Abstract

We report the plasmon hybridization between silver nanoprisms and a thin gold film as a means to tune the plasmon resonance and to achieve enhanced optical second harmonic generation. The hybridization enhances the second harmonic counts by nearly three orders of magnitude when varying the spacer layer between the nanoprisms and the gold film. Finite-difference time-domain calculations agree within a factor of 2 with the experimental findings in terms of the predicted enhancement factor. This plasmon hybridization approach is promising for future applications, including multi-photon lithography and nonlinear sensing using metal nanoparticles.

© 2012 OSA

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    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
  39. J. E. Millstone, S. J. Hurst, G. S. Métraux, J. I. Cutler, and C. A. Mirkin, “Colloidal gold and silver triangular nanoprisms,” Small5(6), 646–664 (2009).
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    [CrossRef]
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    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]

2012

H. Aouani, M. Navarro-Cia, M. Rahmani, T. P. H. Sidiropoulos, M. Hong, R. F. Oulton, and S. A. Maier, “Multiresonant broadband optical antennas as efficient tunable nanosources of second harmonic light,” Nano Lett.12(9), 4997–5002 (2012).
[CrossRef] [PubMed]

S. Linden, F. B. P. Niesler, J. Förstner, Y. Grynko, T. Meier, and M. Wegener, “Collective effects in second-harmonic generation from split-ring-resonator arrays,” Phys. Rev. Lett.109(1), 015502–015506 (2012).
[CrossRef] [PubMed]

M. Hentschel, T. Utikal, H. Giessen, and M. Lippitz, “Quantitative modeling of the third harmonic emission spectrum of plasmonic nanoantennas,” Nano Lett.12(7), 3778–3782 (2012).
[CrossRef] [PubMed]

T. Hanke, J. Cesar, V. Knittel, A. Trügler, U. Hohenester, A. Leitenstorfer, and R. Bratschitsch, “Tailoring spatiotemporal light confinement in single plasmonic nanoantennas,” Nano Lett.12(2), 992–996 (2012).
[CrossRef] [PubMed]

H. Harutyunyan, G. Volpe, R. Quidant, and L. Novotny, “Enhancing the nonlinear optical response using multifrequency gold-nanowire antennas,” Phys. Rev. Lett.108(21), 217403 (2012).
[CrossRef] [PubMed]

G. Volpe, M. Noack, S. S. Aćimović, C. Reinhardt, and R. Quidant, “Near-field mapping of plasmonic antennas by multiphoton absorption in poly(methyl methacrylate),” Nano Lett.12(9), 4864–4868 (2012).
[CrossRef] [PubMed]

D. Y. Lei, A. I. Fernández-Domínguez, Y. Sonnefraud, K. Appavoo, R. F. Haglund, J. B. Pendry, and S. A. Maier, “Revealing plasmonic gap modes in particle-on-film systems using dark-field spectroscopy,” ACS Nano6(2), 1380–1386 (2012).
[CrossRef] [PubMed]

J. J. Mock, R. T. Hill, Y.-J. Tsai, A. Chilkoti, and D. R. Smith, “Probing dynamically tunable localized surface plasmon resonances of film-coupled nanoparticles by evanescent wave excitation,” Nano Lett.12(4), 1757–1764 (2012).
[CrossRef] [PubMed]

C. Lumdee, S. Toroghi, and P. G. Kik, “Post-fabrication voltage controlled resonance tuning of nanoscale plasmonic antennas,” ACS Nano6(7), 6301–6307 (2012).
[CrossRef] [PubMed]

D. Wang, W. Zhu, Y. Chu, and K. B. Crozier, “High directivity optical antenna substrates for surface enhanced Raman scattering,” Adv. Mater. (Deerfield Beach Fla.)24(32), 4376–4380 (2012).
[CrossRef] [PubMed]

C. Ciracì, R. T. Hill, J. J. Mock, Y. Urzhumov, A. I. Fernández-Domínguez, S. A. Maier, J. B. Pendry, A. Chilkoti, and D. R. Smith, “Probing the ultimate limits of plasmonic enhancement,” Science337(6098), 1072–1074 (2012).
[CrossRef] [PubMed]

J. Butet, I. Russier-Antoine, C. Jonin, N. Lascoux, E. Benichou, and P.-F. Brevet, “Sensing with multipolar second harmonic generation from spherical metallic nanoparticles,” Nano Lett.12(3), 1697–1701 (2012).
[CrossRef] [PubMed]

K. Thyagarajan, S. Rivier, A. Lovera, and O. J. F. Martin, “Enhanced second-harmonic generation from double resonant plasmonic antennae,” Opt. Express20(12), 12860–12865 (2012).
[CrossRef] [PubMed]

2011

Q. Min, Y. Pang, D. J. Collins, N. A. Kuklev, K. Gottselig, D. W. Steuerman, and R. Gordon, “Substrate-based platform for boosting the surface-enhanced Raman of plasmonic nanoparticles,” Opt. Express19(2), 1648–1655 (2011).
[CrossRef] [PubMed]

G. X. Li, Z. L. Wang, S. M. Chen, and K. W. Cheah, “Narrowband plasmonic excitation on gold hole-array nanostructures observed using spectroscopic ellipsometer,” Opt. Express19(7), 6348–6353 (2011).
[CrossRef] [PubMed]

A. Ahmed and R. Gordon, “Directivity enhanced Raman spectroscopy using nanoantennas,” Nano Lett.11(4), 1800–1803 (2011).
[PubMed]

A. I. Maaroof, J. V. Nygaard, and D. S. Sutherland, “Plasmon hybridization in silver nanoislands as semishells arrays coupled to a thin metallic film,” Plasmonics6(2), 419–425 (2011).
[CrossRef]

T. Utikal, T. Zentgraf, T. Paul, C. Rockstuhl, F. Lederer, M. Lippitz, and H. Giessen, “Towards the origin of the nonlinear response in hybrid plasmonic systems,” Phys. Rev. Lett.106(13), 133901 (2011).
[CrossRef] [PubMed]

Y. Zhang, N. K. Grady, C. Ayala-Orozco, and N. J. Halas, “Three-dimensional nanostructures as highly efficient generators of second harmonic light,” Nano Lett.11(12), 5519–5523 (2011).
[CrossRef] [PubMed]

2010

M. Hu, A. Ghoshal, M. Marquez, and P. G. Kik, “Single particles spectroscopy study of metal-film-induced tuning of silver nanoparticle plasmon resonances,” J. Phys. Chem. C114(16), 7509–7514 (2010).
[CrossRef]

J. Butet, J. Duboisset, G. Bachelier, I. Russier-Antoine, E. Benichou, C. Jonin, and P.-F. Brevet, “Optical second harmonic generation of single metallic nanoparticles embedded in a homogeneous medium,” Nano Lett.10(5), 1717–1721 (2010).
[CrossRef] [PubMed]

2009

J. Jung, T. Søndergaard, and S. I. Bozhevolnyi, “Gap plasmon-polariton nanoresonators: Scattering enhancement and launching of surface plasmon polaritons,” Phys. Rev. B79(3), 035401–035409 (2009).
[CrossRef]

T. Xu, X. Jiao, and S. Blair, “Third-harmonic generation from arrays of sub-wavelength metal apertures,” Opt. Express17(26), 23582–23588 (2009).
[CrossRef] [PubMed]

A. K. Singh, D. Senapati, A. Neely, G. Kolawole, C. Hawker, and P. C. Ray, “Nonlinear optical properties of triangular silver nanomaterials,” Chem. Phys. Lett.481(1-3), 94–98 (2009).
[CrossRef]

J. E. Millstone, S. J. Hurst, G. S. Métraux, J. I. Cutler, and C. A. Mirkin, “Colloidal gold and silver triangular nanoprisms,” Small5(6), 646–664 (2009).
[CrossRef] [PubMed]

A. M. Funston, C. Novo, T. J. Davis, and P. Mulvaney, “Plasmon coupling of gold nanorods at short distances and in different geometries,” Nano Lett.9(4), 1651–1658 (2009).
[CrossRef] [PubMed]

2008

T. Søndergaard and S. I. Bozhevolnyi, “Strip and gap plasmon polariton optical resonators,” Phys. Status Solidi, B Basic Res.245(1), 9–19 (2008).
[CrossRef]

F. Eftekhari and R. Gordon, “Enhanced second harmonic generation form noncentrosymmetric nanohole arrayes in a gold film,” IEEE J. Sel. Top. Quantum Electron.14(6), 1552–1558 (2008).
[CrossRef]

S. Kim, J. Jin, Y.-J. Kim, I.-Y. Park, Y. Kim, and S.-W. Kim, “High-harmonic generation by resonant plasmon field enhancement,” Nature453(7196), 757–760 (2008).
[CrossRef] [PubMed]

2007

T. Xu, X. Jiao, G.-P. Zhang, and S. Blair, “Second-harmonic emission from sub-wavelength apertures: Effects of aperture symmetry and lattice arrangement,” Opt. Express15(21), 13894–13906 (2007).
[CrossRef] [PubMed]

B. K. Canfield, H. Husu, J. Laukkanen, B. Bai, M. Kuittinen, J. Turunen, and M. Kauranen, “Local field asymmetry drives second-harmonic generation in non-centrosymmetric nanodimers,” Nano Lett.7(5), 1251–1255 (2007).
[CrossRef] [PubMed]

F. Le, N. Z. Lwin, N. J. Halas, and P. Nordlander, “Plasmonic interactions between a metallic nanoshell and a thin metallic film,” Phys. Rev. B76(16), 165410 (2007).
[CrossRef]

F. Hao, P. Nordlander, M. T. Burnett, and S. A. Maier, “Enhanced tunability and linewidth sharpening of plasmon resonances in hybridized metallic ring/disk nanocavities,” Phys. Rev. B76(24), 245417 (2007).
[CrossRef]

A. Lesuffleur, L. K. S. Kumar, and R. Gordon, “Apex-enhanced second-harmonic generation by using double-hole arrays in a gold film,” Phys. Rev. B75(4), 045423–045427 (2007).
[CrossRef]

2006

M. Pelton, M. Liu, S. Park, N. F. Scherer, and P. Guyot-Sionnest, “Ultrafast resonant optical scattering from single gold nanoroes: Large nonlinearities and plasmon saturation,” Phys. Rev. B73(15), 155419 (2006).
[CrossRef]

A. Lesuffleur, L. K. S. Kumar, and R. Gordon, “Enhanced second harmonic generation from nanoscale double-hole arrays in a gold film,” Appl. Phys. Lett.88(26), 261104 (2006).
[CrossRef]

W. Fan, S. Zhang, N.-C. Panoiu, A. Abdenour, S. Krishna, R. M. Osgood, K. J. Malloy, and S. R. J. Brueck, “Second harmonic generation from a nanopatterned isotropic nonlinear material,” Nano Lett.6(5), 1027–1030 (2006).
[CrossRef]

H. T. Miyazaki and Y. Kurokawa, “Squeezing visible light waves into a 3-nm-thick and 55-nm-long plasmon cavity,” Phys. Rev. Lett.96(9), 097401 (2006).
[CrossRef] [PubMed]

2005

M. Lippitz, M. A. van Dijk, and M. Orrit, “Third-harmonic generation from single gold nanoparticles,” Nano Lett.5(4), 799–802 (2005).
[CrossRef] [PubMed]

R. Jin, J. E. Jureller, H. Y. Kim, and N. F. Scherer, “Correlating second harmonic optical responses of single Ag nanoparticles with morphology,” J. Am. Chem. Soc.127(36), 12482–12483 (2005).
[CrossRef] [PubMed]

P. Mühlschlegel, H.-J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science308(5728), 1607–1609 (2005).
[CrossRef] [PubMed]

P. J. Schuck, D. P. Fromm, A. Sundaramurthy, G. S. Kino, and W. E. Moerner, “Improving the mismatch between light and nanoscale objects with gold bowtie nanoantennas,” Phys. Rev. Lett.94(1), 017402–017405 (2005).
[CrossRef] [PubMed]

2004

P. Nordlander, C. Oubre, E. Prodan, K. Li, and M. I. Stockman, “Plasmon hybridization in nanoparticle dimers,” Nano Lett.4(5), 899–903 (2004).
[CrossRef]

P. Nordlander and E. Prodan, “Plasmon hybridization in nanoparticles near metallic surfaces,” Nano Lett.4(11), 2209–2213 (2004).
[CrossRef]

2003

E. Prodan, C. Radloff, N. J. Halas, and P. Nordlander, “A hybridization model for the plasmon response of complex nanostructures,” Science302(5644), 419–422 (2003).
[CrossRef] [PubMed]

W. L. Barnes, A. Dereux, and T. W. Ebbesen, “Surface plasmon subwavelength optics,” Nature424(6950), 824–830 (2003).
[CrossRef] [PubMed]

K.-H. Su, Q.-H. Wei, X. Zhang, J. J. Mock, D. R. Smith, and S. Schultz, “Interparticle coupling effects on plasmon resonances of nanogold particles,” Nano Lett.3(8), 1087–1090 (2003).
[CrossRef]

2001

R. Jin, Y. Cao, C. A. Mirkin, K. L. Kelly, G. C. Schatz, and J. G. Zheng, “Photoinduced conversion of silver nanospheres to nanoprisms,” Science294(5548), 1901–1903 (2001).
[CrossRef] [PubMed]

1972

P. B. Johnson and R. W. Christy, “Optical-constants of noble-metals,” Phys. Rev. B6(12), 4370–4379 (1972).
[CrossRef]

Abdenour, A.

W. Fan, S. Zhang, N.-C. Panoiu, A. Abdenour, S. Krishna, R. M. Osgood, K. J. Malloy, and S. R. J. Brueck, “Second harmonic generation from a nanopatterned isotropic nonlinear material,” Nano Lett.6(5), 1027–1030 (2006).
[CrossRef]

Acimovic, S. S.

G. Volpe, M. Noack, S. S. Aćimović, C. Reinhardt, and R. Quidant, “Near-field mapping of plasmonic antennas by multiphoton absorption in poly(methyl methacrylate),” Nano Lett.12(9), 4864–4868 (2012).
[CrossRef] [PubMed]

Ahmed, A.

A. Ahmed and R. Gordon, “Directivity enhanced Raman spectroscopy using nanoantennas,” Nano Lett.11(4), 1800–1803 (2011).
[PubMed]

Aouani, H.

H. Aouani, M. Navarro-Cia, M. Rahmani, T. P. H. Sidiropoulos, M. Hong, R. F. Oulton, and S. A. Maier, “Multiresonant broadband optical antennas as efficient tunable nanosources of second harmonic light,” Nano Lett.12(9), 4997–5002 (2012).
[CrossRef] [PubMed]

Appavoo, K.

D. Y. Lei, A. I. Fernández-Domínguez, Y. Sonnefraud, K. Appavoo, R. F. Haglund, J. B. Pendry, and S. A. Maier, “Revealing plasmonic gap modes in particle-on-film systems using dark-field spectroscopy,” ACS Nano6(2), 1380–1386 (2012).
[CrossRef] [PubMed]

Ayala-Orozco, C.

Y. Zhang, N. K. Grady, C. Ayala-Orozco, and N. J. Halas, “Three-dimensional nanostructures as highly efficient generators of second harmonic light,” Nano Lett.11(12), 5519–5523 (2011).
[CrossRef] [PubMed]

Bachelier, G.

J. Butet, J. Duboisset, G. Bachelier, I. Russier-Antoine, E. Benichou, C. Jonin, and P.-F. Brevet, “Optical second harmonic generation of single metallic nanoparticles embedded in a homogeneous medium,” Nano Lett.10(5), 1717–1721 (2010).
[CrossRef] [PubMed]

Bai, B.

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M. Hentschel, T. Utikal, H. Giessen, and M. Lippitz, “Quantitative modeling of the third harmonic emission spectrum of plasmonic nanoantennas,” Nano Lett.12(7), 3778–3782 (2012).
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T. Hanke, J. Cesar, V. Knittel, A. Trügler, U. Hohenester, A. Leitenstorfer, and R. Bratschitsch, “Tailoring spatiotemporal light confinement in single plasmonic nanoantennas,” Nano Lett.12(2), 992–996 (2012).
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J. E. Millstone, S. J. Hurst, G. S. Métraux, J. I. Cutler, and C. A. Mirkin, “Colloidal gold and silver triangular nanoprisms,” Small5(6), 646–664 (2009).
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B. K. Canfield, H. Husu, J. Laukkanen, B. Bai, M. Kuittinen, J. Turunen, and M. Kauranen, “Local field asymmetry drives second-harmonic generation in non-centrosymmetric nanodimers,” Nano Lett.7(5), 1251–1255 (2007).
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J. Butet, I. Russier-Antoine, C. Jonin, N. Lascoux, E. Benichou, and P.-F. Brevet, “Sensing with multipolar second harmonic generation from spherical metallic nanoparticles,” Nano Lett.12(3), 1697–1701 (2012).
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J. Butet, J. Duboisset, G. Bachelier, I. Russier-Antoine, E. Benichou, C. Jonin, and P.-F. Brevet, “Optical second harmonic generation of single metallic nanoparticles embedded in a homogeneous medium,” Nano Lett.10(5), 1717–1721 (2010).
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J. Jung, T. Søndergaard, and S. I. Bozhevolnyi, “Gap plasmon-polariton nanoresonators: Scattering enhancement and launching of surface plasmon polaritons,” Phys. Rev. B79(3), 035401–035409 (2009).
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R. Jin, J. E. Jureller, H. Y. Kim, and N. F. Scherer, “Correlating second harmonic optical responses of single Ag nanoparticles with morphology,” J. Am. Chem. Soc.127(36), 12482–12483 (2005).
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B. K. Canfield, H. Husu, J. Laukkanen, B. Bai, M. Kuittinen, J. Turunen, and M. Kauranen, “Local field asymmetry drives second-harmonic generation in non-centrosymmetric nanodimers,” Nano Lett.7(5), 1251–1255 (2007).
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M. Hu, A. Ghoshal, M. Marquez, and P. G. Kik, “Single particles spectroscopy study of metal-film-induced tuning of silver nanoparticle plasmon resonances,” J. Phys. Chem. C114(16), 7509–7514 (2010).
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R. Jin, J. E. Jureller, H. Y. Kim, and N. F. Scherer, “Correlating second harmonic optical responses of single Ag nanoparticles with morphology,” J. Am. Chem. Soc.127(36), 12482–12483 (2005).
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S. Kim, J. Jin, Y.-J. Kim, I.-Y. Park, Y. Kim, and S.-W. Kim, “High-harmonic generation by resonant plasmon field enhancement,” Nature453(7196), 757–760 (2008).
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S. Kim, J. Jin, Y.-J. Kim, I.-Y. Park, Y. Kim, and S.-W. Kim, “High-harmonic generation by resonant plasmon field enhancement,” Nature453(7196), 757–760 (2008).
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S. Kim, J. Jin, Y.-J. Kim, I.-Y. Park, Y. Kim, and S.-W. Kim, “High-harmonic generation by resonant plasmon field enhancement,” Nature453(7196), 757–760 (2008).
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S. Kim, J. Jin, Y.-J. Kim, I.-Y. Park, Y. Kim, and S.-W. Kim, “High-harmonic generation by resonant plasmon field enhancement,” Nature453(7196), 757–760 (2008).
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P. J. Schuck, D. P. Fromm, A. Sundaramurthy, G. S. Kino, and W. E. Moerner, “Improving the mismatch between light and nanoscale objects with gold bowtie nanoantennas,” Phys. Rev. Lett.94(1), 017402–017405 (2005).
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T. Hanke, J. Cesar, V. Knittel, A. Trügler, U. Hohenester, A. Leitenstorfer, and R. Bratschitsch, “Tailoring spatiotemporal light confinement in single plasmonic nanoantennas,” Nano Lett.12(2), 992–996 (2012).
[CrossRef] [PubMed]

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A. K. Singh, D. Senapati, A. Neely, G. Kolawole, C. Hawker, and P. C. Ray, “Nonlinear optical properties of triangular silver nanomaterials,” Chem. Phys. Lett.481(1-3), 94–98 (2009).
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W. Fan, S. Zhang, N.-C. Panoiu, A. Abdenour, S. Krishna, R. M. Osgood, K. J. Malloy, and S. R. J. Brueck, “Second harmonic generation from a nanopatterned isotropic nonlinear material,” Nano Lett.6(5), 1027–1030 (2006).
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B. K. Canfield, H. Husu, J. Laukkanen, B. Bai, M. Kuittinen, J. Turunen, and M. Kauranen, “Local field asymmetry drives second-harmonic generation in non-centrosymmetric nanodimers,” Nano Lett.7(5), 1251–1255 (2007).
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Kumar, L. K. S.

A. Lesuffleur, L. K. S. Kumar, and R. Gordon, “Apex-enhanced second-harmonic generation by using double-hole arrays in a gold film,” Phys. Rev. B75(4), 045423–045427 (2007).
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A. Lesuffleur, L. K. S. Kumar, and R. Gordon, “Enhanced second harmonic generation from nanoscale double-hole arrays in a gold film,” Appl. Phys. Lett.88(26), 261104 (2006).
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B. K. Canfield, H. Husu, J. Laukkanen, B. Bai, M. Kuittinen, J. Turunen, and M. Kauranen, “Local field asymmetry drives second-harmonic generation in non-centrosymmetric nanodimers,” Nano Lett.7(5), 1251–1255 (2007).
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F. Le, N. Z. Lwin, N. J. Halas, and P. Nordlander, “Plasmonic interactions between a metallic nanoshell and a thin metallic film,” Phys. Rev. B76(16), 165410 (2007).
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T. Utikal, T. Zentgraf, T. Paul, C. Rockstuhl, F. Lederer, M. Lippitz, and H. Giessen, “Towards the origin of the nonlinear response in hybrid plasmonic systems,” Phys. Rev. Lett.106(13), 133901 (2011).
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D. Y. Lei, A. I. Fernández-Domínguez, Y. Sonnefraud, K. Appavoo, R. F. Haglund, J. B. Pendry, and S. A. Maier, “Revealing plasmonic gap modes in particle-on-film systems using dark-field spectroscopy,” ACS Nano6(2), 1380–1386 (2012).
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T. Hanke, J. Cesar, V. Knittel, A. Trügler, U. Hohenester, A. Leitenstorfer, and R. Bratschitsch, “Tailoring spatiotemporal light confinement in single plasmonic nanoantennas,” Nano Lett.12(2), 992–996 (2012).
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A. Lesuffleur, L. K. S. Kumar, and R. Gordon, “Apex-enhanced second-harmonic generation by using double-hole arrays in a gold film,” Phys. Rev. B75(4), 045423–045427 (2007).
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A. Lesuffleur, L. K. S. Kumar, and R. Gordon, “Enhanced second harmonic generation from nanoscale double-hole arrays in a gold film,” Appl. Phys. Lett.88(26), 261104 (2006).
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M. Hentschel, T. Utikal, H. Giessen, and M. Lippitz, “Quantitative modeling of the third harmonic emission spectrum of plasmonic nanoantennas,” Nano Lett.12(7), 3778–3782 (2012).
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H. Aouani, M. Navarro-Cia, M. Rahmani, T. P. H. Sidiropoulos, M. Hong, R. F. Oulton, and S. A. Maier, “Multiresonant broadband optical antennas as efficient tunable nanosources of second harmonic light,” Nano Lett.12(9), 4997–5002 (2012).
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J. J. Mock, R. T. Hill, Y.-J. Tsai, A. Chilkoti, and D. R. Smith, “Probing dynamically tunable localized surface plasmon resonances of film-coupled nanoparticles by evanescent wave excitation,” Nano Lett.12(4), 1757–1764 (2012).
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C. Ciracì, R. T. Hill, J. J. Mock, Y. Urzhumov, A. I. Fernández-Domínguez, S. A. Maier, J. B. Pendry, A. Chilkoti, and D. R. Smith, “Probing the ultimate limits of plasmonic enhancement,” Science337(6098), 1072–1074 (2012).
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A. K. Singh, D. Senapati, A. Neely, G. Kolawole, C. Hawker, and P. C. Ray, “Nonlinear optical properties of triangular silver nanomaterials,” Chem. Phys. Lett.481(1-3), 94–98 (2009).
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P. Nordlander and E. Prodan, “Plasmon hybridization in nanoparticles near metallic surfaces,” Nano Lett.4(11), 2209–2213 (2004).
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P. Nordlander, C. Oubre, E. Prodan, K. Li, and M. I. Stockman, “Plasmon hybridization in nanoparticle dimers,” Nano Lett.4(5), 899–903 (2004).
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P. Nordlander, C. Oubre, E. Prodan, K. Li, and M. I. Stockman, “Plasmon hybridization in nanoparticle dimers,” Nano Lett.4(5), 899–903 (2004).
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H. Aouani, M. Navarro-Cia, M. Rahmani, T. P. H. Sidiropoulos, M. Hong, R. F. Oulton, and S. A. Maier, “Multiresonant broadband optical antennas as efficient tunable nanosources of second harmonic light,” Nano Lett.12(9), 4997–5002 (2012).
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T. Utikal, T. Zentgraf, T. Paul, C. Rockstuhl, F. Lederer, M. Lippitz, and H. Giessen, “Towards the origin of the nonlinear response in hybrid plasmonic systems,” Phys. Rev. Lett.106(13), 133901 (2011).
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M. Pelton, M. Liu, S. Park, N. F. Scherer, and P. Guyot-Sionnest, “Ultrafast resonant optical scattering from single gold nanoroes: Large nonlinearities and plasmon saturation,” Phys. Rev. B73(15), 155419 (2006).
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[CrossRef] [PubMed]

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P. Mühlschlegel, H.-J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, “Resonant optical antennas,” Science308(5728), 1607–1609 (2005).
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P. Nordlander and E. Prodan, “Plasmon hybridization in nanoparticles near metallic surfaces,” Nano Lett.4(11), 2209–2213 (2004).
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P. Nordlander, C. Oubre, E. Prodan, K. Li, and M. I. Stockman, “Plasmon hybridization in nanoparticle dimers,” Nano Lett.4(5), 899–903 (2004).
[CrossRef]

E. Prodan, C. Radloff, N. J. Halas, and P. Nordlander, “A hybridization model for the plasmon response of complex nanostructures,” Science302(5644), 419–422 (2003).
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G. Volpe, M. Noack, S. S. Aćimović, C. Reinhardt, and R. Quidant, “Near-field mapping of plasmonic antennas by multiphoton absorption in poly(methyl methacrylate),” Nano Lett.12(9), 4864–4868 (2012).
[CrossRef] [PubMed]

H. Harutyunyan, G. Volpe, R. Quidant, and L. Novotny, “Enhancing the nonlinear optical response using multifrequency gold-nanowire antennas,” Phys. Rev. Lett.108(21), 217403 (2012).
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E. Prodan, C. Radloff, N. J. Halas, and P. Nordlander, “A hybridization model for the plasmon response of complex nanostructures,” Science302(5644), 419–422 (2003).
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H. Aouani, M. Navarro-Cia, M. Rahmani, T. P. H. Sidiropoulos, M. Hong, R. F. Oulton, and S. A. Maier, “Multiresonant broadband optical antennas as efficient tunable nanosources of second harmonic light,” Nano Lett.12(9), 4997–5002 (2012).
[CrossRef] [PubMed]

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A. K. Singh, D. Senapati, A. Neely, G. Kolawole, C. Hawker, and P. C. Ray, “Nonlinear optical properties of triangular silver nanomaterials,” Chem. Phys. Lett.481(1-3), 94–98 (2009).
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G. Volpe, M. Noack, S. S. Aćimović, C. Reinhardt, and R. Quidant, “Near-field mapping of plasmonic antennas by multiphoton absorption in poly(methyl methacrylate),” Nano Lett.12(9), 4864–4868 (2012).
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M. Pelton, M. Liu, S. Park, N. F. Scherer, and P. Guyot-Sionnest, “Ultrafast resonant optical scattering from single gold nanoroes: Large nonlinearities and plasmon saturation,” Phys. Rev. B73(15), 155419 (2006).
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K.-H. Su, Q.-H. Wei, X. Zhang, J. J. Mock, D. R. Smith, and S. Schultz, “Interparticle coupling effects on plasmon resonances of nanogold particles,” Nano Lett.3(8), 1087–1090 (2003).
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A. K. Singh, D. Senapati, A. Neely, G. Kolawole, C. Hawker, and P. C. Ray, “Nonlinear optical properties of triangular silver nanomaterials,” Chem. Phys. Lett.481(1-3), 94–98 (2009).
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H. Aouani, M. Navarro-Cia, M. Rahmani, T. P. H. Sidiropoulos, M. Hong, R. F. Oulton, and S. A. Maier, “Multiresonant broadband optical antennas as efficient tunable nanosources of second harmonic light,” Nano Lett.12(9), 4997–5002 (2012).
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Stockman, M. I.

P. Nordlander, C. Oubre, E. Prodan, K. Li, and M. I. Stockman, “Plasmon hybridization in nanoparticle dimers,” Nano Lett.4(5), 899–903 (2004).
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K.-H. Su, Q.-H. Wei, X. Zhang, J. J. Mock, D. R. Smith, and S. Schultz, “Interparticle coupling effects on plasmon resonances of nanogold particles,” Nano Lett.3(8), 1087–1090 (2003).
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A. I. Maaroof, J. V. Nygaard, and D. S. Sutherland, “Plasmon hybridization in silver nanoislands as semishells arrays coupled to a thin metallic film,” Plasmonics6(2), 419–425 (2011).
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C. Lumdee, S. Toroghi, and P. G. Kik, “Post-fabrication voltage controlled resonance tuning of nanoscale plasmonic antennas,” ACS Nano6(7), 6301–6307 (2012).
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M. Hentschel, T. Utikal, H. Giessen, and M. Lippitz, “Quantitative modeling of the third harmonic emission spectrum of plasmonic nanoantennas,” Nano Lett.12(7), 3778–3782 (2012).
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M. Lippitz, M. A. van Dijk, and M. Orrit, “Third-harmonic generation from single gold nanoparticles,” Nano Lett.5(4), 799–802 (2005).
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H. Harutyunyan, G. Volpe, R. Quidant, and L. Novotny, “Enhancing the nonlinear optical response using multifrequency gold-nanowire antennas,” Phys. Rev. Lett.108(21), 217403 (2012).
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Figures (5)

Fig. 1
Fig. 1

(a) Extinction of silver nanoparticles in aqueous solution as a function of irradiation time. Inset: Scanning electron microscope image of a typical silver nanoprism after 72 h irradiation. (b,c) Atomic force microscope (AFM) characterization of silver nanoprisms spin coated on a silicon substrate. (d) The height of a typical silver nanoprism was measured to be 12 nm with the AFM.

Fig. 2
Fig. 2

(a) Schematic of silver nanoprisms with PMMA spacer layer over a 10 nm thick Au film adhered to a glass substrate with a 2 nm Ti layer. (b) Schematic of scattering measurement setup. WLS = white light source, obj = microscope objective lens. (c) Scattering measurement for three hybrid structures with different PMMA spacer layer thicknesses (shown in legend). Green dotted line: Ti:Sapphire spectrum. (d) Scattering simulation results for silver nanoprisms for the corresponding spacer thicknesses.

Fig. 3
Fig. 3

Peak scattering wavelength as a function of PMMA spacer layer thickness from experiment and FDTD simulations.

Fig. 4
Fig. 4

(a) Schematic of SHG measurement setup. ND = neutral density filter, obj = microscope objective lens, BG40 = blue-green band pass filter. (b) SHG measured using spectrum analyzer in front of streak camera (not shown in (a)). (c) SHG count dependence on PMMA spacer layer thicknesses. (d) Log-log plot of SHG count vs. incident laser power with linear-fit slope of 2.17 ± 0.20. For SHG, a slope of 2 is expected.

Fig. 5
Fig. 5

Near field map of the electric field intensity, (a,b) for a silver nanoprism on 10 nm PMMA, 10 nm Au, 2 nm Ti, glass substrate, at the source wavelength of 808 nm in (a) xy and (b) xz planes. (c,d) shows the same distribution for a silver nanoprism on glass substrate, at the source wavelength of 808 nm in (c) xy and (d) xz planes. The scale bar is logarithmic (base 10).

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