Abstract

We report on an experiment with surface-enhanced Raman scattering on gratings overcoated by copper phtalocyanine that shows that, because of the resonant excitation of surface plasmons, a stimulated Raman scattering process occurs. The corresponding threshold value of the pump power is rather low, of the order of 40 mW. This observation was made with a thin (5-nm) film of copper phtalocyanine. The theoretical study is developed by coupled-mode analysis that makes full use of the electromagnetic resonant feature of this nonlinear interaction.

© 1996 Optical Society of America

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  1. M. Fleischmann, P. J. Hendra, and A. J. McQuillan, Chem. Phys. Lett. 26, 123 (1974); D. L. Jeanmaire and R. P. Van Duyne, J. Electroanal. Chem. 84, 1 (1977); M. G. Albrecht and J. A. Creighton, J. Am. Chem. Soc. 99, 5215 (1977).
    [Crossref]
  2. R. K. Chang and T. E. Furtak, eds., Surface Enhanced Raman Scattering (Plenum, New York, 1982).
    [Crossref]
  3. A. Otto, Phys. Status Solidi. 26, 99 (1968); E. Kretschmann and A. Raether, Z. Naturforsch. 23a, 2135 (1968).
    [Crossref]
  4. M. C. Hutley and D. Maystre, Opt. Commun. 19, 431 (1976).
    [Crossref]
  5. W. H. Weber and G. W. Ford, Opt. Lett. 6, 122 (1981).
    [Crossref] [PubMed]
  6. W. Knoll, M. R. Philpott, J. D. Swalen, and A. Girlando, J. Chem. Phys. 77, 2254 (1982).
    [Crossref]
  7. S. Ushioda and Y. Sasaki, Phys. Rev. B 27, 1401 (1983).
    [Crossref]
  8. I. Baltog, N. Primeau, R. Reinisch, and J. L. Coutaz, Appl. Phys. Lett. 66, 1187 (1995).
    [Crossref]
  9. A. N. Sudarkin and K. N. Ushakov, Sov. Phys. JETP 69, 317 (1989).
  10. A. N. Sudarkin and K. N. Ushakov, in Quantum Electronics and Laser Science, Vol. 13 of 1992 OSA Technical Digest Series (Optical Society of America, Washington, D.C., 1992), paper FrG4.
  11. S. Hayashi and M. Samejima, Surf. Sci. 137, 442 (1984).
    [Crossref]
  12. N. Primeau, J. L. Coutaz, and L. Abello, J. Appl. Phys. 73, 5158 (1993).
    [Crossref]
  13. C. Jennings, R. Aroca, A. Ho, and R. O. Loutfy, Anal. Chem. 56, 2033 (1984).
    [Crossref]
  14. B. H. Schechtman and W. E. Spicer, J. Mol. Spectrosc. 33, 28 (1970).
    [Crossref]
  15. C. Vassalo, Théorie des Guides d’Ondes Électromagnétiques (Centre National d’Etude des Telecommunications—Ecole Nationale Superieure des Telecommunications, Eyrolles, Paris, 1985).
  16. H. Kogelnik, in Integrated Optics, T. Tamir, ed., Vol. 7 of Topics in Applied Physics (Springer-Verlag, New York, 1975), pp. 13–81.
  17. R. Reinisch, G. Vitrant, and M. Haelterman, Phys. Rev. B 44, 7870 (1991).
    [Crossref]
  18. R. Reinisch, M. Nevière, P. Vincent, and G. Vitrant, Optics Commun. 91, 51 (1992).
    [Crossref]
  19. R. Reinisch, M. Nevière, E. Popov, and H. Akhouayri, Opt. Commun. 112, 339 (1994).
    [Crossref]
  20. M. Nevière, in Electromagnetic Theory of Gratings, R. Petit, ed. (Springer-Verlag, New York, 1980), pp. 123–157.
    [Crossref]

1995 (1)

I. Baltog, N. Primeau, R. Reinisch, and J. L. Coutaz, Appl. Phys. Lett. 66, 1187 (1995).
[Crossref]

1994 (1)

R. Reinisch, M. Nevière, E. Popov, and H. Akhouayri, Opt. Commun. 112, 339 (1994).
[Crossref]

1993 (1)

N. Primeau, J. L. Coutaz, and L. Abello, J. Appl. Phys. 73, 5158 (1993).
[Crossref]

1992 (1)

R. Reinisch, M. Nevière, P. Vincent, and G. Vitrant, Optics Commun. 91, 51 (1992).
[Crossref]

1991 (1)

R. Reinisch, G. Vitrant, and M. Haelterman, Phys. Rev. B 44, 7870 (1991).
[Crossref]

1989 (1)

A. N. Sudarkin and K. N. Ushakov, Sov. Phys. JETP 69, 317 (1989).

1984 (2)

S. Hayashi and M. Samejima, Surf. Sci. 137, 442 (1984).
[Crossref]

C. Jennings, R. Aroca, A. Ho, and R. O. Loutfy, Anal. Chem. 56, 2033 (1984).
[Crossref]

1983 (1)

S. Ushioda and Y. Sasaki, Phys. Rev. B 27, 1401 (1983).
[Crossref]

1982 (1)

W. Knoll, M. R. Philpott, J. D. Swalen, and A. Girlando, J. Chem. Phys. 77, 2254 (1982).
[Crossref]

1981 (1)

1976 (1)

M. C. Hutley and D. Maystre, Opt. Commun. 19, 431 (1976).
[Crossref]

1974 (1)

M. Fleischmann, P. J. Hendra, and A. J. McQuillan, Chem. Phys. Lett. 26, 123 (1974); D. L. Jeanmaire and R. P. Van Duyne, J. Electroanal. Chem. 84, 1 (1977); M. G. Albrecht and J. A. Creighton, J. Am. Chem. Soc. 99, 5215 (1977).
[Crossref]

1970 (1)

B. H. Schechtman and W. E. Spicer, J. Mol. Spectrosc. 33, 28 (1970).
[Crossref]

1968 (1)

A. Otto, Phys. Status Solidi. 26, 99 (1968); E. Kretschmann and A. Raether, Z. Naturforsch. 23a, 2135 (1968).
[Crossref]

Abello, L.

N. Primeau, J. L. Coutaz, and L. Abello, J. Appl. Phys. 73, 5158 (1993).
[Crossref]

Akhouayri, H.

R. Reinisch, M. Nevière, E. Popov, and H. Akhouayri, Opt. Commun. 112, 339 (1994).
[Crossref]

Aroca, R.

C. Jennings, R. Aroca, A. Ho, and R. O. Loutfy, Anal. Chem. 56, 2033 (1984).
[Crossref]

Baltog, I.

I. Baltog, N. Primeau, R. Reinisch, and J. L. Coutaz, Appl. Phys. Lett. 66, 1187 (1995).
[Crossref]

Coutaz, J. L.

I. Baltog, N. Primeau, R. Reinisch, and J. L. Coutaz, Appl. Phys. Lett. 66, 1187 (1995).
[Crossref]

N. Primeau, J. L. Coutaz, and L. Abello, J. Appl. Phys. 73, 5158 (1993).
[Crossref]

Fleischmann, M.

M. Fleischmann, P. J. Hendra, and A. J. McQuillan, Chem. Phys. Lett. 26, 123 (1974); D. L. Jeanmaire and R. P. Van Duyne, J. Electroanal. Chem. 84, 1 (1977); M. G. Albrecht and J. A. Creighton, J. Am. Chem. Soc. 99, 5215 (1977).
[Crossref]

Ford, G. W.

Girlando, A.

W. Knoll, M. R. Philpott, J. D. Swalen, and A. Girlando, J. Chem. Phys. 77, 2254 (1982).
[Crossref]

Haelterman, M.

R. Reinisch, G. Vitrant, and M. Haelterman, Phys. Rev. B 44, 7870 (1991).
[Crossref]

Hayashi, S.

S. Hayashi and M. Samejima, Surf. Sci. 137, 442 (1984).
[Crossref]

Hendra, P. J.

M. Fleischmann, P. J. Hendra, and A. J. McQuillan, Chem. Phys. Lett. 26, 123 (1974); D. L. Jeanmaire and R. P. Van Duyne, J. Electroanal. Chem. 84, 1 (1977); M. G. Albrecht and J. A. Creighton, J. Am. Chem. Soc. 99, 5215 (1977).
[Crossref]

Ho, A.

C. Jennings, R. Aroca, A. Ho, and R. O. Loutfy, Anal. Chem. 56, 2033 (1984).
[Crossref]

Hutley, M. C.

M. C. Hutley and D. Maystre, Opt. Commun. 19, 431 (1976).
[Crossref]

Jennings, C.

C. Jennings, R. Aroca, A. Ho, and R. O. Loutfy, Anal. Chem. 56, 2033 (1984).
[Crossref]

Knoll, W.

W. Knoll, M. R. Philpott, J. D. Swalen, and A. Girlando, J. Chem. Phys. 77, 2254 (1982).
[Crossref]

Kogelnik, H.

H. Kogelnik, in Integrated Optics, T. Tamir, ed., Vol. 7 of Topics in Applied Physics (Springer-Verlag, New York, 1975), pp. 13–81.

Loutfy, R. O.

C. Jennings, R. Aroca, A. Ho, and R. O. Loutfy, Anal. Chem. 56, 2033 (1984).
[Crossref]

Maystre, D.

M. C. Hutley and D. Maystre, Opt. Commun. 19, 431 (1976).
[Crossref]

McQuillan, A. J.

M. Fleischmann, P. J. Hendra, and A. J. McQuillan, Chem. Phys. Lett. 26, 123 (1974); D. L. Jeanmaire and R. P. Van Duyne, J. Electroanal. Chem. 84, 1 (1977); M. G. Albrecht and J. A. Creighton, J. Am. Chem. Soc. 99, 5215 (1977).
[Crossref]

Nevière, M.

R. Reinisch, M. Nevière, E. Popov, and H. Akhouayri, Opt. Commun. 112, 339 (1994).
[Crossref]

R. Reinisch, M. Nevière, P. Vincent, and G. Vitrant, Optics Commun. 91, 51 (1992).
[Crossref]

M. Nevière, in Electromagnetic Theory of Gratings, R. Petit, ed. (Springer-Verlag, New York, 1980), pp. 123–157.
[Crossref]

Otto, A.

A. Otto, Phys. Status Solidi. 26, 99 (1968); E. Kretschmann and A. Raether, Z. Naturforsch. 23a, 2135 (1968).
[Crossref]

Philpott, M. R.

W. Knoll, M. R. Philpott, J. D. Swalen, and A. Girlando, J. Chem. Phys. 77, 2254 (1982).
[Crossref]

Popov, E.

R. Reinisch, M. Nevière, E. Popov, and H. Akhouayri, Opt. Commun. 112, 339 (1994).
[Crossref]

Primeau, N.

I. Baltog, N. Primeau, R. Reinisch, and J. L. Coutaz, Appl. Phys. Lett. 66, 1187 (1995).
[Crossref]

N. Primeau, J. L. Coutaz, and L. Abello, J. Appl. Phys. 73, 5158 (1993).
[Crossref]

Reinisch, R.

I. Baltog, N. Primeau, R. Reinisch, and J. L. Coutaz, Appl. Phys. Lett. 66, 1187 (1995).
[Crossref]

R. Reinisch, M. Nevière, E. Popov, and H. Akhouayri, Opt. Commun. 112, 339 (1994).
[Crossref]

R. Reinisch, M. Nevière, P. Vincent, and G. Vitrant, Optics Commun. 91, 51 (1992).
[Crossref]

R. Reinisch, G. Vitrant, and M. Haelterman, Phys. Rev. B 44, 7870 (1991).
[Crossref]

Samejima, M.

S. Hayashi and M. Samejima, Surf. Sci. 137, 442 (1984).
[Crossref]

Sasaki, Y.

S. Ushioda and Y. Sasaki, Phys. Rev. B 27, 1401 (1983).
[Crossref]

Schechtman, B. H.

B. H. Schechtman and W. E. Spicer, J. Mol. Spectrosc. 33, 28 (1970).
[Crossref]

Spicer, W. E.

B. H. Schechtman and W. E. Spicer, J. Mol. Spectrosc. 33, 28 (1970).
[Crossref]

Sudarkin, A. N.

A. N. Sudarkin and K. N. Ushakov, Sov. Phys. JETP 69, 317 (1989).

A. N. Sudarkin and K. N. Ushakov, in Quantum Electronics and Laser Science, Vol. 13 of 1992 OSA Technical Digest Series (Optical Society of America, Washington, D.C., 1992), paper FrG4.

Swalen, J. D.

W. Knoll, M. R. Philpott, J. D. Swalen, and A. Girlando, J. Chem. Phys. 77, 2254 (1982).
[Crossref]

Ushakov, K. N.

A. N. Sudarkin and K. N. Ushakov, Sov. Phys. JETP 69, 317 (1989).

A. N. Sudarkin and K. N. Ushakov, in Quantum Electronics and Laser Science, Vol. 13 of 1992 OSA Technical Digest Series (Optical Society of America, Washington, D.C., 1992), paper FrG4.

Ushioda, S.

S. Ushioda and Y. Sasaki, Phys. Rev. B 27, 1401 (1983).
[Crossref]

Vassalo, C.

C. Vassalo, Théorie des Guides d’Ondes Électromagnétiques (Centre National d’Etude des Telecommunications—Ecole Nationale Superieure des Telecommunications, Eyrolles, Paris, 1985).

Vincent, P.

R. Reinisch, M. Nevière, P. Vincent, and G. Vitrant, Optics Commun. 91, 51 (1992).
[Crossref]

Vitrant, G.

R. Reinisch, M. Nevière, P. Vincent, and G. Vitrant, Optics Commun. 91, 51 (1992).
[Crossref]

R. Reinisch, G. Vitrant, and M. Haelterman, Phys. Rev. B 44, 7870 (1991).
[Crossref]

Weber, W. H.

Anal. Chem. (1)

C. Jennings, R. Aroca, A. Ho, and R. O. Loutfy, Anal. Chem. 56, 2033 (1984).
[Crossref]

Appl. Phys. Lett. (1)

I. Baltog, N. Primeau, R. Reinisch, and J. L. Coutaz, Appl. Phys. Lett. 66, 1187 (1995).
[Crossref]

Chem. Phys. Lett. (1)

M. Fleischmann, P. J. Hendra, and A. J. McQuillan, Chem. Phys. Lett. 26, 123 (1974); D. L. Jeanmaire and R. P. Van Duyne, J. Electroanal. Chem. 84, 1 (1977); M. G. Albrecht and J. A. Creighton, J. Am. Chem. Soc. 99, 5215 (1977).
[Crossref]

J. Appl. Phys. (1)

N. Primeau, J. L. Coutaz, and L. Abello, J. Appl. Phys. 73, 5158 (1993).
[Crossref]

J. Chem. Phys. (1)

W. Knoll, M. R. Philpott, J. D. Swalen, and A. Girlando, J. Chem. Phys. 77, 2254 (1982).
[Crossref]

J. Mol. Spectrosc. (1)

B. H. Schechtman and W. E. Spicer, J. Mol. Spectrosc. 33, 28 (1970).
[Crossref]

Opt. Commun. (2)

M. C. Hutley and D. Maystre, Opt. Commun. 19, 431 (1976).
[Crossref]

R. Reinisch, M. Nevière, E. Popov, and H. Akhouayri, Opt. Commun. 112, 339 (1994).
[Crossref]

Opt. Lett. (1)

Optics Commun. (1)

R. Reinisch, M. Nevière, P. Vincent, and G. Vitrant, Optics Commun. 91, 51 (1992).
[Crossref]

Phys. Rev. B (2)

S. Ushioda and Y. Sasaki, Phys. Rev. B 27, 1401 (1983).
[Crossref]

R. Reinisch, G. Vitrant, and M. Haelterman, Phys. Rev. B 44, 7870 (1991).
[Crossref]

Phys. Status Solidi. (1)

A. Otto, Phys. Status Solidi. 26, 99 (1968); E. Kretschmann and A. Raether, Z. Naturforsch. 23a, 2135 (1968).
[Crossref]

Sov. Phys. JETP (1)

A. N. Sudarkin and K. N. Ushakov, Sov. Phys. JETP 69, 317 (1989).

Surf. Sci. (1)

S. Hayashi and M. Samejima, Surf. Sci. 137, 442 (1984).
[Crossref]

Other (5)

C. Vassalo, Théorie des Guides d’Ondes Électromagnétiques (Centre National d’Etude des Telecommunications—Ecole Nationale Superieure des Telecommunications, Eyrolles, Paris, 1985).

H. Kogelnik, in Integrated Optics, T. Tamir, ed., Vol. 7 of Topics in Applied Physics (Springer-Verlag, New York, 1975), pp. 13–81.

A. N. Sudarkin and K. N. Ushakov, in Quantum Electronics and Laser Science, Vol. 13 of 1992 OSA Technical Digest Series (Optical Society of America, Washington, D.C., 1992), paper FrG4.

R. K. Chang and T. E. Furtak, eds., Surface Enhanced Raman Scattering (Plenum, New York, 1982).
[Crossref]

M. Nevière, in Electromagnetic Theory of Gratings, R. Petit, ed. (Springer-Verlag, New York, 1980), pp. 123–157.
[Crossref]

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Figures (3)

Fig. 1
Fig. 1

IRaman/ILaser versus the incident laser intensity. Notice that the vertical scale is logarithmic. Squares: groove depth, 70 nm; filled, at the SP resonance at ωl; open, slightly detuned from the SP resonance at ωl. Circles: groove depth, 35 nm; filled, at the SP resonance at ωl; open, slightly detuned from the SP resonance at ωl. The straight lines are a guide for the eye.

Fig. 2
Fig. 2

Second-order Raman spectrum for an incident power of 50 mW at the SP resonance angle for the 70-nm deep grating. CTS, counts.

Fig. 3
Fig. 3

Geometry for SP-enhanced Raman scattering at a grating.

Equations (27)

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s , z ( x , y ) = c s n H s , n ( y ) exp [ j ( γ s + n σ ) x ] ,
γ ˜ l , p = γ l + q σ for the space harmonic q of the SP at ω l , γ ˜ s , n = γ s + n σ for the space harmonic n of the SP at ω s .
P k NL ( ω l ) = 0 χ k , h , i , j ( ω l ) E s , m , h ( y ) E s , m , i * ( y ) E l , p , j ( y ) | c s | 2 c l × exp [ j ( y ˜ s , m γ ˜ s , m * + γ ˜ l , p ) x ] ,
P j NL ( ω s ) = 0 χ j , h , i , k ( ω s ) E l , p , h ( y ) E l , p , i * ( y ) E s , m , k ( y ) | c l | 2 c s × exp [ j ( y ˜ l , p γ ˜ l , p * + γ ˜ s , m ) x ] .
d c l d x = j ω l ξ l | c s | 2 c l exp [ j ( γ ˜ s , m γ ˜ s , m * ) x ] j τ l A l ( x ) exp [ j ( β + p σ γ ˜ l , p ) x ] ,
d c s d x = j ω s ξ s | c l | 2 c s exp [ j ( γ ˜ l , p γ ˜ l , p * ) x ] ,
β = k ( ω l ) sin θ i , τ l A l ( x ) exp [ j ( β + p σ ) x ] = ω l E l , p t , P L ( x , y ) N l , p ,
ξ l = 0 χ k , h , i , j ( ω l , x , y ) E l , p , k t ( y ) E s , m , h ( y ) E s , m , i * ( y ) E l , p , j ( y ) N l , p ,
ξ s = 0 χ j , h , i , k ( ω s , x , y ) E s , m , j t ( y ) E l , p , h ( y ) E l , p , i * ( y ) E s , m , k ( y ) N s , m .
d c l d x = j τ l A l exp [ j ( β + p σ γ ˜ l , p ) x ] .
c s ( x ) = c s ( 0 ) exp ( ω s ξ s | τ l C l A l | 2 x ) exp ( j ω s ξ s | τ l C l A l | 2 x ) ,
C l = 1 β + p σ γ ˜ l , p ,
ξ s = ξ s + j ξ s .
s , z , m ( x , y ) = c s ( 0 ) H s , m ( y ) exp [ ( ω s ξ s | τ l C l A l | 2 γ ˜ s , m ) x ] × exp [ j ( γ ˜ s , m ω s ξ s | τ l C l A l | 2 ) x ] ,
ξ s > 0
| A l | 2 γ s , m ω s ξ s | τ l C l | 2 .
g s ( θ i , h ) = ω s ξ s | τ l C l A l | 2 γ s , m .
s , z , n ( x , y ) = c s ( 0 ) a s , n exp ( j α s , n y ) exp [ ( ω s ξ s | τ l C l A l | 2 γ ˜ s , n ) x ] exp [ j ( γ ˜ s , n ω s ξ s | τ l C l A l | 2 ) x ] .
γ ˜ s , n NL = γ ˜ s , n ω s ξ s | τ l C l A l | 2 .
rot E = j ω [ μ ] ,
rot = - j ω [ ε ] E j ω P ,
rot E n t = j ω t [ μ ] n t ,
rot n t = - j ω t [ ε ] E n t .
div ( E × n t - E n t × )= j ω E n t · P .
d d x u · ( E × n t - E n t × ) = j ω E n t · P ,
= + + d y d z
N n d c n d x = j ω E n t · P ,

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