Abstract

Thin films containing light emitters act as light-to-light converters that absorb the incident light and emit luminescence. This well-known phenomenon is photoluminescence (PL). When a photoluminescent film is notably thinner than the absorption length of emitters, it exhibits weak absorption of incident light. The absorption can be increased by depositing the thin film on a plasmonic array of metallic nanocylinders arranged with a specific periodicity. The array couples the incident light into the thin film, facilitating the plasmon-enhanced absorption by the emitters in the film. In this study, we demonstrate both experimentally and numerically the plasmon-enhanced absorption of a rhodamine 6G-containing film that is thinner than its absorption length using a periodic array of Al nanocylinders. The experimental results demonstrate that the spectrally integrated PL intensity is increased up to 3.78 times. In addition to enhanced absorption, the array is also found to diffract the PL into a direction determined by the periodicity, thereby facilitating the multiplied enhancement of PL. The combination of the two factors yields a PL intensity enhanced up to 10 times at a specific angle and wavelength. Numerical simulations combining the carrier kinetics with full-wave electromagnetics in the time-domain support the experimental observations.

© 2019 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

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References

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    [Crossref]

2018 (3)

V. G. Kravets, A. V. Kabashin, W. L. Barnes, and A. N. Grigorenko, “Plasmonic surface lattice resonances: A review of properties and applications,” Chem. Rev. 118(12), 5912–5951 (2018).
[Crossref] [PubMed]

Y. Kawachiya, S. Murai, M. Saito, H. Sakamoto, K. Fujita, and K. Tanaka, “Collective plasmonic modes excited in Al nanocylinder arrays in the UV spectral region,” Opt. Express 26(5), 5970–5982 (2018).
[Crossref] [PubMed]

R. Kamakura, S. Murai, Y. Yokobayashi, K. Takashima, M. Kuramoto, K. Fujita, and K. Tanaka, “Enhanced photoluminescence and directional white-light generation by plasmonic array,” J. Appl. Phys. 124(21), 213105 (2018).
[Crossref]

2017 (5)

Z. Hosseini, N. Taghavinia, and E. Wei-Guang Diau, “Luminescent spectral conversion to improve the performance of dye-sensitized solar cells,” ChemPhysChem 18(23), 3292–3308 (2017).
[Crossref] [PubMed]

S. Murai, M. Saito, H. Sakamoto, M. Yamamoto, R. Kamakura, T. Nakanishi, K. Fujita, M. Verschuuren, Y. Hasegawa, and K. Tanaka, “Directional outcoupling of photoluminescence from Eu (III)-complex thin films by plasmonic array,” APL Photonics 2(2), 026104 (2017).
[Crossref]

F. Laux, N. Bonod, and D. Gerard, “Single emitter fluorescence enhancement with surface lattice resonances,” J. Phys. Chem. C 121(24), 13280–13289 (2017).
[Crossref]

Y. Zhao, N. Hoivik, M. N. Akram, and K. Wang, “Study of plasmonics induced optical absorption enhancement of Au embedded in titanium dioxide nanohole arrays,” Opt. Mater. Express 7(8), 2871–2879 (2017).
[Crossref]

J. S. T. Smalley, F. Vallini, S. A. Montoya, L. Ferrari, S. Shahin, C. T. Riley, B. Kanté, E. E. Fullerton, Z. Liu, and Y. Fainman, “Luminescent hyperbolic metasurfaces,” Nat. Commun. 8, 13793 (2017).
[Crossref] [PubMed]

2016 (1)

G. Lozano, S. R. K. Rodriguez, M. A. Verschuuren, and J. Gómez Rivas, “Metallic nanostructures for efficient LED lighting,” Light Sci. Appl. 5(6), e16080 (2016).
[Crossref] [PubMed]

2015 (2)

2014 (2)

D. Lu, J. J. Kan, E. E. Fullerton, and Z. Liu, “Enhancing spontaneous emission rates of molecules using nanopatterned multilayer hyperbolic metamaterials,” Nat. Nanotechnol. 9(1), 48–53 (2014).
[Crossref] [PubMed]

X. Meng, J. Liu, A. V. Kildishev, and V. M. Shalaev, “Highly directional spaser array for the red wavelength region,” Laser Photonics Rev. 8(6), 896–903 (2014).
[Crossref]

2013 (7)

A. V. Dorofeenko, A. A. Zyablovsky, A. P. Vinogradov, E. S. Andrianov, A. A. Pukhov, and A. A. Lisyansky, “Steady state superradiance of a 2D-spaser array,” Opt. Express 21(12), 14539–14547 (2013).
[Crossref] [PubMed]

F. van Beijnum, P. J. van Veldhoven, E. J. Geluk, M. J. A. de Dood, G. W. ’t Hooft, and M. P. van Exter, “Surface plasmon lasing observed in metal hole arrays,” Phys. Rev. Lett. 110(20), 206802 (2013).
[Crossref] [PubMed]

W. Zhou, M. Dridi, J. Y. Suh, C. H. Kim, D. T. Co, M. R. Wasielewski, G. C. Schatz, and T. W. Odom, “Lasing action in strongly coupled plasmonic nanocavity arrays,” Nat. Nanotechnol. 8(7), 506–511 (2013).
[Crossref] [PubMed]

M. Saboktakin, X. Ye, U. K. Chettiar, N. Engheta, C. B. Murray, and C. R. Kagan, “Plasmonic Enhancement of Nanophosphor Upconversion Luminescence in Au Nanohole Arrays,” ACS Nano 7(8), 7186–7192 (2013).
[Crossref] [PubMed]

S. Murai, M. A. Verschuuren, G. Lozano, G. Pirruccio, S. R. K. Rodriguez, and J. G. Rivas, “Hybrid plasmonic-photonic modes in diffractive arrays of nanoparticles coupled to light-emitting optical waveguides,” Opt. Express 21(4), 4250–4262 (2013).
[Crossref] [PubMed]

M. Y. Shalaginov, S. Ishii, J. Liu, J. Liu, J. Irudayaraj, A. Lagutchev, A. V. Kildishev, and V. M. Shalaev, “Broadband enhancement of spontaneous emission from nitrogen-vacancy centers in nanodiamonds by hyperbolic metamaterials,” Appl. Phys. Lett. 102(17), 173114 (2013).
[Crossref]

G. Lozano, D. J. Louwers, S. R. K. Rodríguez, S. Murai, O. T. A. Jansen, M. A. Verschuuren, and J. Gómez Rivas, “Plasmonics for solid-state lighting: enhanced excitation and directional emission of highly efficient light sources,” Light Sci. Appl. 2(5), e66 (2013).
[Crossref]

2011 (2)

T. Coenen, E. J. R. Vesseur, A. Polman, and A. F. Koenderink, “Directional emission from plasmonic Yagi-Uda antennas probed by angle-resolved cathodoluminescence spectroscopy,” Nano Lett. 11(9), 3779–3784 (2011).
[Crossref] [PubMed]

C.-H. Lu, C.-C. Lan, Y.-L. Lai, Y.-L. Li, and C.-P. Liu, “Enhancement of Green Emission from InGaN/GaN multiple quantum wells via coupling to surface plasmons in a two-dimensional silver array,” Adv. Funct. Mater. 21(24), 4719–4723 (2011).
[Crossref]

2010 (3)

K. Tanaka, E. Plum, J. Y. Ou, T. Uchino, and N. I. Zheludev, “Multifold Enhancement of Quantum Dot Luminescence in Plasmonic Metamaterials,” Phys. Rev. Lett. 105(22), 227403 (2010).
[Crossref] [PubMed]

T. Kosako, Y. Kadoya, and H. F. Hofmann, “Directional control of light by a nano-optical Yagi-Uda antenna,” Nat. Photonics 4(5), 312–315 (2010).
[Crossref]

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

2009 (2)

G. Vecchi, V. Giannini, and J. Gómez Rivas, “Surface modes in plasmonic crystals induced by diffractive coupling of nanoantennas,” Phys. Rev. B Condens. Matter Mater. Phys. 80(20), 201401 (2009).
[Crossref]

A. Kinkhabwala, Z. F. Yu, S. H. Fan, Y. Avlasevich, K. Mullen, and W. E. Moerner, “Large single-molecule fluorescence enhancements produced by a bowtie nanoantenna,” Nat. Photonics 3(11), 654–657 (2009).
[Crossref]

2008 (6)

R. M. Bakker, H.-K. Yuan, Z. Liu, V. P. Drachev, A. V. Kildishev, V. M. Shalaev, R. H. Pedersen, S. Gresillon, and A. Boltasseva, “Enhanced localized fluorescence in plasmonic nanoantennae,” Appl. Phys. Lett. 92(4), 043101 (2008).
[Crossref]

J. R. Lakowicz, K. Ray, M. Chowdhury, H. Szmacinski, Y. Fu, J. Zhang, and K. Nowaczyk, “Plasmon-controlled fluorescence: a new paradigm in fluorescence spectroscopy,” Analyst (Lond.) 133(10), 1308 (2008).
[Crossref]

V. G. Kravets, F. Schedin, and A. N. Grigorenko, “Extremely narrow plasmon resonances based on diffraction coupling of localized plasmons in arrays of metallic nanoparticles,” Phys. Rev. Lett. 101(8), 087403 (2008).
[Crossref] [PubMed]

B. Auguié and W. L. Barnes, “Collective resonances in gold nanoparticle arrays,” Phys. Rev. Lett. 101(14), 143902 (2008).
[Crossref] [PubMed]

Y. Z. Chu, E. Schonbrun, T. Yang, and K. B. Crozier, “Experimental observation of narrow surface plasmon resonances in gold nanoparticle arrays,” Appl. Phys. Lett. 93(18), 181108 (2008).
[Crossref]

V. E. Ferry, L. A. Sweatlock, D. Pacifici, and H. A. Atwater, “Plasmonic nanostructure design for efficient light coupling into solar cells,” Nano Lett. 8(12), 4391–4397 (2008).
[Crossref] [PubMed]

2007 (1)

O. L. Muskens, V. Giannini, J. A. Sánchez-Gil, and J. Gómez Rivas, “Strong Enhancement of the Radiative Decay Rate of Emitters by Single Plasmonic Nanoantennas,” Nano Lett. 7(9), 2871–2875 (2007).
[Crossref] [PubMed]

2006 (2)

P. Anger, P. Bharadwaj, and L. Novotny, “Enhancement and quenching of single-molecule fluorescence,” Phys. Rev. Lett. 96(11), 113002 (2006).
[Crossref] [PubMed]

M. A. Noginov, G. Zhu, M. Bahoura, C. E. Small, C. Davison, J. Adegoke, V. P. Drachev, P. Nyga, and V. M. Shalaev, “Enhancement of spontaneous and stimulated emission of a rhodamine 6G dye by an Ag aggregate,” Phys. Rev. B Condens. Matter Mater. Phys. 74(18), 184203 (2006).
[Crossref]

2005 (2)

J. Feng, T. Okamoto, and S. Kawata, “Highly directional emission via coupled surface-plasmon tunneling from electroluminescence in organic light-emitting devices,” Appl. Phys. Lett. 87(24), 241109 (2005).
[Crossref]

A. G. Brolo, S. C. Kwok, M. G. Moffitt, R. Gordon, J. Riordon, and K. L. Kavanagh, “Enhanced Fluorescence from Arrays of Nanoholes in a Gold Film,” J. Am. Chem. Soc. 127(42), 14936–14941 (2005).
[Crossref] [PubMed]

2004 (3)

S. Zou, N. Janel, and G. C. Schatz, “Silver nanoparticle array structures that produce remarkably narrow plasmon lineshapes,” J. Chem. Phys. 120(23), 10871–10875 (2004).
[Crossref] [PubMed]

K. Okamoto, I. Niki, A. Shvartser, Y. Narukawa, T. Mukai, and A. Scherer, “Surface-plasmon-enhanced light emitters based on InGaN quantum wells,” Nat. Mater. 3(9), 601–605 (2004).
[Crossref] [PubMed]

T. Okamoto, F. H’Dhili, and S. Kawata, “Towards plasmonic band gap laser,” Appl. Phys. Lett. 85(18), 3968–3970 (2004).
[Crossref]

2000 (1)

X. Jiang and C. M. Soukoulis, “Time dependent theory for random lasers,” Phys. Rev. Lett. 85(1), 70–73 (2000).
[Crossref] [PubMed]

1979 (1)

H. J. Hovel, R. T. Hodgson, and J. M. Woodall, “The effect of fluorescent wavelength shifting on solar cell spectral response,” Sol. Energy Mater. 2(1), 19–29 (1979).
[Crossref]

1974 (1)

R. R. Chance, A. Prock, and R. Silbey, “Lifetime of an excited molecule near a metal mirror: Energy transfer in the Eu3+/silver system,” J. Chem. Phys. 60(5), 2184–2185 (1974).
[Crossref]

1973 (1)

K. H. Tews, “Zur Variation von Lumineszens-Lebensdauern,” Ann. Phys. (Leipz.) 29(2), 97–120 (1973).
[Crossref]

1970 (1)

K. H. Drexhage, “Influence of a dielectric interface on fluorescence decay time,” J. Lumin. 1–2, 693–701 (1970).
[Crossref]

1969 (1)

H. Morawitz, “Self-coupling of a two-level system by a mirror,” Phys. Rev. 187(5), 1792–1796 (1969).
[Crossref]

’t Hooft, G. W.

F. van Beijnum, P. J. van Veldhoven, E. J. Geluk, M. J. A. de Dood, G. W. ’t Hooft, and M. P. van Exter, “Surface plasmon lasing observed in metal hole arrays,” Phys. Rev. Lett. 110(20), 206802 (2013).
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Adegoke, J.

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[Crossref] [PubMed]

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V. G. Kravets, A. V. Kabashin, W. L. Barnes, and A. N. Grigorenko, “Plasmonic surface lattice resonances: A review of properties and applications,” Chem. Rev. 118(12), 5912–5951 (2018).
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V. E. Ferry, L. A. Sweatlock, D. Pacifici, and H. A. Atwater, “Plasmonic nanostructure design for efficient light coupling into solar cells,” Nano Lett. 8(12), 4391–4397 (2008).
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Figures (9)

Fig. 1
Fig. 1 Refractive index and extinction coefficient of the PMMA + R6G film extracted from the fit of a Lorentzian model to the spectroscopic ellipsometry data, i.e., ε(ω)= ε inf + f ω 0 2 / ( ω 0 2 ω 2 +iγω ) , with ε inf =2.3185, f=6.8755× 10 4 ( eV ), ω 0 =2.3396 ( eV ),and γ= 0.0722 ( eV ).
Fig. 2
Fig. 2 (a) Sketch of the unit cell of simulated structure used for a 3D multiphysics framework based on FDTD Maxwell solver with embedded quantum emitters. The top panel displays the x-y plane (top view) of the structure. The black circle indicates the Al nanocylinder. Periodic boundary conditions are applied in x- and y-directions to simulate the square lattice with periodicity a = 400 nm. The bottom panel shows the x-z plane (side view) of the structure. The thicknesses of the PMMA + R6G film, t, and the SiO2 glass substrate, tsub, were 700 and 2000 nm, respectively. (b) Sketch of the four-level energy diagram simulating the electronic transition of R6G.
Fig. 3
Fig. 3 (a) Top-view SEM image of the array. Scale bar = 500 nm. The x-, y-, and z-axes used in this study are also defined. The inset is the experimental configuration: the incident light is polarized along the y-direction (s-polarized), and θin was varied in the z-x plane, with the azimuth angle being fixed. (b), (c) Wavelength and incident angle dependence of zeroth-order transmission for the array without (b) and with (c) the PMMA + R6G thin film. The dashed curves are the diffraction conditions (Eq. (4)) with different orders. (d) Cuts of transmittance at θin = 0 ° for the array without (top) and with (bottom) the PMMA + R6G thin film.
Fig. 4
Fig. 4 (a) Absorptance, A, calculated by the relation A = 1 – Transmittance – Reflectance for s-polarized light at θin = 5°. The solid line represents A for the PMMA + R6G film on the array (Aarray + R6G), while the grey area is for the same film on the flat substrate (AR6G). The arrows show the in-plane diffraction conditions. (b) Absorptance enhancement by the array, Aarray + R6G / AR6G.
Fig. 5
Fig. 5 (a) Emission angle θem dependence of PL enhancement for λex = 445 (top), 473 (middle), and 532 nm (bottom), respectively. θem was varied from 0 to 30 °, with θin being fixed to 5°. PL enhancement was defined as the spectra from the sample (Iarray + R6G) divided by that of the reference (IR6G), i.e., Iarray + R6G/IR6G. The inset shows the configuration where θem is varied in z-x-plane. (b) PL spectra at θin = 5° and collected at θem = 0°(see the inset). The dots and grey area represent the spectra from the sample and the reference, respectively. λex = 445 (top panel), 473 (middle), and 532 nm (bottom). The sharp peak in the bottom panel denoted by an arrow is the excitation laser line. (c) PL enhancement, defined as Iarray + R6G/IR6G for λex = 445, 473, and 532 nm, respectively (left axis) and zeroth-order T at θin = 0° (right). (d) Comparison between Aarray + R6G/AR6G at λex and Iarray + R6G/IR6G averaged spectrally over λ = 545 to 650 nm.
Fig. 6
Fig. 6 PL decay curves of the PMMA + R6G film on the array (red curve) and that on the glass substrate(black). The excitation wavelength was 470 nm.
Fig. 7
Fig. 7 Simulated absorptance spectra of PMMA + R6G films (thickness = 700 nm) at θin = 5° on the Al nanocylinder array (Aarray + R6G) (denoted as a red line) and that on the flat glass substrate (AR6G) (grey area)
Fig. 8
Fig. 8 Simulated PL spectra at θin = 5° and θem = 0°. The solid line and grey area represent the spectra from the sample (Iarray + R6G) and the reference (IR6G), respectively. λex = 445 (top panel), 473 (middle), and 532 nm (bottom).
Fig. 9
Fig. 9 Comparison between the simulated Aarray + R6G/AR6G (left axis) and Iarray + R6G/IR6G averaged spectrally over λ = 545 to 650 nm (right).

Tables (2)

Tables Icon

Table 1 Parameter list for numerical simulations.

Tables Icon

Table 2 Absorption lengths at the three wavelengths in the reference film calculated by the relation 1 – A = exp(–t/a) where t is the film thickness for s-polarized light at θin = 5°.

Equations (7)

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

N 3 t = N 3 τ 32 + 1 ω 30 E P 30 t
N 2 t = N 3 τ 32 N 2 τ 21 + 1 ω 21 E P 21 t
N 1 t = N 2 τ 21 N 1 τ 10 1 ω 21 E P 21 t
N 0 t = N 1 τ 10 1 ω 30 E P 30 t
2 P ij t 2 +Δ ω ij P ij t + ω ij 2 P ij = k ij ( N j N i )E
×H= ε 0 ε h E t + ij P ij
k out|| 2 = [ k in + m 1 ( 2π a ) ] 2 + m 2 2 ( 2π a ) 2 ,