Abstract

The optical constants of discontinuous gold films consisting of both embedded and unembedded spherical particles in the size range 5–14 nm were determined from spectroellipsometric and spectrophotometric measurements. The optical response was modeled with the Yamaguchi anisotropic dielectric function. The energy and width dependence of the surface-plasmon resonance owing to the finite size of the gold particles was determined with a phenomenologically modified metal dielectric function. The expected blueshift and broadening of the resonance with decreasing particle size was observed. The magnitude of the shift suggests that lattice contraction, including its effect on both the free-electron response and the core response, plays an important role in determining the resonant energy. The width dependence on particle size was found to be well described by broadening parameters A=0.15 and A=0.22 for embedded and unembedded particles, respectively.

© 2001 Optical Society of America

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2000

D. Dalacu and L. Martinu, “Spectroellipsometric characterization of plasma deposited Au/SiO2 nanocomposite films,” J. Appl. Phys. 87, 228–235 (2000).
[CrossRef]

1998

B. Palpant, B. Prével, J. Lermé, E. Cottancin, M. Pellarin, M. Treilleux, A. Perez, J. Vialle, and M. Broyer, “Optical properties of gold clusters in the size range 2–4 nm,” Phys. Rev. B 57, 1963–1970 (1998).
[CrossRef]

M. Valden, X. Lai, and D. W. Goodman, “Onset of catalytic activity of gold clusters on titania with the appearance of nonmetallic properties,” Science 281, 1647–1650 (1998).
[CrossRef] [PubMed]

R. Doremus, “Optical absorption of island films of noble metals: wavelength of the plasma absorption band,” Thin Solid Films 326, 205–210 (1998).
[CrossRef]

K. Mümmler and P. Wimann, “Spectroscopic ellipsometry on gold clusters embedded in a Si(111) surface,” Thin Solid Films 313–314, 522–526 (1998).
[CrossRef]

A. Heilmann and J. Werner, “In situ observation of microstructural changes of embedded silver particles,” Thin Solid Films 317, 21–26 (1998).
[CrossRef]

J. Lermé, B. Palpant, B. Prével, E. Cottancin, M. Pellarin, M. Treilleux, J. Vialle, A. Perez, and M. Broyer, “Optical properties of gold metal clusters: a time-dependent local-density-approximation investigation,” Eur. Phys. J. D 4, 95–108 (1998).
[CrossRef]

1997

L. Serra and A. Rubio, “Optical response of Ag clusters,” Z. Phys. D 40, 262–264 (1997).
[CrossRef]

1996

M. Quinten, “Optical constants of gold and silver clusters in the spectral range between 1.5 eV and 4.5 eV,” Z. Phys. B 100, 211–217 (1996).
[CrossRef]

1995

T. Reiners, C. Ellert, M. Schmidt, and H. Haberland, “Size dependence of the optical response of spherical sodium clusters,” Phys. Rev. Lett. 74, 1558–1561 (1995).
[CrossRef] [PubMed]

R. Lamber, S. Wetjen, and G. Schulz-Ekloff, “Metal clusters in plasma polymer matrices: gold clusters,” J. Phys. C 99, 13834–13838 (1995).

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]

1994

L. Martinu, J. E. Klemberg-Sapieha, O. M. Kuttel, A. Raveh, and M. R. Wertheimer, “Critical ion energy and ion flux in the growth of films by plasma-enhanced chemical-vapor deposition,” J. Vac. Sci. Technol. A 12, 1360–1364 (1994).
[CrossRef]

1993

A. Rubio and L. Serra, “Dielectric screening effects on the photoabsorption cross section of embedded metallic clusters,” Phys. Rev. B 48, 18222–18229 (1993).
[CrossRef]

B. N. J. Persson, “Polarizability of small spherical metal particles: influence of the matrix environment,” Surf. Sci. 281, 153–162 (1993).
[CrossRef]

H. Hovel, S. Fritz, A. Hilger, U. Kreibig, and M. Vollmer, “Width of cluster plasmon resonances: bulk dielectric function and chemical interface damping,” Phys. Rev. B 48, 18178–18188 (1993).
[CrossRef]

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

J. Tiggesbäumker, L. Köller, K.-H. Meiwes-Broer, and A. Liebsch, “Blue shift of the Mie plasma frequency in Ag clusters and particles,” Phys. Rev. A 48, R1749–R1752 (1993).
[CrossRef] [PubMed]

W. A. de Heer, “The physics of simple metal clusters: experimental and simple models,” Rev. Mod. Phys. 65, 611–676 (1993).
[CrossRef]

1992

C. Yannouleas and R. A. Broglia, “Landau damping and wall dissipation in large metal clusters,” Ann. Phys. (N.Y.) 217, 105–141 (1992).
[CrossRef]

J. Tiggesbäumker, L. Köller, H. O. Lutz, and K.-H. Meiwes-Broer, “Giant resonances in silver-cluster photofragmentation,” Chem. Phys. Lett. 190, 42–47 (1992).
[CrossRef]

M. Miki-Yoshida, S. Techuacanero, and M. José-Yacamán, “On the high temperature coalescence of metallic nanocrystals,” Surf. Sci. Lett. 274, L569–L576 (1992).
[CrossRef]

1990

G. K. Wertheim, “The insulator–metal transition in supported clusters,” Phase Transit. 24–26, 203–214 (1990).
[CrossRef]

J. E. Klemberg-Sapieha, O. M. Kuttel, L. Martinu, and M. R. Wertheimer, “Dual microwave–RF plasma deposition of functional coatings,” Thin Solid Films 93–94, 965–972 (1990).
[CrossRef]

G. Bader, P. Ashrit, F. Girouard, and V. Truong, “p-polarized optical properties of aggregrated Au films,” J. Appl. Phys. 68, 1820–1824 (1990).
[CrossRef]

1989

K. P. Charlé, W. Schulze, and B. Winter, “The size dependent shift of the surface plasmon absorption band of small spherical metal particles,” Z. Phys. D 12, 471–475 (1989).
[CrossRef]

1988

1987

G. A. Niklasson, “Optical properties of gas-evaporated metal particles: effects of a fractal structure,” J. Appl. Phys. 62, 258–265 (1987).
[CrossRef]

E. Zaremba and B. N. J. Persson, “Dynamic polarizability of small metal particles,” Phys. Rev. B 35, 596–606 (1987).
[CrossRef]

1986

R. J. Warmack and S. L. Humphrey, “Observation of two surface-plasmon modes on gold particles,” Phys. Rev. B 34, 2246–2252 (1986).
[CrossRef]

Y. Borensztein, P. D. Andrès, R. Monreal, T. Lopez-Rios, and F. Flores, “Blue-shift of the dipolar plasma resonance in small silver particles on an alumina surface,” Phys. Rev. B 33, 2828–2830 (1986).
[CrossRef]

1985

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

D. Ricard, P. Roussignol, and C. Flytzanis, “Surface-mediated enhancement of optical phase conjugation in metal colloids,” Opt. Lett. 10, 511–513 (1985).
[CrossRef] [PubMed]

C. Solliard and M. Flueli, “Surface stress and size effects on the lattice parameter in small particles of gold and platinum,” Surf. Sci. 156, 487–494 (1985).
[CrossRef]

A. Balerna, E. Bernieri, P. Picozzi, A. Reale, and S. Santucci, “A structural investigation on small gold clusters by EXAFS,” Surf. Sci. 156, 206–213 (1985).
[CrossRef]

1984

T. Yamaguchi, M. Takiguchi, S. Fujioka, and H. Takahashi, “Optical absorption of submonolayer gold films: size dependence of εbound in small island particles,” Surf. Sci. 138, 449–463 (1984).
[CrossRef]

J. Little, T. Callcott, T. Ferrel, and E. Arakawa, “Surface-plasmon radiation from ellipsoidal silver spheroids,” Phys. Rev. B 29, 1606–1615 (1984).
[CrossRef]

1983

T. Yamaguchi, M. Ogawa, H. Takahashi, and N. Saito, “Optical absorption of submonolayer silver films: size dependence of εbound in small island particles,” Surf. Sci. 129, 232–246 (1983).
[CrossRef]

D. Bedeaux and J. Vlieger, “A statistical theory for the dielectric properties of thin island films: application and comparison with experimental results,” Thin Solid Films 102, 265–281 (1983).
[CrossRef]

P. Apell and D. R. Penn, “Optical properties of small metal spheres: surface effects,” Phys. Rev. Lett. 50, 1316–1319 (1983).
[CrossRef]

1982

P. Apell and A. Ljungbert, “A general nonlocal theory for the electromagnetic response of a small metal particle,” Phys. Scr. 26, 113–118 (1982).
[CrossRef]

P. J. Feibelman, “Surface electromagnetic fields,” Prog. Surf. Sci. 12, 287–408 (1982).
[CrossRef]

1981

J. L. Martins, R. Car, and J. Buffet, “Variational spherical model of small metallic particles,” Surf. Sci. 106, 265–271 (1981).
[CrossRef]

R. Lässer and N. V. Smith, “Interband optical transitions in gold in the photon energy range 2–25 eV,” Solid State Commun. 37, 507–509 (1981).
[CrossRef]

1980

H. Roulet, G. D. J. M. Mariot, and C. F. Hague, “Size dependence of the valence bands in gold clusters,” J. Phys. F 10, 1025–1030 (1980).
[CrossRef]

1979

C. G. Granqvist, N. Calander, and O. Hunderi, “Optical properties of ultrafine silver particles,” Solid State Commun. 31, 249–252 (1979).
[CrossRef]

1978

J. C. C. Fan, “Selective-black absorbers using sputtered cermet films,” Thin Solid Films 54, 139–148 (1978).
[CrossRef]

S. Norman, T. Andersson, and C. Granqvist, “Optical properties of discontinuous gold films,” Phys. Rev. B 18, 674–695 (1978).
[CrossRef]

T. Yamaguchi, H. Hidetoshi, and A. Sudoh, “Optical behavior of a metal island film,” J. Opt. Soc. Am. 68, 1039–1044 (1978).
[CrossRef]

1977

C. Granqvist and O. Hunderi, “Optical properties of ultrafine gold particles,” Phys. Rev. B 16, 3513–3534 (1977).
[CrossRef]

U. Kreibig, “Anomalous frequency and temperature dependence of the optical absorption of small gold particles,” J. Phys. (Paris) Colloq. 27, 97–103 (1977).

1976

D. Jarret and L. Ward, “Optical properties of discontinuous gold films,” J. Phys. D 9, 1515–1527 (1976).
[CrossRef]

V. Truong and G. Scott, “Optical constants of aggregated gold films,” J. Opt. Soc. Am. 66, 124–131 (1976).
[CrossRef]

K. Liang, W. Salaneck, and I. Aksay, “X-ray photoemission studies of thin gold films,” Solid State Commun. 19, 329–334 (1976).
[CrossRef]

1975

P. Winsemius, H. P. Lengkeek, and F. F. V. Kampen, “Structure dependence of the optical properties of Cu, Ag and Au,” Physica B 79, 529–546 (1975).
[CrossRef]

1974

T. Yamaguchi, S. Yoshida, and A. Kinbara, “Optical effect of the substrate on the anomalous absorption of aggregated silver films,” Thin Solid Films 21, 173–187 (1974).
[CrossRef]

1973

T. Yamaguchi, S. Yoshida, and A. Kinbara, “Anomalous optical absorption of aggregated silver films,” Thin Solid Films 18, 63–70 (1973).
[CrossRef]

1971

N. E. Christensen and B. O. Seraphin, “Relativistic band calculation and the optical properties of gold,” Phys. Rev. B 4, 3321–3344 (1971).
[CrossRef]

1970

U. Kreibig and P. Zacharias, “Surface plasma resonances in small spherical silver and gold particles,” Z. Phys. 231, 128–143 (1970).
[CrossRef]

1969

U. Kreibig and C. von Fragstein, “The limitation of electron mean free path in small silver particles,” Z. Phys. 224, 307–323 (1969).
[CrossRef]

1968

C. W. Mays, J. S. Vermaak, and D. Kuhlmann-Wilsdorf, “On surface stress and surface tension,” Surf. Sci. 12, 134–140 (1968).
[CrossRef]

1966

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

1908

G. Mie, “Beiträge zur Optik trüber Medien, speziell kolloidaler Metallösungen,” Ann. Phys. (Leipzig) 25, 377–445 (1908).
[CrossRef]

1904

J. C. Maxwell-Garnett, “Colours in metal glasses and in metallic films,” Philos. Trans. R. Soc. London 203, 385–420 (1904).
[CrossRef]

1857

M. Faraday, “Experimental relations of gold (and other metals) to light,” Philos. Trans. R. Soc. London 147, 145–181 (1857).
[CrossRef]

Aksay, I.

K. Liang, W. Salaneck, and I. Aksay, “X-ray photoemission studies of thin gold films,” Solid State Commun. 19, 329–334 (1976).
[CrossRef]

Andersson, T.

S. Norman, T. Andersson, and C. Granqvist, “Optical properties of discontinuous gold films,” Phys. Rev. B 18, 674–695 (1978).
[CrossRef]

Andrès, P. D.

Y. Borensztein, P. D. Andrès, R. Monreal, T. Lopez-Rios, and F. Flores, “Blue-shift of the dipolar plasma resonance in small silver particles on an alumina surface,” Phys. Rev. B 33, 2828–2830 (1986).
[CrossRef]

Apell, P.

P. Apell and D. R. Penn, “Optical properties of small metal spheres: surface effects,” Phys. Rev. Lett. 50, 1316–1319 (1983).
[CrossRef]

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D. Dalacu and L. Martinu, “Spectroellipsometric characterization of plasma deposited Au/SiO2 nanocomposite films,” J. Appl. Phys. 87, 228–235 (2000).
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[CrossRef]

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R. Lamber, S. Wetjen, and G. Schulz-Ekloff, “Metal clusters in plasma polymer matrices: gold clusters,” J. Phys. C 99, 13834–13838 (1995).

Scott, G.

Seraphin, B. O.

N. E. Christensen and B. O. Seraphin, “Relativistic band calculation and the optical properties of gold,” Phys. Rev. B 4, 3321–3344 (1971).
[CrossRef]

Serra, L.

L. Serra and A. Rubio, “Optical response of Ag clusters,” Z. Phys. D 40, 262–264 (1997).
[CrossRef]

A. Rubio and L. Serra, “Dielectric screening effects on the photoabsorption cross section of embedded metallic clusters,” Phys. Rev. B 48, 18222–18229 (1993).
[CrossRef]

Smith, N. V.

R. Lässer and N. V. Smith, “Interband optical transitions in gold in the photon energy range 2–25 eV,” Solid State Commun. 37, 507–509 (1981).
[CrossRef]

Solliard, C.

C. Solliard and M. Flueli, “Surface stress and size effects on the lattice parameter in small particles of gold and platinum,” Surf. Sci. 156, 487–494 (1985).
[CrossRef]

Sudoh, A.

Takahashi, H.

T. Yamaguchi, M. Takiguchi, S. Fujioka, and H. Takahashi, “Optical absorption of submonolayer gold films: size dependence of εbound in small island particles,” Surf. Sci. 138, 449–463 (1984).
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T. Yamaguchi, M. Takiguchi, S. Fujioka, and H. Takahashi, “Optical absorption of submonolayer gold films: size dependence of εbound in small island particles,” Surf. Sci. 138, 449–463 (1984).
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H. Hovel, S. Fritz, A. Hilger, U. Kreibig, and M. Vollmer, “Width of cluster plasmon resonances: bulk dielectric function and chemical interface damping,” Phys. Rev. B 48, 18178–18188 (1993).
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R. Lamber, S. Wetjen, and G. Schulz-Ekloff, “Metal clusters in plasma polymer matrices: gold clusters,” J. Phys. C 99, 13834–13838 (1995).

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K. Mümmler and P. Wimann, “Spectroscopic ellipsometry on gold clusters embedded in a Si(111) surface,” Thin Solid Films 313–314, 522–526 (1998).
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T. Yamaguchi, M. Takiguchi, S. Fujioka, and H. Takahashi, “Optical absorption of submonolayer gold films: size dependence of εbound in small island particles,” Surf. Sci. 138, 449–463 (1984).
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Eur. Phys. J. D

J. Lermé, B. Palpant, B. Prével, E. Cottancin, M. Pellarin, M. Treilleux, J. Vialle, A. Perez, and M. Broyer, “Optical properties of gold metal clusters: a time-dependent local-density-approximation investigation,” Eur. Phys. J. D 4, 95–108 (1998).
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Phys. Rev. B

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[CrossRef]

C. Solliard and M. Flueli, “Surface stress and size effects on the lattice parameter in small particles of gold and platinum,” Surf. Sci. 156, 487–494 (1985).
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A. Balerna, E. Bernieri, P. Picozzi, A. Reale, and S. Santucci, “A structural investigation on small gold clusters by EXAFS,” Surf. Sci. 156, 206–213 (1985).
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[CrossRef]

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[CrossRef]

Surf. Sci. Lett.

M. Miki-Yoshida, S. Techuacanero, and M. José-Yacamán, “On the high temperature coalescence of metallic nanocrystals,” Surf. Sci. Lett. 274, L569–L576 (1992).
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Thin Solid Films

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[CrossRef]

T. Yamaguchi, S. Yoshida, and A. Kinbara, “Optical effect of the substrate on the anomalous absorption of aggregated silver films,” Thin Solid Films 21, 173–187 (1974).
[CrossRef]

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[CrossRef]

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[CrossRef]

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U. Kreibig and P. Zacharias, “Surface plasma resonances in small spherical silver and gold particles,” Z. Phys. 231, 128–143 (1970).
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Figures (8)

Fig. 1
Fig. 1

Schematic representation of the multilayer dielectric/gold/dielectric structure.

Fig. 2
Fig. 2

Optical constants of (a) glass, SiO2, TiO2, and (b) gold.

Fig. 3
Fig. 3

TEM micrographs and particle-size distributions for the SiO2/gold/SiO2 samples.

Fig. 4
Fig. 4

Transmission spectra of discontinuous gold films on a SiO2 base layer with (a) no cladding, (b) SiO2 cladding, and (c) TiO2 cladding.

Fig. 5
Fig. 5

Transmission spectrum of sample C cladded with TiO2 on TiO2 base layers of different thicknesses.

Fig. 6
Fig. 6

Ellipsometric data (top) Ψ and (bottom) Δ, and model fit for sample C with a base and cladding layer of SiO2.

Fig. 7
Fig. 7

Dependence of (a) δ and (b) Γ on reciprocal particle size for the SiO2/gold/SiO2 and SiO2/gold/vacuum samples corresponding to the TEM images in Fig. 3. The filled circles represent the calculations for the cladded sample with two depolarization factors to describe .

Fig. 8
Fig. 8

Normalized finite-size effect shifts of the SPR of Au/SiO2 films. Data for Au/Al2O3 cermets33 are also included as well as the theoretical shifts predicted from TDLDA calculations with a 0.1-nm region of nonoverlap between d-electron and conduction-electron wave functions.61

Tables (1)

Tables Icon

Table 1 Results of the Image Analysis Performed on the TEM Micrographsa

Equations (6)

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

=h1+p(m-h)h+F(m-h),
1=1h 1-p(m-h)h+F(m-h),
F=f-γ224η3 s-hs+h-C pdζ 2hs+h,
F=f-γ212η3 s-hs+h+C pdζ 2ss+h,
m=core+1-ωp2ω(ω+i/τB),
Γ=τB-1+AνFR,

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