Abstract

We have studied strong exciton-plasmon coupling in the films of Ag nanoislands as well as in the layer-by-layer (LBL) deposited films of Au nanoparticles (NPs) coated with highly concentrated rhodamine 6G (R6G) dye. Their absorbance and the reflectance spectra featured the peaks or dips, which were not characteristic of dye or NPs/nanoislands taken separately. The positions of the spectral maxima (or minima) in the dye-doped films, plotted against those in pristine Ag nanoislands films, resulted in the dispersion curves comprised of three branches. They could be described by the analytical model based on the Hamiltonian accounting for the unperturbed energies of the surface plasmon (SP) resonance, the two bands composing the absorption spectrum of R6G dye, and the exciton-plasmon coupling energy Δ. Its value was larger in Ag nanoislands films deposited on hyperbolic metamaterials (0.221 eV) than on glass (0.165 eV). The minimal gap between the upper and the lower branches was equal to ≈3Δ. The dispersion curves in the Au NPs LBL films could be described with the Hamiltonian equation at relatively small dye concentrations. At larger concentrations of R6G molecules, the spectral peaks shifted and became more pronounced. The corresponding dispersion curve could not be described in terms of the existing model, indicating the need for further theoretical studies.

© 2016 Optical Society of America

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2016 (1)

2015 (6)

J. K. Kitur, L. Gu, T. Tumkur, C. Bonner, and M. A. Noginov, “Stimulated emission of surface plasmons on top of metamaterials with hyperbolic dispersion,” ACS Photonics 2(8), 1019–1024 (2015).
[Crossref]

T. Tumkur, Y. Barnakov, S. T. Kee, M. A. Noginov, and V. Liberman, “Permittivity evaluation of multilayered hyperbolic metamaterials: Ellipsometry vs. reflectometry,” J. Appl. Phys. 117(10), 103104 (2015).
[Crossref]

T. U. Tumkur, J. K. Kitur, C. E. Bonner, A. N. Poddubny, E. E. Narimanov, and M. A. Noginov, “Control of Förster energy transfer in the vicinity of metallic surfaces and hyperbolic metamaterials,” Faraday Discuss. 178, 395–412 (2015).
[Crossref] [PubMed]

P. Törmä and W. L. Barnes, “Strong coupling between surface plasmon polaritons and emitters: a review,” Rep. Prog. Phys. 78(1), 013901 (2015).
[Crossref] [PubMed]

A. Salleo, “Organic electronics: Something out of nothing,” Nat. Mater. 14(11), 1077–1078 (2015).
[Crossref] [PubMed]

C. Gonzalez-Ballestero, J. Feist, E. Moreno, and F. J. Garcia-Vidal, “Harvesting excitons through plasmonic strong coupling,” Phys. Rev. B 92(12), 121402 (2015).
[Crossref]

2014 (2)

W. Park, “Optical interactions in plasmonic nanostructures,” Nano Converg. 1(1), 2 (2014).
[Crossref]

L. Gu, T. U. Tumkur, G. Zhu, and M. A. Noginov, “Blue shift of spontaneous emission in hyperbolic metamaterial,” Sci. Rep. 4, 4969 (2014).
[Crossref] [PubMed]

2013 (5)

Y. Kim, J. Zhu, B. Yeom, M. Di Prima, X. Su, J.-G. Kim, S. J. Yoo, C. Uher, and N. A. Kotov, “Stretchable nanoparticle conductors with self-organized conductive pathways,” Nature 500(7460), 59–63 (2013).
[Crossref] [PubMed]

E. E. Narimanov, H. Li, Y. A. Barnakov, T. U. Tumkur, and M. A. Noginov, “Reduced reflection from roughened hyperbolic metamaterial,” Opt. Express 21(12), 14956–14961 (2013).
[Crossref] [PubMed]

M. A. Kats, R. Blanchard, S. Zhang, P. Genevet, C. Ko, S. Ramanathan, and F. Capasso, “Vanadium dioxide as a natural disordered metamaterial: perfect thermal emission and large broadband negative differential thermal emittance,” Phys. Rev. X 3(4), 041004 (2013).
[Crossref]

J. A. Hutchison, A. Liscio, T. Schwartz, A. Canaguier-Durand, C. Genet, V. Palermo, P. Samorì, and T. W. Ebbesen, “Tuning the work-function via strong coupling,” Adv. Mater. 25(17), 2481–2485 (2013).
[Crossref] [PubMed]

A. Canaguier-Durand, E. Devaux, J. George, Y. Pang, J. A. Hutchison, T. Schwartz, C. Genet, N. Wilhelms, J.-M. Lehn, and T. W. Ebbesen, “Thermodynamics of molecules strongly coupled to the vacuum field,” Angew. Chem. Int. Ed. Engl. 52(40), 10533–10536 (2013).
[Crossref] [PubMed]

2012 (4)

A. Fontcuberta i Morral and F. Stellacci, “Light-matter interactions: Ultrastrong routes to new chemistry,” Nat. Mater. 11(4), 272–273 (2012).
[Crossref] [PubMed]

V. J. Sorger, R. F. Oulton, R.-M. Ma, and X. Zhang, “Toward integrated plasmonic circuits,” MRS Bull. 37(08), 728–738 (2012).
[Crossref]

Z. Jacob, I. I. Smolyaninov, and E. E. Narimanov, “Broadband Purcell effect: Radiative decay engineering with metamaterials,” Appl. Phys. Lett. 100(18), 181105 (2012).
[Crossref]

T. U. Tumkur, J. K. Kitur, B. Chu, L. Gu, V. A. Podolskiy, E. E. Narimanov, and M. A. Noginov, “Control of reflectance and transmittance in scattering and curvilinear hyperbolic metamaterials,” Appl. Phys. Lett. 101(9), 091105 (2012).
[Crossref]

2011 (5)

T. Tumkur, G. Zhu, P. Black, Y. A. Barnakov, C. E. Bonner, and M. A. Noginov, “Control of spontaneous emission in a volume of functionalized hyperbolic metamaterial,” Appl. Phys. Lett. 99(15), 151115 (2011).
[Crossref]

N. T. Fofang, N. K. Grady, Z. Fan, A. O. Govorov, and N. J. Halas, “Plexciton dynamics: Exciton-plasmon coupling in a J-aggregate-Au nanoshell complex provides a mechanism for nonlinearity,” Nano Lett. 11(4), 1556–1560 (2011).
[Crossref] [PubMed]

A. N. Poddubny, P. A. Belov, and Y. S. Kivshar, “Spontaneous radiation of a finite-size dipole emitter in hyperbolic media,” Phys. Rev. A 84(2), 023807 (2011).
[Crossref]

A. Manjavacas, F. J. García de Abajo, and P. Nordlander, “Quantum plexcitonics: strongly interacting plasmons and excitons,” Nano Lett. 11(6), 2318–2323 (2011).
[Crossref] [PubMed]

T. Schwartz, J. A. Hutchison, C. Genet, and T. W. Ebbesen, “Reversible switching of ultrastrong light-molecule coupling,” Phys. Rev. Lett. 106(19), 196405 (2011).
[Crossref] [PubMed]

2010 (5)

J. B. Khurgin and G. Sun, “In search of the elusive lossless metal,” Appl. Phys. Lett. 96(18), 181102 (2010).
[Crossref]

B. Luk’yanchuk, N. I. Zheludev, S. A. Maier, N. J. Halas, P. Nordlander, H. Giessen, and C. T. Chong, “The Fano resonance in plasmonic nanostructures and metamaterials,” Nat. Mater. 9(9), 707–715 (2010).
[Crossref] [PubMed]

H. A. Atwater and A. Polman, “Plasmonics for improved photovoltaic devices,” Nat. Mater. 9(3), 205–213 (2010).
[Crossref] [PubMed]

D. E. Gómez, K. C. Vernon, P. Mulvaney, and T. J. Davis, “Surface plasmon mediated strong exciton-photon coupling in semiconductor nanocrystals,” Nano Lett. 10(1), 274–278 (2010).
[Crossref] [PubMed]

P. Vasa, R. Pomraenke, G. Cirmi, E. De Re, W. Wang, S. Schwieger, D. Leipold, E. Runge, G. Cerullo, and C. Lienau, “Ultrafast manipulation of strong coupling in metal-molecular aggregate hybrid nanostructures,” ACS Nano 4(12), 7559–7565 (2010).
[Crossref] [PubMed]

2009 (4)

N. I. Cade, T. Ritman-Meer, and D. Richards, “Strong coupling of localized plasmons and molecular excitons in nanostructured silver films,” Phys. Rev. B – Condens. Matter Mater. Phys. 79(24), 241404 (2009).
[Crossref]

T. K. Hakala, J. J. Toppari, A. Kuzyk, M. Pettersson, H. Tikkanen, H. Kunttu, and P. Törmä, “Vacuum Rabi splitting and strong-coupling dynamics for surface-plasmon polaritons and rhodamine 6G molecules,” Phys. Rev. Lett. 103(5), 053602 (2009).
[Crossref] [PubMed]

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2008 (3)

J. Dintinger, S. Klein, F. Bustos, W. L. Barnes, and T. W. Ebbesen, “Strong coupling between surface plasmon-polaritons and organic molecules in subwavelength hole arrays,” Phys. Rev. B 71, 1–5 (2008).

N. T. Fofang, T.-H. Park, O. Neumann, N. A. Mirin, P. Nordlander, and N. J. Halas, “Plexcitonic nanoparticles: plasmon-exciton coupling in nanoshell-J-aggregate complexes,” Nano Lett. 8(10), 3481–3487 (2008).
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2007 (7)

N. E. Engheta, A. Alù, M. Silveirinha, and A. Salandrino, “Epsilon-Near-Zero (ENZ) metamaterials and electromagnetic sources: tailoring the radiation phase pattern,” Phys. Rev. B 75, 1–37 (2007).

G. A. Wurtz, P. R. Evans, W. Hendren, R. Atkinson, W. Dickson, R. J. Pollard, A. V. Zayats, W. Harrison, and C. Bower, “Molecular plasmonics with tunable exciton-plasmon coupling strength in J-aggregate hybridized Au nanorod assemblies,” Nano Lett. 7(5), 1297–1303 (2007).
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A. O. Govorov and I. Carmeli, “Hybrid structures composed of photosynthetic system and metal nanoparticles: plasmon enhancement effect,” Nano Lett. 7(3), 620–625 (2007).
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2006 (7)

J. Lee, T. Javed, T. Skeini, A. O. Govorov, G. W. Bryant, and N. A. Kotov, “Bioconjugated Ag nanoparticles and CdTe nanowires: metamaterials with field-enhanced light absorption,” Angew. Chem. Int. Ed. Engl. 45(29), 4819–4823 (2006).
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S. W. Bishnoi, C. J. Rozell, C. S. Levin, M. K. Gheith, B. R. Johnson, D. H. Johnson, and N. J. Halas, “All-optical nanoscale pH meter,” Nano Lett. 6(8), 1687–1692 (2006).
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W. Zhang, A. O. Govorov, and G. W. Bryant, “Semiconductor-metal nanoparticle molecules: hybrid excitons and the nonlinear fano effect,” Phys. Rev. Lett. 97(14), 146804 (2006).
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2005 (1)

J. Lee, A. O. Govorov, and N. A. Kotov, “Nanoparticle assemblies with molecular springs: a nanoscale thermometer,” Angew. Chem. Int. Ed. Engl. 44(45), 7439–7442 (2005).
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2004 (2)

M. Nezhad, K. Tetz, and Y. Fainman, “Gain assisted propagation of surface plasmon polaritons on planar metallic waveguides,” Opt. Express 12(17), 4072–4079 (2004).
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2003 (3)

D. R. Smith and D. Schurig, “Electromagnetic wave propagation in media with indefinite permittivity and permeability tensors,” Phys. Rev. Lett. 90(7), 077405 (2003).
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2002 (1)

N. Malikova, I. Pastoriza-Santos, M. Schierhorn, N. A. Kotov, and L. M. Liz-Marzán, “Layer-by-layer assembled mixed spherical and planar gold nanoparticles: Control of interparticle interactions,” Langmuir 18(9), 3694–3697 (2002).
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1989 (1)

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1983 (1)

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V. M. Agranovich and A. G. Malshukov, “Surface polariton spectra if the resonance with the transition layer vibrations exist,” Opt. Commun. 11(2), 169–171 (1974).
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N. E. Engheta, A. Alù, M. Silveirinha, and A. Salandrino, “Epsilon-Near-Zero (ENZ) metamaterials and electromagnetic sources: tailoring the radiation phase pattern,” Phys. Rev. B 75, 1–37 (2007).

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K. Hennessy, A. Badolato, M. Winger, D. Gerace, M. Atatüre, S. Gulde, S. Fält, E. L. Hu, and A. Imamoğlu, “Quantum nature of a strongly coupled single quantum dot-cavity system,” Nature 445(7130), 896–899 (2007).
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G. A. Wurtz, P. R. Evans, W. Hendren, R. Atkinson, W. Dickson, R. J. Pollard, A. V. Zayats, W. Harrison, and C. Bower, “Molecular plasmonics with tunable exciton-plasmon coupling strength in J-aggregate hybridized Au nanorod assemblies,” Nano Lett. 7(5), 1297–1303 (2007).
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T. Tumkur, Y. Barnakov, S. T. Kee, M. A. Noginov, and V. Liberman, “Permittivity evaluation of multilayered hyperbolic metamaterials: Ellipsometry vs. reflectometry,” J. Appl. Phys. 117(10), 103104 (2015).
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R. F. Oulton, V. J. Sorger, T. Zentgraf, R.-M. Ma, C. Gladden, L. Dai, G. Bartal, and X. Zhang, “Plasmon lasers at deep subwavelength scale,” Nature 461(7264), 629–632 (2009).
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Y. Sugawara, T. A. Kelf, J. J. Baumberg, M. E. Abdelsalam, and P. N. Bartlett, “Strong coupling between localized plasmons and organic excitons in metal nanovoids,” Phys. Rev. Lett. 97(26), 266808 (2006).
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Y. Sugawara, T. A. Kelf, J. J. Baumberg, M. E. Abdelsalam, and P. N. Bartlett, “Strong coupling between localized plasmons and organic excitons in metal nanovoids,” Phys. Rev. Lett. 97(26), 266808 (2006).
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M. A. Noginov, G. Zhu, A. M. Belgrave, R. Bakker, V. M. Shalaev, E. E. Narimanov, S. Stout, E. Herz, T. Suteewong, and U. Wiesner, “Demonstration of a spaser-based nanolaser,” Nature 460(7259), 1110–1112 (2009).
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J. Bellessa, C. Bonnand, J. C. Plenet, and J. Mugnier, “Strong coupling between surface plasmons and excitons in an organic semiconductor,” Phys. Rev. Lett. 93(3), 036404 (2004).
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S. W. Bishnoi, C. J. Rozell, C. S. Levin, M. K. Gheith, B. R. Johnson, D. H. Johnson, and N. J. Halas, “All-optical nanoscale pH meter,” Nano Lett. 6(8), 1687–1692 (2006).
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T. Tumkur, G. Zhu, P. Black, Y. A. Barnakov, C. E. Bonner, and M. A. Noginov, “Control of spontaneous emission in a volume of functionalized hyperbolic metamaterial,” Appl. Phys. Lett. 99(15), 151115 (2011).
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M. A. Kats, R. Blanchard, S. Zhang, P. Genevet, C. Ko, S. Ramanathan, and F. Capasso, “Vanadium dioxide as a natural disordered metamaterial: perfect thermal emission and large broadband negative differential thermal emittance,” Phys. Rev. X 3(4), 041004 (2013).
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J. Bellessa, C. Bonnand, J. C. Plenet, and J. Mugnier, “Strong coupling between surface plasmons and excitons in an organic semiconductor,” Phys. Rev. Lett. 93(3), 036404 (2004).
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J. K. Kitur, L. Gu, T. Tumkur, C. Bonner, and M. A. Noginov, “Stimulated emission of surface plasmons on top of metamaterials with hyperbolic dispersion,” ACS Photonics 2(8), 1019–1024 (2015).
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T. U. Tumkur, J. K. Kitur, C. E. Bonner, A. N. Poddubny, E. E. Narimanov, and M. A. Noginov, “Control of Förster energy transfer in the vicinity of metallic surfaces and hyperbolic metamaterials,” Faraday Discuss. 178, 395–412 (2015).
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T. Tumkur, G. Zhu, P. Black, Y. A. Barnakov, C. E. Bonner, and M. A. Noginov, “Control of spontaneous emission in a volume of functionalized hyperbolic metamaterial,” Appl. Phys. Lett. 99(15), 151115 (2011).
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G. A. Wurtz, P. R. Evans, W. Hendren, R. Atkinson, W. Dickson, R. J. Pollard, A. V. Zayats, W. Harrison, and C. Bower, “Molecular plasmonics with tunable exciton-plasmon coupling strength in J-aggregate hybridized Au nanorod assemblies,” Nano Lett. 7(5), 1297–1303 (2007).
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G. Rempe, R. J. Thompson, R. J. Brecha, W. D. Lee, and H. J. Kimble, “Optical bistability and photon statistics in cavity quantum electrodynamics,” Phys. Rev. Lett. 67(13), 1727–1730 (1991).
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W. Zhang, A. O. Govorov, and G. W. Bryant, “Semiconductor-metal nanoparticle molecules: hybrid excitons and the nonlinear fano effect,” Phys. Rev. Lett. 97(14), 146804 (2006).
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J. Lee, T. Javed, T. Skeini, A. O. Govorov, G. W. Bryant, and N. A. Kotov, “Bioconjugated Ag nanoparticles and CdTe nanowires: metamaterials with field-enhanced light absorption,” Angew. Chem. Int. Ed. Engl. 45(29), 4819–4823 (2006).
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J. Dintinger, S. Klein, F. Bustos, W. L. Barnes, and T. W. Ebbesen, “Strong coupling between surface plasmon-polaritons and organic molecules in subwavelength hole arrays,” Phys. Rev. B 71, 1–5 (2008).

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N. I. Cade, T. Ritman-Meer, and D. Richards, “Strong coupling of localized plasmons and molecular excitons in nanostructured silver films,” Phys. Rev. B – Condens. Matter Mater. Phys. 79(24), 241404 (2009).
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J. A. Hutchison, A. Liscio, T. Schwartz, A. Canaguier-Durand, C. Genet, V. Palermo, P. Samorì, and T. W. Ebbesen, “Tuning the work-function via strong coupling,” Adv. Mater. 25(17), 2481–2485 (2013).
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A. O. Govorov and I. Carmeli, “Hybrid structures composed of photosynthetic system and metal nanoparticles: plasmon enhancement effect,” Nano Lett. 7(3), 620–625 (2007).
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M. G. Raizen, R. J. Thompson, R. J. Brecha, H. J. Kimble, and H. J. Carmichael, “Normal-mode splitting and linewidth averaging for two-state atoms in an optical cavity,” Phys. Rev. Lett. 63(3), 240–243 (1989).
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W. L. Barnes, A. Dereux, and T. W. Ebbesen, “Surface plasmon subwavelength optics,” Nature 424(6950), 824–830 (2003).
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Figures (7)

Fig. 1
Fig. 1 Schematics of the Ag nanoislands sample on top of lamellar hyperbolic metamaterial (a) and glass (b). Scanning electron microscope (SEM) image of a typical Ag nanoislands film (c).
Fig. 2
Fig. 2 Absorbance spectra of the Ag nanoislands films (deposited on glass) without (a) and with (b) R6G:PMMA film on top. Black trace – absorbance spectrum of the R6G:PMMA film on glass and its decomposition into two bands (dashed lines). With increase of the nominal thickness of silver, Ag nanoislands become larger and the SP resonance shifts to longer wavelengths.
Fig. 3
Fig. 3 Reflectance spectra of the Ag nanoislands films (deposited on metamaterial) without (a) and with (b) R6G:PMMA film on top. Dashed green trace, corresponding to the same sample as solid green traces in figures (a) and (b), depicts typical reflectance spectrum of the lamellar metamaterial substrate before deposition of Ag nanoislands.
Fig. 4
Fig. 4 (a) Positions of the spectral peaks in the “Ag nanoislands+dye” samples, λ max SP+R6G , plotted versus localized surface plasmon resonance maxima in pristine Ag nanoisland films deposited on glass, λ max SP . Solid lines: fitting with Eq. (2). Dashed horizontal lines correspond to the peak (M) and the shoulder (D) in the R6G absorption spectrum. The dotted line is the function y = x. (b) Same for the dips in the reflectance spectra of the Ag nanoislands sample deposited on the hyperbolic metamaterial substrate.
Fig. 5
Fig. 5 (a) Schematics of the LBL Au nanoparticles film. (b) Transmission electron microscope (TEM) image of Au NPs. (c) Photograph of the [(PDDA/PSS)5 (PU/Au)3]5 LBL film.
Fig. 6
Fig. 6 Sample [(PDDA/PSS)5 (PU/Au)3]5. (a) Reflectance spectra of the pristine (1), single dipped (2) and double dipped (3) sample. Absorbance spectra of the R6G film and its fit with two Gaussian bands (black solid and dashed lines, respectively). The error bar in the bottom shows the accuracy of the reflectance measurement. (b) Transmittance spectra of the pristine (1) and single dipped (2) sample. The red arrow shows the reflectance maximum in Figure a. Inset of Figure a: Reflectance maximum of the pristine [(PDDA/PSS)5 (PU/Au)3]m film as the function of the number of deposition cycles m.
Fig. 7
Fig. 7 (a) Positions of spectral peaks in single dipped “Au LBL+dye” samples, λ max SP+R6G , plotted versus localized surface plasmon resonance maxima in pristine Au LBL films, λ max SP . Solid lines: fitting with Eq. (2). The dotted line is the function y = x. (b) Same as above for double dipped “Au LBL+dye” samples. The solid lines are linear trendlines.

Tables (1)

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Table 1 List of the Au LBL samples studied

Equations (2)

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H ^ =( E SP Δ Δ Δ E m 0 Δ 0 E D ),
det H ^ =| ( E SP E ) Δ Δ Δ ( E M E ) 0 Δ 0 ( E D E ) |=0,

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