Abstract

We observed that a monomolecular layer of an organic dye strongly influences the surface plasma oscillation (SPO) on thin silver films in spectral regions where the dye absorbs. Experimentally, squarylium dye was deposited by the Langmuir-Blodgett monolayer technique and the silver-dye films were investigated by their SPO’s. Within the absorption band, the SPO’s exhibited an anomalous dispersion and a pronounced variation in the damping. To explain this behavior, theoretical model calculations and approximate expressions are presented which show the relationship between the dielectric function of the coating and the observed effect. The influence of anisotropy is briefly outlined.

© 1978 Optical Society of America

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References

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  1. H. Raether, “Surface Plasma Oscillations and Their Applications,” Phys. Thin Films 9, 145 (1977).
  2. D. Hornauer, H. Kapitza, H. Raether, and J. Phys, D Appl. Phys. 7, L100 (1974).
    [CrossRef]
  3. A. J. Braundmeier and E. T. Arakawa, J. Phys. Chem. Solids 35, 517 (1974).
    [CrossRef]
  4. K. Holst and H. Raether, Opt. Commun. 2, 312 (1970).
    [CrossRef]
  5. J. J. Cowan and E. T. Arakawa, Z. Phys. 235, 97 (1970).
    [CrossRef]
  6. F. Abelès, Surf. Sci. 56, 237 (1976).
    [CrossRef]
  7. J. G. Gordon and J. D. Swalen, Opt. Commun. 22, 374 (1977).
    [CrossRef]
  8. I. Pockrand, “Surface Plasma Oscillations at Silver Surfaces with Thin Transparent and Absorbing Coatings,” Surf. Sci. 72, 577 (1978).
    [CrossRef]
  9. I. Pockrand, J. D. Swalen, J. A. Gordon, and M. R. Philpott, “Surface Plasmon Spectroscopy of Organic Monolayer Assemblies,” Surf. Sci. (to be published).
  10. P. B. Johnson and R. W. Christy, Phys. Rev. B 12, 4370 (1972).
    [CrossRef]
  11. T. Lopez-Rios, Opt. Commun. 17, 342 (1976).
    [CrossRef]
  12. H. Seki and U. Itoh, (unpublished results).
  13. I. Pockrand, J. D. Swalen, A. Brillante, J. A. Gordon, M. R. Philpott, and R. Santo, (unpublished).

1978 (1)

I. Pockrand, “Surface Plasma Oscillations at Silver Surfaces with Thin Transparent and Absorbing Coatings,” Surf. Sci. 72, 577 (1978).
[CrossRef]

1977 (2)

J. G. Gordon and J. D. Swalen, Opt. Commun. 22, 374 (1977).
[CrossRef]

H. Raether, “Surface Plasma Oscillations and Their Applications,” Phys. Thin Films 9, 145 (1977).

1976 (2)

F. Abelès, Surf. Sci. 56, 237 (1976).
[CrossRef]

T. Lopez-Rios, Opt. Commun. 17, 342 (1976).
[CrossRef]

1974 (2)

D. Hornauer, H. Kapitza, H. Raether, and J. Phys, D Appl. Phys. 7, L100 (1974).
[CrossRef]

A. J. Braundmeier and E. T. Arakawa, J. Phys. Chem. Solids 35, 517 (1974).
[CrossRef]

1972 (1)

P. B. Johnson and R. W. Christy, Phys. Rev. B 12, 4370 (1972).
[CrossRef]

1970 (2)

K. Holst and H. Raether, Opt. Commun. 2, 312 (1970).
[CrossRef]

J. J. Cowan and E. T. Arakawa, Z. Phys. 235, 97 (1970).
[CrossRef]

Abelès, F.

F. Abelès, Surf. Sci. 56, 237 (1976).
[CrossRef]

Arakawa, E. T.

A. J. Braundmeier and E. T. Arakawa, J. Phys. Chem. Solids 35, 517 (1974).
[CrossRef]

J. J. Cowan and E. T. Arakawa, Z. Phys. 235, 97 (1970).
[CrossRef]

Braundmeier, A. J.

A. J. Braundmeier and E. T. Arakawa, J. Phys. Chem. Solids 35, 517 (1974).
[CrossRef]

Brillante, A.

I. Pockrand, J. D. Swalen, A. Brillante, J. A. Gordon, M. R. Philpott, and R. Santo, (unpublished).

Christy, R. W.

P. B. Johnson and R. W. Christy, Phys. Rev. B 12, 4370 (1972).
[CrossRef]

Cowan, J. J.

J. J. Cowan and E. T. Arakawa, Z. Phys. 235, 97 (1970).
[CrossRef]

Gordon, J. A.

I. Pockrand, J. D. Swalen, J. A. Gordon, and M. R. Philpott, “Surface Plasmon Spectroscopy of Organic Monolayer Assemblies,” Surf. Sci. (to be published).

I. Pockrand, J. D. Swalen, A. Brillante, J. A. Gordon, M. R. Philpott, and R. Santo, (unpublished).

Gordon, J. G.

J. G. Gordon and J. D. Swalen, Opt. Commun. 22, 374 (1977).
[CrossRef]

Holst, K.

K. Holst and H. Raether, Opt. Commun. 2, 312 (1970).
[CrossRef]

Hornauer, D.

D. Hornauer, H. Kapitza, H. Raether, and J. Phys, D Appl. Phys. 7, L100 (1974).
[CrossRef]

Itoh, U.

H. Seki and U. Itoh, (unpublished results).

Johnson, P. B.

P. B. Johnson and R. W. Christy, Phys. Rev. B 12, 4370 (1972).
[CrossRef]

Kapitza, H.

D. Hornauer, H. Kapitza, H. Raether, and J. Phys, D Appl. Phys. 7, L100 (1974).
[CrossRef]

Lopez-Rios, T.

T. Lopez-Rios, Opt. Commun. 17, 342 (1976).
[CrossRef]

Philpott, M. R.

I. Pockrand, J. D. Swalen, A. Brillante, J. A. Gordon, M. R. Philpott, and R. Santo, (unpublished).

I. Pockrand, J. D. Swalen, J. A. Gordon, and M. R. Philpott, “Surface Plasmon Spectroscopy of Organic Monolayer Assemblies,” Surf. Sci. (to be published).

Phys, J.

D. Hornauer, H. Kapitza, H. Raether, and J. Phys, D Appl. Phys. 7, L100 (1974).
[CrossRef]

Pockrand, I.

I. Pockrand, “Surface Plasma Oscillations at Silver Surfaces with Thin Transparent and Absorbing Coatings,” Surf. Sci. 72, 577 (1978).
[CrossRef]

I. Pockrand, J. D. Swalen, J. A. Gordon, and M. R. Philpott, “Surface Plasmon Spectroscopy of Organic Monolayer Assemblies,” Surf. Sci. (to be published).

I. Pockrand, J. D. Swalen, A. Brillante, J. A. Gordon, M. R. Philpott, and R. Santo, (unpublished).

Raether, H.

H. Raether, “Surface Plasma Oscillations and Their Applications,” Phys. Thin Films 9, 145 (1977).

D. Hornauer, H. Kapitza, H. Raether, and J. Phys, D Appl. Phys. 7, L100 (1974).
[CrossRef]

K. Holst and H. Raether, Opt. Commun. 2, 312 (1970).
[CrossRef]

Santo, R.

I. Pockrand, J. D. Swalen, A. Brillante, J. A. Gordon, M. R. Philpott, and R. Santo, (unpublished).

Seki, H.

H. Seki and U. Itoh, (unpublished results).

Swalen, J. D.

J. G. Gordon and J. D. Swalen, Opt. Commun. 22, 374 (1977).
[CrossRef]

I. Pockrand, J. D. Swalen, J. A. Gordon, and M. R. Philpott, “Surface Plasmon Spectroscopy of Organic Monolayer Assemblies,” Surf. Sci. (to be published).

I. Pockrand, J. D. Swalen, A. Brillante, J. A. Gordon, M. R. Philpott, and R. Santo, (unpublished).

D Appl. Phys. (1)

D. Hornauer, H. Kapitza, H. Raether, and J. Phys, D Appl. Phys. 7, L100 (1974).
[CrossRef]

J. Phys. Chem. Solids (1)

A. J. Braundmeier and E. T. Arakawa, J. Phys. Chem. Solids 35, 517 (1974).
[CrossRef]

Opt. Commun. (3)

K. Holst and H. Raether, Opt. Commun. 2, 312 (1970).
[CrossRef]

J. G. Gordon and J. D. Swalen, Opt. Commun. 22, 374 (1977).
[CrossRef]

T. Lopez-Rios, Opt. Commun. 17, 342 (1976).
[CrossRef]

Phys. Rev. B (1)

P. B. Johnson and R. W. Christy, Phys. Rev. B 12, 4370 (1972).
[CrossRef]

Phys. Thin Films (1)

H. Raether, “Surface Plasma Oscillations and Their Applications,” Phys. Thin Films 9, 145 (1977).

Surf. Sci. (2)

F. Abelès, Surf. Sci. 56, 237 (1976).
[CrossRef]

I. Pockrand, “Surface Plasma Oscillations at Silver Surfaces with Thin Transparent and Absorbing Coatings,” Surf. Sci. 72, 577 (1978).
[CrossRef]

Z. Phys. (1)

J. J. Cowan and E. T. Arakawa, Z. Phys. 235, 97 (1970).
[CrossRef]

Other (3)

I. Pockrand, J. D. Swalen, J. A. Gordon, and M. R. Philpott, “Surface Plasmon Spectroscopy of Organic Monolayer Assemblies,” Surf. Sci. (to be published).

H. Seki and U. Itoh, (unpublished results).

I. Pockrand, J. D. Swalen, A. Brillante, J. A. Gordon, M. R. Philpott, and R. Santo, (unpublished).

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Figures (4)

FIG. 1
FIG. 1

Calculated SPO resonance angle versus wavelength for a layer system as sketched in the top left [dAg = 55 nm, dc = 2.5 nm, Ag from Ref. 10, and c given by Eq. (1) with ωsτ = 10, 20, and 50]. The solid line represents the bare silver film, the dotted line silver with a coating of constant dielectric function, c = 2.25( c = 0).

FIG. 2
FIG. 2

Calculated SPO resonance half-width versus wavelength (see Fig. 1 for notation).

FIG. 3
FIG. 3

Attenuated total reflectivity curves measured on a glass-silver-squarylium dye (one monolayer)-Cd-arachidate (one monolayer)-air arrangement for three wavelengths as indicated. The reference curves (bare silver) are given by the solid lines. The refractive index np of a 90° prism was 1.5161 at λ = 632.8 nm and 1.5258 at λ = 457.9 nm; the thickness dAg of the silver films was 61.5 nm; the thickness of the dye layer, dd, was 2.7 nm and the thickness of the cadmium-arachidate layer, da, 2.68 nm. Cd-arachidate is transparent in the visible wavelength range and exhibits only a small dispersion in the refractive index (na = 1.532 at λ = 632.8 nm and na = 1.552 at λ = 457.8 nm) (Ref. 9), the squarylium dye is characterized by a pronounced absorption band at λs = 538 nm (half-width approximately 40 nm).

FIG. 4
FIG. 4

Experimentally measured resonance shift Δϕ (circles), half-width broadening Δϕ1/2 (rhombs), and change of resonance depth ϕRmin (triangles, all with respect to the bare silver film) for the dye-coated silver film as described in Fig. 3. The molecular formula of the squarylium dye is shown as an insert in the lower right corner.

Equations (4)

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c = + ω p 2 f ω s 2 [ 1 - ( ω ω s ) 2 - i ( 1 ω s τ ω ω s ) ] - 1
Δ ϕ = f ( ϕ 0 , d c , λ , Ag ) [ c ( 1 + Ag c 2 + c 2 ) - Ag - 1 ]
f ( ϕ 0 , d c , λ , Ag ) = 2 π λ d c 1 n p cos ϕ 0 × ( 1 - Ag ) 1 / 2 ( Ag Ag + 1 ) 2 ( 1 1 - Ag ) ,
Δ ϕ 1 / 2 = f ( ϕ 0 , d c , λ , Ag ) [ c ( 1 - A g c 2 + c 2 ) ]