Abstract

We introduce a manufacturable and scalable method for creating tunable wrinkled ferromagnetic-metallic structures to enhance fluorescence signals. Thin layers of nickel (Ni) and gold (Au) were deposited onto a pre-stressed thermoplastic (shrink wrap film) polymer. Heating briefly forced the metal films to buckle when the thermoplastic retracted, resulting in multi-scale composite ‘wrinkles’. This is the first demonstration of leveraging the plasmons in such hybrid nanostructures by metal enhanced fluorescence (MEF) in the near-infrared wavelengths. We observed more than three orders of magnitude enhancement in the fluorescence signal of a single molecule of goat anti-mouse immunoglobulin G (IgG) antibody conjugated to fluorescein isothiocyanate, FITC, (FITC-IgG) by two-photon excitation with these structures. These large enhancements in the fluorescence signal at the nanoscale gaps between the composite wrinkles corresponded to shortened lifetimes due to localized surface plasmons. To characterize these structures, we combined fluctuation correlation spectroscopy (FCS), fluorescence lifetime imaging microscopy (FLIM), and two-photon microscopy to spatially and temporally map the hot spots with high resolution.

© 2014 Optical Society of America

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2014

A. Chen, E. Lee, R. Tu, K. Santiago, A. Grosberg, C. Fowlkes, and M. Khine, “Integrated platform for functional monitoring of biomimetic heart sheets derived from human pluripotent stem cells,” Biomaterials35(2), 675–683 (2014).
[CrossRef] [PubMed]

2013

D. Nawarathna, N. Norouzi, J. McLane, H. Sharma, N. Sharac, T. Grant, A. Chen, S. Strayer, R. Ragan, and M. Khine, “Shrink-induced sorting using integrated nanoscale magnetic traps,” Appl. Phys. Lett.102(6), 063504 (2013).
[CrossRef] [PubMed]

J. D. Pegan, A. Y. Ho, M. Bachman, and M. Khine, “Flexible shrink-induced high surface area electrodes for electrochemiluminescent sensing,” Lab Chip13(21), 4205–4209 (2013).
[CrossRef] [PubMed]

Y. Y. Li, S. X. Dai, J. John, and K. R. Carter, “Superhydrophobic surfaces from hierarchically structured wrinkled polymers,” ACS Appl. Mater. Interfaces5(21), 11066–11073 (2013).
[CrossRef] [PubMed]

J. Y. Chin, T. Steinle, T. Wehlus, D. Dregely, T. Weiss, V. I. Belotelov, B. Stritzker, and H. Giessen, “Nonreciprocal plasmonics enables giant enhancement of thin-film Faraday rotation,” Nat Commun4, 1599 (2013).
[CrossRef] [PubMed]

S. Jayadev, J. Pegan, D. Dyer, J. McLane, J. Lim, and M. Khine, “Adaptive wettability-enhanced surfaces ordered on molded etched substrates using shrink film,” Smart Mater. Struct.22(1), 014014 (2013).
[CrossRef]

M. D. Huntington, C. J. Engel, A. J. Hryn, and T. W. Odom, “Polymer nanowrinkles with continuously tunable wavelengths,” ACS Appl. Mater. Interfaces5(13), 6438–6442 (2013).
[CrossRef] [PubMed]

C. M. Gabardo, Y. J. Zhu, L. Soleymani, and J. M. Moran-Mirabal, “Bench-top fabrication of hierarchically structured high-surface-area electrodes,” Adv. Funct. Mater.23(24), 3030–3039 (2013).
[CrossRef]

C. G. L. Ferri, R. H. Inman, B. Rich, A. Gopinathan, M. Khine, and S. Ghosh, “Plasmon-induced enhancement of intra-ensemble FRET in quantum dots on wrinkled thin films,” Opt. Mater. Express3(3), 383–389 (2013).
[CrossRef]

K. T. Takasaki, J. B. Ding, and B. L. Sabatini, “Live-cell superresolution imaging by pulsed STED two-photon excitation microscopy,” Biophys. J.104(4), 770–777 (2013).
[CrossRef] [PubMed]

Y. Zhang, B. Kim, S. Yao, M. V. Bondar, and K. D. Belfield, “Controlled aggregation and enhanced two-photon absorption of a water-soluble squaraine dye with a poly(acrylic acid) template,” Langmuir29(35), 11005–11012 (2013).
[CrossRef] [PubMed]

N. C. Lindquist, T. W. Johnson, P. Nagpal, D. J. Norris, and S. H. Oh, “Plasmonic nanofocusing with a metallic pyramid and an integrated C-shaped aperture,” Sci Rep3, 1857 (2013).
[CrossRef] [PubMed]

D. Punj, M. Mivelle, S. B. Moparthi, T. S. van Zanten, H. Rigneault, N. F. van Hulst, M. F. García-Parajó, and J. Wenger, “A plasmonic ‘antenna-in-box’ platform for enhanced single-molecule analysis at micromolar concentrations,” Nat. Nanotechnol.8(7), 512–516 (2013).
[CrossRef] [PubMed]

M. Pohl, L. E. Kreilkamp, V. I. Belotelov, I. A. Akimov, A. N. Kalish, N. E. Khokhlov, V. J. Yallapragada, A. V. Gopal, M. Nur-E-Alam, M. Vasiliev, D. R. Yakovlev, K. Alameh, A. K. Zvezdin, and M. Bayer, “Tuning of the transverse magneto-optical Kerr effect in magneto-plasmonic crystals,” New J. Phys.15(7), 075024 (2013).

J. Lim and S. A. Majetich, “Composite magnetic-plasmonic nanoparticles for biomedicine: manipulation and imaging,” Nano Today8(1), 98–113 (2013).
[CrossRef]

A. R. Halpern and R. M. Corn, “Lithographically patterned electrodeposition of gold, silver, and nickel nanoring arrays with widely tunable near-infrared plasmonic resonances,” ACS Nano7(2), 1755–1762 (2013).
[CrossRef] [PubMed]

G. Armelles, A. Cebollada, A. Garcia-Martin, and M. U. Gonzalez, “Magnetoplasmonics: combining magnetic and plasmonic functionalities,” Adv. Opt. Mater.1(1), 10–35 (2013).
[CrossRef]

2012

K. Uetsuki, P. Verma, P. Nordlander, and S. Kawata, “Tunable plasmon resonances in a metallic nanotip-film system,” Nanoscale4(19), 5931–5935 (2012).
[CrossRef] [PubMed]

J. H. Vella and A. M. Urbas, “Nanoplasmonic array enhancement of two-photon absorption in a dye film,” J. Phys. Chem. C116(32), 17169–17173 (2012).
[CrossRef]

L. C. Estrada, M. J. Roberti, S. Simoncelli, V. Levi, P. F. Aramendía, and O. E. Martínez, “Detection of low quantum yield fluorophores and improved imaging times using metallic nanoparticles,” J. Phys. Chem. B116(7), 2306–2313 (2012).
[CrossRef] [PubMed]

P. Zhu and H. G. Craighead, “Zero-mode waveguides for single-molecule analysis,” Annu Rev Biophys41(1), 269–293 (2012).
[CrossRef] [PubMed]

W. H. Zhang, F. Ding, W. D. Li, Y. X. Wang, J. Hu, and S. Y. Chou, “Giant and uniform fluorescence enhancement over large areas using plasmonic nanodots in 3D resonant cavity nanoantenna by nanoimprinting,” Nanotechnology23(22), 225301 (2012).
[CrossRef] [PubMed]

T. Lohmüller, L. Iversen, M. Schmidt, C. Rhodes, H. L. Tu, W. C. Lin, and J. T. Groves, “Single molecule tracking on supported membranes with arrays of optical nanoantennas,” Nano Lett.12(3), 1717–1721 (2012).
[CrossRef] [PubMed]

L. R. Freschauf, J. McLane, H. Sharma, and M. Khine, “Shrink-induced superhydrophobic and antibacterial surfaces in consumer plastics,” PLoS ONE7(8), e40987 (2012).
[CrossRef] [PubMed]

J. C. Banthí, D. Meneses-Rodríguez, F. García, M. U. González, A. García-Martín, A. Cebollada, and G. Armelles, “High magneto-optical activity and low optical losses in metal-dielectric Au/Co/Au-SiO2 magnetoplasmonic nanodisks,” Adv. Mater.24(10), OP36–OP41 (2012).
[PubMed]

2011

L. Zhang, X. Y. Lang, A. Hirata, and M. W. Chen, “Wrinkled nanoporous gold films with ultrahigh surface-enhanced Raman scattering enhancement,” ACS Nano5(6), 4407–4413 (2011).
[CrossRef] [PubMed]

H. W. Liu, L. Zhang, X. Y. Lang, Y. Yamaguchi, H. S. Iwasaki, Y. S. Inouye, Q. K. Xue, and M. W. Chen, “Single molecule detection from a large-scale SERS-active Au79Ag21 substrate,” Sci. Rep.1, 1–5 (2011).
[CrossRef] [PubMed]

A. Chen, D. K. Lieu, L. Freschauf, V. Lew, H. Sharma, J. X. Wang, D. Nguyen, I. Karakikes, R. J. Hajjar, A. Gopinathan, E. Botvinick, C. C. Fowlkes, R. A. Li, and M. Khine, “Shrink-film configurable multiscale wrinkles for functional alignment of human embryonic stem cells and their cardiac derivatives,” Adv. Mater.23(48), 5785–5791 (2011).
[CrossRef] [PubMed]

C. Stringari, A. Cinquin, O. Cinquin, M. A. Digman, P. J. Donovan, and E. Gratton, “Phasor approach to fluorescence lifetime microscopy distinguishes different metabolic states of germ cells in a live tissue,” Proc. Natl. Acad. Sci. U.S.A.108(33), 13582–13587 (2011).
[CrossRef] [PubMed]

V. I. Belotelov, I. A. Akimov, M. Pohl, V. A. Kotov, S. Kasture, A. S. Vengurlekar, A. V. Gopal, D. R. Yakovlev, A. K. Zvezdin, and M. Bayer, “Enhanced magneto-optical effects in magnetoplasmonic crystals,” Nat. Nanotechnol.6(6), 370–376 (2011).
[CrossRef] [PubMed]

D. Regatos, B. Sepúlveda, D. Fariña, L. G. Carrascosa, and L. M. Lechuga, “Suitable combination of noble/ferromagnetic metal multilayers for enhanced magneto-plasmonic biosensing,” Opt. Express19(9), 8336–8346 (2011).
[CrossRef] [PubMed]

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2002

W. Wenseleers, F. Stellacci, T. Meyer-Friedrichsen, T. Mangel, C. A. Bauer, S. J. K. Pond, S. R. Marder, and J. W. Perry, “Five orders-of-magnitude enhancement of two-photon absorption for dyes on silver nanoparticle fractal clusters,” J. Phys. Chem. B106(27), 6853–6863 (2002).
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J. F. Torrado, J. B. González-Díaz, M. U. González, A. García-Martín, and G. Armelles, “Magneto-optical effects in interacting localized and propagating surface plasmon modes,” Opt. Express18(15), 15635–15642 (2010).
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J. C. Banthí, D. Meneses-Rodríguez, F. García, M. U. González, A. García-Martín, A. Cebollada, and G. Armelles, “High magneto-optical activity and low optical losses in metal-dielectric Au/Co/Au-SiO2 magnetoplasmonic nanodisks,” Adv. Mater.24(10), OP36–OP41 (2012).
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M. Pohl, L. E. Kreilkamp, V. I. Belotelov, I. A. Akimov, A. N. Kalish, N. E. Khokhlov, V. J. Yallapragada, A. V. Gopal, M. Nur-E-Alam, M. Vasiliev, D. R. Yakovlev, K. Alameh, A. K. Zvezdin, and M. Bayer, “Tuning of the transverse magneto-optical Kerr effect in magneto-plasmonic crystals,” New J. Phys.15(7), 075024 (2013).

V. I. Belotelov, I. A. Akimov, M. Pohl, V. A. Kotov, S. Kasture, A. S. Vengurlekar, A. V. Gopal, D. R. Yakovlev, A. K. Zvezdin, and M. Bayer, “Enhanced magneto-optical effects in magnetoplasmonic crystals,” Nat. Nanotechnol.6(6), 370–376 (2011).
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I. Cohanoschi, S. Yao, K. D. Belfield, and F. E. Hernandez, “Effect of the concentration of organic dyes on their surface plasmon enhanced two-photon absorption cross section using activated Au nanoparticles,” J. Appl. Phys.101(8), 086112 (2007).
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M. Pohl, L. E. Kreilkamp, V. I. Belotelov, I. A. Akimov, A. N. Kalish, N. E. Khokhlov, V. J. Yallapragada, A. V. Gopal, M. Nur-E-Alam, M. Vasiliev, D. R. Yakovlev, K. Alameh, A. K. Zvezdin, and M. Bayer, “Tuning of the transverse magneto-optical Kerr effect in magneto-plasmonic crystals,” New J. Phys.15(7), 075024 (2013).

J. Y. Chin, T. Steinle, T. Wehlus, D. Dregely, T. Weiss, V. I. Belotelov, B. Stritzker, and H. Giessen, “Nonreciprocal plasmonics enables giant enhancement of thin-film Faraday rotation,” Nat Commun4, 1599 (2013).
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K. M. Berland, P. T. So, Y. Chen, W. W. Mantulin, and E. Gratton, “Scanning two-photon fluctuation correlation spectroscopy: particle counting measurements for detection of molecular aggregation,” Biophys. J.71(1), 410–420 (1996).
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L. Novotny, R. X. Bian, and X. S. Xie, “Theory of nanometric optical tweezers,” Phys. Rev. Lett.79(4), 645–648 (1997).
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R. M. Bakker, H. K. Yuan, Z. T. 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).
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J. Chen, P. Albella, Z. Pirzadeh, P. Alonso-González, F. Huth, S. Bonetti, V. Bonanni, J. Akerman, J. Nogués, P. Vavassori, A. Dmitriev, J. Aizpurua, and R. Hillenbrand, “Plasmonic nickel nanoantennas,” Small7(16), 2341–2347 (2011).
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Y. Zhang, B. Kim, S. Yao, M. V. Bondar, and K. D. Belfield, “Controlled aggregation and enhanced two-photon absorption of a water-soluble squaraine dye with a poly(acrylic acid) template,” Langmuir29(35), 11005–11012 (2013).
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J. Chen, P. Albella, Z. Pirzadeh, P. Alonso-González, F. Huth, S. Bonetti, V. Bonanni, J. Akerman, J. Nogués, P. Vavassori, A. Dmitriev, J. Aizpurua, and R. Hillenbrand, “Plasmonic nickel nanoantennas,” Small7(16), 2341–2347 (2011).
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V. V. Temnov, G. Armelles, U. Woggon, D. Guzatov, A. Cebollada, A. Garcia-Martin, J. M. Garcia-Martin, T. Thomay, A. Leitenstorfer, and R. Bratschitsch, “Active magneto-plasmonics in hybrid metal-ferromagnet structures,” Nat. Photonics4(2), 107–111 (2010).
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G. Armelles, A. Cebollada, A. Garcia-Martin, and M. U. Gonzalez, “Magnetoplasmonics: combining magnetic and plasmonic functionalities,” Adv. Opt. Mater.1(1), 10–35 (2013).
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J. C. Banthí, D. Meneses-Rodríguez, F. García, M. U. González, A. García-Martín, A. Cebollada, and G. Armelles, “High magneto-optical activity and low optical losses in metal-dielectric Au/Co/Au-SiO2 magnetoplasmonic nanodisks,” Adv. Mater.24(10), OP36–OP41 (2012).
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J. Chen, P. Albella, Z. Pirzadeh, P. Alonso-González, F. Huth, S. Bonetti, V. Bonanni, J. Akerman, J. Nogués, P. Vavassori, A. Dmitriev, J. Aizpurua, and R. Hillenbrand, “Plasmonic nickel nanoantennas,” Small7(16), 2341–2347 (2011).
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S. M. Williams, A. D. Stafford, K. R. Rodriguez, T. M. Rogers, and J. V. Coe, “Accessing surface plasmons with Ni microarrays for enhanced IR absorption by monolayers,” J. Phys. Chem. B107(43), 11871–11879 (2003).
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I. Cohanoschi, S. Yao, K. D. Belfield, and F. E. Hernandez, “Effect of the concentration of organic dyes on their surface plasmon enhanced two-photon absorption cross section using activated Au nanoparticles,” J. Appl. Phys.101(8), 086112 (2007).
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ACS Nano

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Adv. Mater.

C. C. Fu, A. Grimes, M. Long, C. G. L. Ferri, B. D. Rich, S. Ghosh, S. Ghosh, L. P. Lee, A. Gopinathan, and M. Khine, “Tunable nanowrinkles on shape memory polymer sheets,” Adv. Mater.21(44), 4472–4476 (2009).
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Adv. Opt. Mater.

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Appl. Opt.

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R. M. Bakker, H. K. Yuan, Z. T. 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).
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Biomaterials

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Biophys. J.

K. T. Takasaki, J. B. Ding, and B. L. Sabatini, “Live-cell superresolution imaging by pulsed STED two-photon excitation microscopy,” Biophys. J.104(4), 770–777 (2013).
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Circ. Res.

M. Rubart, “Two-photon microscopy of cells and tissue,” Circ. Res.95(12), 1154–1166 (2004).
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Imaging & Microscopy

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I. Cohanoschi, S. Yao, K. D. Belfield, and F. E. Hernandez, “Effect of the concentration of organic dyes on their surface plasmon enhanced two-photon absorption cross section using activated Au nanoparticles,” J. Appl. Phys.101(8), 086112 (2007).
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J. Biomed. Opt.

C. Tregidgo, J. A. Levitt, and K. Suhling, “Effect of refractive index on the fluorescence lifetime of green fluorescent protein,” J. Biomed. Opt.13(3), 031218 (2008).
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Y. Fu, J. Zhang, and J. R. Lakowicz, “Plasmonic enhancement of single-molecule fluorescence near a silver nanoparticle,” J. Fluoresc.17(6), 811–816 (2007).
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Lab Chip

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Langmuir

Y. Zhang, B. Kim, S. Yao, M. V. Bondar, and K. D. Belfield, “Controlled aggregation and enhanced two-photon absorption of a water-soluble squaraine dye with a poly(acrylic acid) template,” Langmuir29(35), 11005–11012 (2013).
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Nano Today

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Nanoscale

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Nanotechnology

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Nat Commun

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Nat. Photonics

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Opt. Express

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PLoS ONE

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Sci Rep

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Figures (4)

Fig. 1
Fig. 1

Characterization of bimetallic structures (a) Process flow for creating islands of bimetallic structures on PO. SEM images of composite structures with different thickness of Au (b) 10 nm, (c) 20 nm, (d) 30 nm. Black arrow in (b) indicates a nanogap.

Fig. 2
Fig. 2

SEM characterization of composite structures with fixed 10 nm Au and varying thicknesses of Ni (a) 5 nm, (b) 15 nm, (c) 25 nm.

Fig. 3
Fig. 3

Fluorescence line scan analysis of 1 µM FITC-IgG and PBS at 785 nm excitation on glass coverslip and composite structures (a) Fluorescence image from scanning FCS of composite structure where hotspots were observed indicated by white arrow (b) Horizontal line intensity profile for fixed time point (c) Vertical line intensity profile for a fixed pixel position collected for 60 sec (d) Histogram distribution profile of the fluorescence intensities.

Fig. 4
Fig. 4

Fluorescence lifetime analysis of 1 µM FITC-IgG at 785 nm excitation. (a) FLIM image on glass (b) FLIM image on composite structures (c) Phasor plot to show lifetime distribution (d) Normalized frequency profile of lifetimes.

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