Khurgin, J. B.

G. Sun, J. B. Khurgin, and A. Bratkovsky, Phys. Rev. B 84, 045415 (2011).
[CrossRef]

G. Sun, J. B. Khurgin, and C. C. Yang, Appl. Phys. Lett. 95, 171103 (2009).
[CrossRef]

Kildishev, A. V.

M. Bakker, V. P. Drachev, Z. Liu, H.-K. Yuan, R. H. Pedersen, A. Boltasseva, J. Chen, J. Irudayaraj, A. V. Kildishev, and V. M. Shalaev, New J. Phys. 10, 125022 (2008).
[CrossRef]

Klar, T. A.

E. Dulkeith, A. C. Morteani, T. Niedereichholz, T. A. Klar, and J. Feldmann, Phys. Rev. Lett. 89, 203002 (2002).
[CrossRef]

Liu, Z.

M. Bakker, V. P. Drachev, Z. Liu, H.-K. Yuan, R. H. Pedersen, A. Boltasseva, J. Chen, J. Irudayaraj, A. V. Kildishev, and V. M. Shalaev, New J. Phys. 10, 125022 (2008).
[CrossRef]

McQuillan, A. J.

M. Fleischmann, P. J. Hendra, and A. J. McQuillan, Chem. Phys. Lett. 26, 163 (1974).
[CrossRef]

Morteani, A. C.

E. Dulkeith, A. C. Morteani, T. Niedereichholz, T. A. Klar, and J. Feldmann, Phys. Rev. Lett. 89, 203002 (2002).
[CrossRef]

Nie, S.

S. Nie and S. R. Emory, Science 275, 1102 (1997).
[CrossRef]

Niedereichholz, T.

E. Dulkeith, A. C. Morteani, T. Niedereichholz, T. A. Klar, and J. Feldmann, Phys. Rev. Lett. 89, 203002 (2002).
[CrossRef]

Nitzan, A.

D. A. Weitz, S. Garoff, J. I. Gersten, and A. Nitzan, J. Chem. Phys. 78, 5324 (1983).
[CrossRef]

Novotny, L.

Pedersen, R. H.

M. Bakker, V. P. Drachev, Z. Liu, H.-K. Yuan, R. H. Pedersen, A. Boltasseva, J. Chen, J. Irudayaraj, A. V. Kildishev, and V. M. Shalaev, New J. Phys. 10, 125022 (2008).
[CrossRef]

Persson, M. P.

H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, Phys. Rev. Lett. 93, 243002 (2004).
[CrossRef]

Pettinger, B.

B. Pettinger, J. Chem. Phys. 85, 7442 (1986).
[CrossRef]

Shalaev, V. M.

M. Bakker, V. P. Drachev, Z. Liu, H.-K. Yuan, R. H. Pedersen, A. Boltasseva, J. Chen, J. Irudayaraj, A. V. Kildishev, and V. M. Shalaev, New J. Phys. 10, 125022 (2008).
[CrossRef]

Sun, G.

G. Sun, J. B. Khurgin, and A. Bratkovsky, Phys. Rev. B 84, 045415 (2011).
[CrossRef]

G. Sun, J. B. Khurgin, and C. C. Yang, Appl. Phys. Lett. 95, 171103 (2009).
[CrossRef]

Wang, X.-H.

H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, Phys. Rev. Lett. 93, 243002 (2004).
[CrossRef]

Weitz, D. A.

D. A. Weitz, S. Garoff, J. I. Gersten, and A. Nitzan, J. Chem. Phys. 78, 5324 (1983).
[CrossRef]

Xu, H.

H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, Phys. Rev. Lett. 93, 243002 (2004).
[CrossRef]

Xu, H. Q.

H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, Phys. Rev. Lett. 93, 243002 (2004).
[CrossRef]

Yang, C. C.

G. Sun, J. B. Khurgin, and C. C. Yang, Appl. Phys. Lett. 95, 171103 (2009).
[CrossRef]

Yuan, H.-K.

M. Bakker, V. P. Drachev, Z. Liu, H.-K. Yuan, R. H. Pedersen, A. Boltasseva, J. Chen, J. Irudayaraj, A. V. Kildishev, and V. M. Shalaev, New J. Phys. 10, 125022 (2008).
[CrossRef]

Adv. Opt. Photon. (1)

Appl. Phys. Lett. (1)

G. Sun, J. B. Khurgin, and C. C. Yang, Appl. Phys. Lett. 95, 171103 (2009).
[CrossRef]

Chem. Phys. Lett. (1)

M. Fleischmann, P. J. Hendra, and A. J. McQuillan, Chem. Phys. Lett. 26, 163 (1974).
[CrossRef]

J. Chem. Phys. (2)

D. A. Weitz, S. Garoff, J. I. Gersten, and A. Nitzan, J. Chem. Phys. 78, 5324 (1983).
[CrossRef]

B. Pettinger, J. Chem. Phys. 85, 7442 (1986).
[CrossRef]

New J. Phys. (1)

M. Bakker, V. P. Drachev, Z. Liu, H.-K. Yuan, R. H. Pedersen, A. Boltasseva, J. Chen, J. Irudayaraj, A. V. Kildishev, and V. M. Shalaev, New J. Phys. 10, 125022 (2008).
[CrossRef]

Phys. Rev. B (2)

G. Sun, J. B. Khurgin, and A. Bratkovsky, Phys. Rev. B 84, 045415 (2011).
[CrossRef]

P. B. Johnson and R. W. Christy, Phys. Rev. B 6, 4370 (1972).
[CrossRef]

Phys. Rev. Lett. (2)

H. Xu, X.-H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, Phys. Rev. Lett. 93, 243002 (2004).
[CrossRef]

E. Dulkeith, A. C. Morteani, T. Niedereichholz, T. A. Klar, and J. Feldmann, Phys. Rev. Lett. 89, 203002 (2002).
[CrossRef]

Science (1)

S. Nie and S. R. Emory, Science 275, 1102 (1997).
[CrossRef]

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Figures (2)

Fig. 1.
Fig. 1.

Illustration of energy-transfer processes in (a) PL enhancement and (b) Raman enhancement.

Fig. 2.
Fig. 2.

Raman and PL enhancement for molecules with σabs=0.1nm2 and 104ηrad101 for an Au sphere of a=30nm. Excitations for both processes are at the dipole-mode resonance ωex=ω1=2.562eV, and PL and Stokes Raman emission are both at ωPL=ωS=2.462eV. (Inset: PL enhancement dependence on sphere radius a and separation d.)

Equations (4)

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

Fabs(ωex)=|Emax,1Efoc|2(aa+d)6=2[γabsωex+γωex+γradωex]2+δ2(aa+d)6
Fem(ωs)=1+ηoutFP,1(ωS)1+ηradl=1FP,l(ωPS).
γRM=2π|dmEex|22(ωexωm)2|Heν|22(ωSωm)2|dm|2ωSε0ρ(ωS),
FRM(ωex,ωS)=|Emax,1Efoc|2(aa+d)6[1+ηoutFP,1(ωS)].

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