Abstract

We have compared the plasmonic enhancement of second-order nonlinear optical (NLO) properties in two types of ionic self-assembled multilayer (ISAM) films combined with Ag nanoparticles fabricated using nanosphere lithography (NSL). The light-concentrating properties of the Ag particles lead to a marked increase in the NLO efficiencies of thin ISAM films. The induced enhancement is found to be much larger in conventional ISAM films than in films made with the hybrid covalent ISAM technique (HCISAM), even though the latter have a significantly larger intrinsic bulk second-order nonlinear susceptibility (χ(2)). The plasmonic enhancement of NLO effects is shown to be primarily an interface effect due to the short decay length of the plasmon modes. The importance of interface effects in the films has been investigated by surrounding thin ISAM and HCISAM films with NLO-inactive buffer layers, which confirmed the important role played by the interfaces, particularly for the HCISAM films.

© 2009 Optical Society of America

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2009 (1)

M. Ishifuji, M. Mitsuishi, and T. Miyashita, “Bottom-up design of hybrid polymer nanoassemblies elucidates plasmon-enhanced second-harmonic generation from nonlinear optical dyes,” J. Am. Chem. Soc. 131, 4418-4424 (2009).
[CrossRef] [PubMed]

2008 (1)

A. Garg, R. M. Davis, C. Durak, J. R. Heflin, and H. W. Gibson, “Polar orientation of a pendant anionic chromophore in thick layer-by-layer self-assembled polymeric films,” J. Appl. Phys. 104, 053116 (2008).
[CrossRef]

2007 (1)

K. Chen, C. Durak, J. R. Heflin, and H. D. Robinson, “Plasmon-enhanced second-harmonic generation from ionic self-assembled multilayer films,” Nano Lett. 7, 254-258 (2007).
[CrossRef] [PubMed]

2006 (4)

J. R. Heflin, M. T. Guzy, P. J. Neyman, K. J. Gaskins, C. Brands, Z. Wang, H. W. Gibson, R. M. Davis, and K. E. Van Cott, “Efficient, thermally stable, second-order nonlinear optical response in organic hybrid covalent/ionic self-assembled films,” Langmuir 22, 5723-5727 (2006).
[CrossRef] [PubMed]

K. Tsuboi, S. Abe, S. Fukuba, M. Shimojo, M. Tanaka, K. Furuya, K. Fujita, and K. Kajikawa, “Second-harmonic spectroscopy of surface immobilized gold nanospheres above a gold surface supported by self-assembled monolayers,” J. Phys. Chem. B 125, 174703 (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, 1027-1030 (2006).
[CrossRef]

M. C. Tong, W. Chen, J. Sun, D. Ghosh, and S. W. Chen, “Dithiocarbamate-capped silver nanoparticles,” J. Phys. B 110, 19238-19242 (2006).

2005 (2)

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

Y. Zhao, W. Perez-Segarra, Q. C. Shi, and A. Wei, “Dithiocarbamate assembly on gold,” J. Am. Chem. Soc. 127, 7328-7329 (2005).
[CrossRef] [PubMed]

2004 (2)

B. G. Prevo and O. D. Velev, “Controlled, rapid deposition of structured coatings from micro- and nanoparticle suspensions,” Langmuir 20, 2099-2107 (2004).
[CrossRef]

E. Hao and G. C. Schatz, “Electromagnetic fields around silver nanoparticles and dimers,” J. Phys. Chem. 120, 357-366 (2004).
[CrossRef]

2003 (2)

D. Yelin, D. Oron, S. Thiberge, E. Moses, and Y. Silberberg, “Multiphoton plasmon-resonance microscopy,” Opt. Express 11, 1385-1391 (2003).
[CrossRef] [PubMed]

D. A. Genov, A. K. Sarychev, V. M. Shalaev, and A. Wei, “Resonant field enhancements from metal nanoparticle arrays,” Nano Lett. 4, 153-158 (2003).
[CrossRef]

2002 (3)

A. J. Haes and R. P. Van Duyne, “A nanoscale optical blosensor: sensitivity and selectivity of an approach based on the localized surface plasmon resonance spectroscopy of triangular silver nanoparticles,” J. Am. Chem. Soc. 124, 10596-10604 (2002).
[CrossRef] [PubMed]

W. E. Doering and S. M. Nie, “Single-molecule and single-nanoparticle SERS: examining the roles of surface active sites and chemical enhancement,” J. Phys. B 106, 311-317 (2002).

K. E. Van Cott, M. T. Guzy, P. J. Neyman, C. Brands, J. R. Heflin, H. W. Gibson, and R. M. Davis, “Layer-by-layer deposition and ordering of low-molecular-weight dye molecules for second-order nonlinear optics,” Angew. Chem., Int. Ed. Engl. 41, 3236-3238 (2002).
[CrossRef]

2001 (1)

C. L. Haynes and R. P. Van Duyne, “Nanosphere lithography: a versatile nanofabrication tool for studies of size-dependent nanoparticle optics,” J. Phys. Chem. B 105, 5599-5611 (2001).
[CrossRef]

2000 (3)

T. R. Jensen, M. D. Malinsky, C. L. Haynes, and R. P. Van Duyne, “Nanosphere lithography: tunable localized surface plasmon resonance spectra of silver nanoparticles,” J. Phys. Chem. B 104, 10549-10556 (2000).
[CrossRef]

H. A. Clark, P. J. Campagnola, J. P. Wuskell, A. Lewis, and L. M. Loew, “Second-harmonic generation properties of fluorescent polymer-encapsulated gold nanoparticles,” J. Am. Chem. Soc. 122, 10234-10235 (2000).
[CrossRef]

A. C. Templeton, M. P. Wuelfing, and R. W. Murray, “Monolayer protected cluster molecules,” Acc. Chem. Res. 33, 27-36 (2000).
[CrossRef] [PubMed]

1999 (1)

J. R. Heflin, C. Figura, D. Marciu, Y. Liu, and R. O. Claus, “Thickness dependence of second-harmonic generation in thin films fabricated from ionically self-assembled monolayers,” Appl. Phys. Lett. 74, 495-497 (1999).
[CrossRef]

1998 (1)

A. Campion and P. Kambhampati, “Surface-enhanced Raman scattering,” Chem. Soc. Rev. 27, 241-250 (1998).
[CrossRef]

1997 (3)

G. Decher, “Fuzzy nanoassemblies: toward layered polymeric multicomposites,” Science 277, 1232-1237 (1997).
[CrossRef]

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. Dasari, and M. S. Feld, “Single molecule detection using surface-enhanced Raman scattering (SERS),” Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

S. Nie and S. R. Emory, “Probing single molecules and single nanoparticles by surface-enhanced Raman scattering,” Science 275, 1102-1106 (1997).
[CrossRef] [PubMed]

1996 (1)

1989 (1)

C. D. Bain, E. B. Troughton, Y. T. Tao, J. Evall, G. M. Whitesides, and R. G. Nuzzo, “Formation of monolayer films by the spontaneous assembly of organic thiols from solution onto gold,” J. Am. Chem. Soc. 111, 321-335 (1989).
[CrossRef]

1984 (1)

W. Kern, “Purifying Si and SiO2 surfaces with hydrogen peroxide,” Semicond. Int. 7, 94-99 (1984).

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, 1027-1030 (2006).
[CrossRef]

Abe, S.

K. Tsuboi, S. Abe, S. Fukuba, M. Shimojo, M. Tanaka, K. Furuya, K. Fujita, and K. Kajikawa, “Second-harmonic spectroscopy of surface immobilized gold nanospheres above a gold surface supported by self-assembled monolayers,” J. Phys. Chem. B 125, 174703 (2006).
[CrossRef]

Bain, C. D.

C. D. Bain, E. B. Troughton, Y. T. Tao, J. Evall, G. M. Whitesides, and R. G. Nuzzo, “Formation of monolayer films by the spontaneous assembly of organic thiols from solution onto gold,” J. Am. Chem. Soc. 111, 321-335 (1989).
[CrossRef]

Brands, C.

J. R. Heflin, M. T. Guzy, P. J. Neyman, K. J. Gaskins, C. Brands, Z. Wang, H. W. Gibson, R. M. Davis, and K. E. Van Cott, “Efficient, thermally stable, second-order nonlinear optical response in organic hybrid covalent/ionic self-assembled films,” Langmuir 22, 5723-5727 (2006).
[CrossRef] [PubMed]

K. E. Van Cott, M. T. Guzy, P. J. Neyman, C. Brands, J. R. Heflin, H. W. Gibson, and R. M. Davis, “Layer-by-layer deposition and ordering of low-molecular-weight dye molecules for second-order nonlinear optics,” Angew. Chem., Int. Ed. Engl. 41, 3236-3238 (2002).
[CrossRef]

Brueck, S. R. J.

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, 1027-1030 (2006).
[CrossRef]

Campagnola, P. J.

H. A. Clark, P. J. Campagnola, J. P. Wuskell, A. Lewis, and L. M. Loew, “Second-harmonic generation properties of fluorescent polymer-encapsulated gold nanoparticles,” J. Am. Chem. Soc. 122, 10234-10235 (2000).
[CrossRef]

Campion, A.

A. Campion and P. Kambhampati, “Surface-enhanced Raman scattering,” Chem. Soc. Rev. 27, 241-250 (1998).
[CrossRef]

Chen, K.

K. Chen, C. Durak, J. R. Heflin, and H. D. Robinson, “Plasmon-enhanced second-harmonic generation from ionic self-assembled multilayer films,” Nano Lett. 7, 254-258 (2007).
[CrossRef] [PubMed]

Chen, S. W.

M. C. Tong, W. Chen, J. Sun, D. Ghosh, and S. W. Chen, “Dithiocarbamate-capped silver nanoparticles,” J. Phys. B 110, 19238-19242 (2006).

Chen, W.

M. C. Tong, W. Chen, J. Sun, D. Ghosh, and S. W. Chen, “Dithiocarbamate-capped silver nanoparticles,” J. Phys. B 110, 19238-19242 (2006).

Clark, H. A.

H. A. Clark, P. J. Campagnola, J. P. Wuskell, A. Lewis, and L. M. Loew, “Second-harmonic generation properties of fluorescent polymer-encapsulated gold nanoparticles,” J. Am. Chem. Soc. 122, 10234-10235 (2000).
[CrossRef]

Claus, R. O.

J. R. Heflin, C. Figura, D. Marciu, Y. Liu, and R. O. Claus, “Thickness dependence of second-harmonic generation in thin films fabricated from ionically self-assembled monolayers,” Appl. Phys. Lett. 74, 495-497 (1999).
[CrossRef]

Dasari, R.

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. Dasari, and M. S. Feld, “Single molecule detection using surface-enhanced Raman scattering (SERS),” Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

Davis, R. M.

A. Garg, R. M. Davis, C. Durak, J. R. Heflin, and H. W. Gibson, “Polar orientation of a pendant anionic chromophore in thick layer-by-layer self-assembled polymeric films,” J. Appl. Phys. 104, 053116 (2008).
[CrossRef]

J. R. Heflin, M. T. Guzy, P. J. Neyman, K. J. Gaskins, C. Brands, Z. Wang, H. W. Gibson, R. M. Davis, and K. E. Van Cott, “Efficient, thermally stable, second-order nonlinear optical response in organic hybrid covalent/ionic self-assembled films,” Langmuir 22, 5723-5727 (2006).
[CrossRef] [PubMed]

K. E. Van Cott, M. T. Guzy, P. J. Neyman, C. Brands, J. R. Heflin, H. W. Gibson, and R. M. Davis, “Layer-by-layer deposition and ordering of low-molecular-weight dye molecules for second-order nonlinear optics,” Angew. Chem., Int. Ed. Engl. 41, 3236-3238 (2002).
[CrossRef]

Decher, G.

G. Decher, “Fuzzy nanoassemblies: toward layered polymeric multicomposites,” Science 277, 1232-1237 (1997).
[CrossRef]

Doering, W. E.

W. E. Doering and S. M. Nie, “Single-molecule and single-nanoparticle SERS: examining the roles of surface active sites and chemical enhancement,” J. Phys. B 106, 311-317 (2002).

Durak, C.

A. Garg, R. M. Davis, C. Durak, J. R. Heflin, and H. W. Gibson, “Polar orientation of a pendant anionic chromophore in thick layer-by-layer self-assembled polymeric films,” J. Appl. Phys. 104, 053116 (2008).
[CrossRef]

K. Chen, C. Durak, J. R. Heflin, and H. D. Robinson, “Plasmon-enhanced second-harmonic generation from ionic self-assembled multilayer films,” Nano Lett. 7, 254-258 (2007).
[CrossRef] [PubMed]

Emory, S. R.

S. Nie and S. R. Emory, “Probing single molecules and single nanoparticles by surface-enhanced Raman scattering,” Science 275, 1102-1106 (1997).
[CrossRef] [PubMed]

Evall, J.

C. D. Bain, E. B. Troughton, Y. T. Tao, J. Evall, G. M. Whitesides, and R. G. Nuzzo, “Formation of monolayer films by the spontaneous assembly of organic thiols from solution onto gold,” J. Am. Chem. Soc. 111, 321-335 (1989).
[CrossRef]

Fan, W.

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, 1027-1030 (2006).
[CrossRef]

Feld, M. S.

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. Dasari, and M. S. Feld, “Single molecule detection using surface-enhanced Raman scattering (SERS),” Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

Figura, C.

J. R. Heflin, C. Figura, D. Marciu, Y. Liu, and R. O. Claus, “Thickness dependence of second-harmonic generation in thin films fabricated from ionically self-assembled monolayers,” Appl. Phys. Lett. 74, 495-497 (1999).
[CrossRef]

Fujita, K.

K. Tsuboi, S. Abe, S. Fukuba, M. Shimojo, M. Tanaka, K. Furuya, K. Fujita, and K. Kajikawa, “Second-harmonic spectroscopy of surface immobilized gold nanospheres above a gold surface supported by self-assembled monolayers,” J. Phys. Chem. B 125, 174703 (2006).
[CrossRef]

Fukuba, S.

K. Tsuboi, S. Abe, S. Fukuba, M. Shimojo, M. Tanaka, K. Furuya, K. Fujita, and K. Kajikawa, “Second-harmonic spectroscopy of surface immobilized gold nanospheres above a gold surface supported by self-assembled monolayers,” J. Phys. Chem. B 125, 174703 (2006).
[CrossRef]

Furuya, K.

K. Tsuboi, S. Abe, S. Fukuba, M. Shimojo, M. Tanaka, K. Furuya, K. Fujita, and K. Kajikawa, “Second-harmonic spectroscopy of surface immobilized gold nanospheres above a gold surface supported by self-assembled monolayers,” J. Phys. Chem. B 125, 174703 (2006).
[CrossRef]

Garg, A.

A. Garg, R. M. Davis, C. Durak, J. R. Heflin, and H. W. Gibson, “Polar orientation of a pendant anionic chromophore in thick layer-by-layer self-assembled polymeric films,” J. Appl. Phys. 104, 053116 (2008).
[CrossRef]

Gaskins, K. J.

J. R. Heflin, M. T. Guzy, P. J. Neyman, K. J. Gaskins, C. Brands, Z. Wang, H. W. Gibson, R. M. Davis, and K. E. Van Cott, “Efficient, thermally stable, second-order nonlinear optical response in organic hybrid covalent/ionic self-assembled films,” Langmuir 22, 5723-5727 (2006).
[CrossRef] [PubMed]

Genov, D. A.

D. A. Genov, A. K. Sarychev, V. M. Shalaev, and A. Wei, “Resonant field enhancements from metal nanoparticle arrays,” Nano Lett. 4, 153-158 (2003).
[CrossRef]

Ghosh, D.

M. C. Tong, W. Chen, J. Sun, D. Ghosh, and S. W. Chen, “Dithiocarbamate-capped silver nanoparticles,” J. Phys. B 110, 19238-19242 (2006).

Gibson, H. W.

A. Garg, R. M. Davis, C. Durak, J. R. Heflin, and H. W. Gibson, “Polar orientation of a pendant anionic chromophore in thick layer-by-layer self-assembled polymeric films,” J. Appl. Phys. 104, 053116 (2008).
[CrossRef]

J. R. Heflin, M. T. Guzy, P. J. Neyman, K. J. Gaskins, C. Brands, Z. Wang, H. W. Gibson, R. M. Davis, and K. E. Van Cott, “Efficient, thermally stable, second-order nonlinear optical response in organic hybrid covalent/ionic self-assembled films,” Langmuir 22, 5723-5727 (2006).
[CrossRef] [PubMed]

K. E. Van Cott, M. T. Guzy, P. J. Neyman, C. Brands, J. R. Heflin, H. W. Gibson, and R. M. Davis, “Layer-by-layer deposition and ordering of low-molecular-weight dye molecules for second-order nonlinear optics,” Angew. Chem., Int. Ed. Engl. 41, 3236-3238 (2002).
[CrossRef]

Guzy, M. T.

J. R. Heflin, M. T. Guzy, P. J. Neyman, K. J. Gaskins, C. Brands, Z. Wang, H. W. Gibson, R. M. Davis, and K. E. Van Cott, “Efficient, thermally stable, second-order nonlinear optical response in organic hybrid covalent/ionic self-assembled films,” Langmuir 22, 5723-5727 (2006).
[CrossRef] [PubMed]

K. E. Van Cott, M. T. Guzy, P. J. Neyman, C. Brands, J. R. Heflin, H. W. Gibson, and R. M. Davis, “Layer-by-layer deposition and ordering of low-molecular-weight dye molecules for second-order nonlinear optics,” Angew. Chem., Int. Ed. Engl. 41, 3236-3238 (2002).
[CrossRef]

Haes, A. J.

A. J. Haes and R. P. Van Duyne, “A nanoscale optical blosensor: sensitivity and selectivity of an approach based on the localized surface plasmon resonance spectroscopy of triangular silver nanoparticles,” J. Am. Chem. Soc. 124, 10596-10604 (2002).
[CrossRef] [PubMed]

Hao, E.

E. Hao and G. C. Schatz, “Electromagnetic fields around silver nanoparticles and dimers,” J. Phys. Chem. 120, 357-366 (2004).
[CrossRef]

Haynes, C. L.

C. L. Haynes and R. P. Van Duyne, “Nanosphere lithography: a versatile nanofabrication tool for studies of size-dependent nanoparticle optics,” J. Phys. Chem. B 105, 5599-5611 (2001).
[CrossRef]

T. R. Jensen, M. D. Malinsky, C. L. Haynes, and R. P. Van Duyne, “Nanosphere lithography: tunable localized surface plasmon resonance spectra of silver nanoparticles,” J. Phys. Chem. B 104, 10549-10556 (2000).
[CrossRef]

Heflin, J. R.

A. Garg, R. M. Davis, C. Durak, J. R. Heflin, and H. W. Gibson, “Polar orientation of a pendant anionic chromophore in thick layer-by-layer self-assembled polymeric films,” J. Appl. Phys. 104, 053116 (2008).
[CrossRef]

K. Chen, C. Durak, J. R. Heflin, and H. D. Robinson, “Plasmon-enhanced second-harmonic generation from ionic self-assembled multilayer films,” Nano Lett. 7, 254-258 (2007).
[CrossRef] [PubMed]

J. R. Heflin, M. T. Guzy, P. J. Neyman, K. J. Gaskins, C. Brands, Z. Wang, H. W. Gibson, R. M. Davis, and K. E. Van Cott, “Efficient, thermally stable, second-order nonlinear optical response in organic hybrid covalent/ionic self-assembled films,” Langmuir 22, 5723-5727 (2006).
[CrossRef] [PubMed]

K. E. Van Cott, M. T. Guzy, P. J. Neyman, C. Brands, J. R. Heflin, H. W. Gibson, and R. M. Davis, “Layer-by-layer deposition and ordering of low-molecular-weight dye molecules for second-order nonlinear optics,” Angew. Chem., Int. Ed. Engl. 41, 3236-3238 (2002).
[CrossRef]

J. R. Heflin, C. Figura, D. Marciu, Y. Liu, and R. O. Claus, “Thickness dependence of second-harmonic generation in thin films fabricated from ionically self-assembled monolayers,” Appl. Phys. Lett. 74, 495-497 (1999).
[CrossRef]

Ishifuji, M.

M. Ishifuji, M. Mitsuishi, and T. Miyashita, “Bottom-up design of hybrid polymer nanoassemblies elucidates plasmon-enhanced second-harmonic generation from nonlinear optical dyes,” J. Am. Chem. Soc. 131, 4418-4424 (2009).
[CrossRef] [PubMed]

Itzkan, I.

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. Dasari, and M. S. Feld, “Single molecule detection using surface-enhanced Raman scattering (SERS),” Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

Jensen, T. R.

T. R. Jensen, M. D. Malinsky, C. L. Haynes, and R. P. Van Duyne, “Nanosphere lithography: tunable localized surface plasmon resonance spectra of silver nanoparticles,” J. Phys. Chem. B 104, 10549-10556 (2000).
[CrossRef]

Kajikawa, K.

K. Tsuboi, S. Abe, S. Fukuba, M. Shimojo, M. Tanaka, K. Furuya, K. Fujita, and K. Kajikawa, “Second-harmonic spectroscopy of surface immobilized gold nanospheres above a gold surface supported by self-assembled monolayers,” J. Phys. Chem. B 125, 174703 (2006).
[CrossRef]

Kambhampati, P.

A. Campion and P. Kambhampati, “Surface-enhanced Raman scattering,” Chem. Soc. Rev. 27, 241-250 (1998).
[CrossRef]

Kern, W.

W. Kern, “Purifying Si and SiO2 surfaces with hydrogen peroxide,” Semicond. Int. 7, 94-99 (1984).

Kneipp, H.

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. Dasari, and M. S. Feld, “Single molecule detection using surface-enhanced Raman scattering (SERS),” Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

Kneipp, K.

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. Dasari, and M. S. Feld, “Single molecule detection using surface-enhanced Raman scattering (SERS),” Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

Krishna, S.

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, 1027-1030 (2006).
[CrossRef]

Lewis, A.

H. A. Clark, P. J. Campagnola, J. P. Wuskell, A. Lewis, and L. M. Loew, “Second-harmonic generation properties of fluorescent polymer-encapsulated gold nanoparticles,” J. Am. Chem. Soc. 122, 10234-10235 (2000).
[CrossRef]

Lippitz, M.

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

Liu, Y.

J. R. Heflin, C. Figura, D. Marciu, Y. Liu, and R. O. Claus, “Thickness dependence of second-harmonic generation in thin films fabricated from ionically self-assembled monolayers,” Appl. Phys. Lett. 74, 495-497 (1999).
[CrossRef]

Loew, L. M.

H. A. Clark, P. J. Campagnola, J. P. Wuskell, A. Lewis, and L. M. Loew, “Second-harmonic generation properties of fluorescent polymer-encapsulated gold nanoparticles,” J. Am. Chem. Soc. 122, 10234-10235 (2000).
[CrossRef]

Malinsky, M. D.

T. R. Jensen, M. D. Malinsky, C. L. Haynes, and R. P. Van Duyne, “Nanosphere lithography: tunable localized surface plasmon resonance spectra of silver nanoparticles,” J. Phys. Chem. B 104, 10549-10556 (2000).
[CrossRef]

Malloy, K. J.

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, 1027-1030 (2006).
[CrossRef]

Marciu, D.

J. R. Heflin, C. Figura, D. Marciu, Y. Liu, and R. O. Claus, “Thickness dependence of second-harmonic generation in thin films fabricated from ionically self-assembled monolayers,” Appl. Phys. Lett. 74, 495-497 (1999).
[CrossRef]

Mitsuishi, M.

M. Ishifuji, M. Mitsuishi, and T. Miyashita, “Bottom-up design of hybrid polymer nanoassemblies elucidates plasmon-enhanced second-harmonic generation from nonlinear optical dyes,” J. Am. Chem. Soc. 131, 4418-4424 (2009).
[CrossRef] [PubMed]

Miyashita, T.

M. Ishifuji, M. Mitsuishi, and T. Miyashita, “Bottom-up design of hybrid polymer nanoassemblies elucidates plasmon-enhanced second-harmonic generation from nonlinear optical dyes,” J. Am. Chem. Soc. 131, 4418-4424 (2009).
[CrossRef] [PubMed]

Moses, E.

Murray, R. W.

A. C. Templeton, M. P. Wuelfing, and R. W. Murray, “Monolayer protected cluster molecules,” Acc. Chem. Res. 33, 27-36 (2000).
[CrossRef] [PubMed]

Neyman, P. J.

J. R. Heflin, M. T. Guzy, P. J. Neyman, K. J. Gaskins, C. Brands, Z. Wang, H. W. Gibson, R. M. Davis, and K. E. Van Cott, “Efficient, thermally stable, second-order nonlinear optical response in organic hybrid covalent/ionic self-assembled films,” Langmuir 22, 5723-5727 (2006).
[CrossRef] [PubMed]

K. E. Van Cott, M. T. Guzy, P. J. Neyman, C. Brands, J. R. Heflin, H. W. Gibson, and R. M. Davis, “Layer-by-layer deposition and ordering of low-molecular-weight dye molecules for second-order nonlinear optics,” Angew. Chem., Int. Ed. Engl. 41, 3236-3238 (2002).
[CrossRef]

Nie, S.

S. Nie and S. R. Emory, “Probing single molecules and single nanoparticles by surface-enhanced Raman scattering,” Science 275, 1102-1106 (1997).
[CrossRef] [PubMed]

Nie, S. M.

W. E. Doering and S. M. Nie, “Single-molecule and single-nanoparticle SERS: examining the roles of surface active sites and chemical enhancement,” J. Phys. B 106, 311-317 (2002).

Nuzzo, R. G.

C. D. Bain, E. B. Troughton, Y. T. Tao, J. Evall, G. M. Whitesides, and R. G. Nuzzo, “Formation of monolayer films by the spontaneous assembly of organic thiols from solution onto gold,” J. Am. Chem. Soc. 111, 321-335 (1989).
[CrossRef]

Oron, D.

Orrit, M.

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

Osgood, R. M.

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, 1027-1030 (2006).
[CrossRef]

Panoiu, N. C.

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, 1027-1030 (2006).
[CrossRef]

Perelman, L. T.

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. Dasari, and M. S. Feld, “Single molecule detection using surface-enhanced Raman scattering (SERS),” Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

Perez-Segarra, W.

Y. Zhao, W. Perez-Segarra, Q. C. Shi, and A. Wei, “Dithiocarbamate assembly on gold,” J. Am. Chem. Soc. 127, 7328-7329 (2005).
[CrossRef] [PubMed]

Prevo, B. G.

B. G. Prevo and O. D. Velev, “Controlled, rapid deposition of structured coatings from micro- and nanoparticle suspensions,” Langmuir 20, 2099-2107 (2004).
[CrossRef]

Robinson, H. D.

K. Chen, C. Durak, J. R. Heflin, and H. D. Robinson, “Plasmon-enhanced second-harmonic generation from ionic self-assembled multilayer films,” Nano Lett. 7, 254-258 (2007).
[CrossRef] [PubMed]

Sarychev, A. K.

D. A. Genov, A. K. Sarychev, V. M. Shalaev, and A. Wei, “Resonant field enhancements from metal nanoparticle arrays,” Nano Lett. 4, 153-158 (2003).
[CrossRef]

Schatz, G. C.

E. Hao and G. C. Schatz, “Electromagnetic fields around silver nanoparticles and dimers,” J. Phys. Chem. 120, 357-366 (2004).
[CrossRef]

Shalaev, V. M.

D. A. Genov, A. K. Sarychev, V. M. Shalaev, and A. Wei, “Resonant field enhancements from metal nanoparticle arrays,” Nano Lett. 4, 153-158 (2003).
[CrossRef]

Shi, Q. C.

Y. Zhao, W. Perez-Segarra, Q. C. Shi, and A. Wei, “Dithiocarbamate assembly on gold,” J. Am. Chem. Soc. 127, 7328-7329 (2005).
[CrossRef] [PubMed]

Shimojo, M.

K. Tsuboi, S. Abe, S. Fukuba, M. Shimojo, M. Tanaka, K. Furuya, K. Fujita, and K. Kajikawa, “Second-harmonic spectroscopy of surface immobilized gold nanospheres above a gold surface supported by self-assembled monolayers,” J. Phys. Chem. B 125, 174703 (2006).
[CrossRef]

Silberberg, Y.

Sun, J.

M. C. Tong, W. Chen, J. Sun, D. Ghosh, and S. W. Chen, “Dithiocarbamate-capped silver nanoparticles,” J. Phys. B 110, 19238-19242 (2006).

Tanaka, M.

K. Tsuboi, S. Abe, S. Fukuba, M. Shimojo, M. Tanaka, K. Furuya, K. Fujita, and K. Kajikawa, “Second-harmonic spectroscopy of surface immobilized gold nanospheres above a gold surface supported by self-assembled monolayers,” J. Phys. Chem. B 125, 174703 (2006).
[CrossRef]

Tao, Y. T.

C. D. Bain, E. B. Troughton, Y. T. Tao, J. Evall, G. M. Whitesides, and R. G. Nuzzo, “Formation of monolayer films by the spontaneous assembly of organic thiols from solution onto gold,” J. Am. Chem. Soc. 111, 321-335 (1989).
[CrossRef]

Templeton, A. C.

A. C. Templeton, M. P. Wuelfing, and R. W. Murray, “Monolayer protected cluster molecules,” Acc. Chem. Res. 33, 27-36 (2000).
[CrossRef] [PubMed]

Thiberge, S.

Tong, M. C.

M. C. Tong, W. Chen, J. Sun, D. Ghosh, and S. W. Chen, “Dithiocarbamate-capped silver nanoparticles,” J. Phys. B 110, 19238-19242 (2006).

Troughton, E. B.

C. D. Bain, E. B. Troughton, Y. T. Tao, J. Evall, G. M. Whitesides, and R. G. Nuzzo, “Formation of monolayer films by the spontaneous assembly of organic thiols from solution onto gold,” J. Am. Chem. Soc. 111, 321-335 (1989).
[CrossRef]

Tsang, T. Y. F.

Tsuboi, K.

K. Tsuboi, S. Abe, S. Fukuba, M. Shimojo, M. Tanaka, K. Furuya, K. Fujita, and K. Kajikawa, “Second-harmonic spectroscopy of surface immobilized gold nanospheres above a gold surface supported by self-assembled monolayers,” J. Phys. Chem. B 125, 174703 (2006).
[CrossRef]

Van Cott, K. E.

J. R. Heflin, M. T. Guzy, P. J. Neyman, K. J. Gaskins, C. Brands, Z. Wang, H. W. Gibson, R. M. Davis, and K. E. Van Cott, “Efficient, thermally stable, second-order nonlinear optical response in organic hybrid covalent/ionic self-assembled films,” Langmuir 22, 5723-5727 (2006).
[CrossRef] [PubMed]

K. E. Van Cott, M. T. Guzy, P. J. Neyman, C. Brands, J. R. Heflin, H. W. Gibson, and R. M. Davis, “Layer-by-layer deposition and ordering of low-molecular-weight dye molecules for second-order nonlinear optics,” Angew. Chem., Int. Ed. Engl. 41, 3236-3238 (2002).
[CrossRef]

van Dijk, M. A.

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

Van Duyne, R. P.

A. J. Haes and R. P. Van Duyne, “A nanoscale optical blosensor: sensitivity and selectivity of an approach based on the localized surface plasmon resonance spectroscopy of triangular silver nanoparticles,” J. Am. Chem. Soc. 124, 10596-10604 (2002).
[CrossRef] [PubMed]

C. L. Haynes and R. P. Van Duyne, “Nanosphere lithography: a versatile nanofabrication tool for studies of size-dependent nanoparticle optics,” J. Phys. Chem. B 105, 5599-5611 (2001).
[CrossRef]

T. R. Jensen, M. D. Malinsky, C. L. Haynes, and R. P. Van Duyne, “Nanosphere lithography: tunable localized surface plasmon resonance spectra of silver nanoparticles,” J. Phys. Chem. B 104, 10549-10556 (2000).
[CrossRef]

Velev, O. D.

B. G. Prevo and O. D. Velev, “Controlled, rapid deposition of structured coatings from micro- and nanoparticle suspensions,” Langmuir 20, 2099-2107 (2004).
[CrossRef]

Wang, Y.

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. Dasari, and M. S. Feld, “Single molecule detection using surface-enhanced Raman scattering (SERS),” Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

Wang, Z.

J. R. Heflin, M. T. Guzy, P. J. Neyman, K. J. Gaskins, C. Brands, Z. Wang, H. W. Gibson, R. M. Davis, and K. E. Van Cott, “Efficient, thermally stable, second-order nonlinear optical response in organic hybrid covalent/ionic self-assembled films,” Langmuir 22, 5723-5727 (2006).
[CrossRef] [PubMed]

Wei, A.

Y. Zhao, W. Perez-Segarra, Q. C. Shi, and A. Wei, “Dithiocarbamate assembly on gold,” J. Am. Chem. Soc. 127, 7328-7329 (2005).
[CrossRef] [PubMed]

D. A. Genov, A. K. Sarychev, V. M. Shalaev, and A. Wei, “Resonant field enhancements from metal nanoparticle arrays,” Nano Lett. 4, 153-158 (2003).
[CrossRef]

Whitesides, G. M.

C. D. Bain, E. B. Troughton, Y. T. Tao, J. Evall, G. M. Whitesides, and R. G. Nuzzo, “Formation of monolayer films by the spontaneous assembly of organic thiols from solution onto gold,” J. Am. Chem. Soc. 111, 321-335 (1989).
[CrossRef]

Wuelfing, M. P.

A. C. Templeton, M. P. Wuelfing, and R. W. Murray, “Monolayer protected cluster molecules,” Acc. Chem. Res. 33, 27-36 (2000).
[CrossRef] [PubMed]

Wuskell, J. P.

H. A. Clark, P. J. Campagnola, J. P. Wuskell, A. Lewis, and L. M. Loew, “Second-harmonic generation properties of fluorescent polymer-encapsulated gold nanoparticles,” J. Am. Chem. Soc. 122, 10234-10235 (2000).
[CrossRef]

Yelin, D.

Zhang, S.

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, 1027-1030 (2006).
[CrossRef]

Zhao, Y.

Y. Zhao, W. Perez-Segarra, Q. C. Shi, and A. Wei, “Dithiocarbamate assembly on gold,” J. Am. Chem. Soc. 127, 7328-7329 (2005).
[CrossRef] [PubMed]

Acc. Chem. Res. (1)

A. C. Templeton, M. P. Wuelfing, and R. W. Murray, “Monolayer protected cluster molecules,” Acc. Chem. Res. 33, 27-36 (2000).
[CrossRef] [PubMed]

Angew. Chem., Int. Ed. Engl. (1)

K. E. Van Cott, M. T. Guzy, P. J. Neyman, C. Brands, J. R. Heflin, H. W. Gibson, and R. M. Davis, “Layer-by-layer deposition and ordering of low-molecular-weight dye molecules for second-order nonlinear optics,” Angew. Chem., Int. Ed. Engl. 41, 3236-3238 (2002).
[CrossRef]

Appl. Phys. Lett. (1)

J. R. Heflin, C. Figura, D. Marciu, Y. Liu, and R. O. Claus, “Thickness dependence of second-harmonic generation in thin films fabricated from ionically self-assembled monolayers,” Appl. Phys. Lett. 74, 495-497 (1999).
[CrossRef]

Chem. Soc. Rev. (1)

A. Campion and P. Kambhampati, “Surface-enhanced Raman scattering,” Chem. Soc. Rev. 27, 241-250 (1998).
[CrossRef]

J. Am. Chem. Soc. (5)

A. J. Haes and R. P. Van Duyne, “A nanoscale optical blosensor: sensitivity and selectivity of an approach based on the localized surface plasmon resonance spectroscopy of triangular silver nanoparticles,” J. Am. Chem. Soc. 124, 10596-10604 (2002).
[CrossRef] [PubMed]

Y. Zhao, W. Perez-Segarra, Q. C. Shi, and A. Wei, “Dithiocarbamate assembly on gold,” J. Am. Chem. Soc. 127, 7328-7329 (2005).
[CrossRef] [PubMed]

H. A. Clark, P. J. Campagnola, J. P. Wuskell, A. Lewis, and L. M. Loew, “Second-harmonic generation properties of fluorescent polymer-encapsulated gold nanoparticles,” J. Am. Chem. Soc. 122, 10234-10235 (2000).
[CrossRef]

M. Ishifuji, M. Mitsuishi, and T. Miyashita, “Bottom-up design of hybrid polymer nanoassemblies elucidates plasmon-enhanced second-harmonic generation from nonlinear optical dyes,” J. Am. Chem. Soc. 131, 4418-4424 (2009).
[CrossRef] [PubMed]

C. D. Bain, E. B. Troughton, Y. T. Tao, J. Evall, G. M. Whitesides, and R. G. Nuzzo, “Formation of monolayer films by the spontaneous assembly of organic thiols from solution onto gold,” J. Am. Chem. Soc. 111, 321-335 (1989).
[CrossRef]

J. Appl. Phys. (1)

A. Garg, R. M. Davis, C. Durak, J. R. Heflin, and H. W. Gibson, “Polar orientation of a pendant anionic chromophore in thick layer-by-layer self-assembled polymeric films,” J. Appl. Phys. 104, 053116 (2008).
[CrossRef]

J. Phys. B (2)

M. C. Tong, W. Chen, J. Sun, D. Ghosh, and S. W. Chen, “Dithiocarbamate-capped silver nanoparticles,” J. Phys. B 110, 19238-19242 (2006).

W. E. Doering and S. M. Nie, “Single-molecule and single-nanoparticle SERS: examining the roles of surface active sites and chemical enhancement,” J. Phys. B 106, 311-317 (2002).

J. Phys. Chem. (1)

E. Hao and G. C. Schatz, “Electromagnetic fields around silver nanoparticles and dimers,” J. Phys. Chem. 120, 357-366 (2004).
[CrossRef]

J. Phys. Chem. B (3)

K. Tsuboi, S. Abe, S. Fukuba, M. Shimojo, M. Tanaka, K. Furuya, K. Fujita, and K. Kajikawa, “Second-harmonic spectroscopy of surface immobilized gold nanospheres above a gold surface supported by self-assembled monolayers,” J. Phys. Chem. B 125, 174703 (2006).
[CrossRef]

C. L. Haynes and R. P. Van Duyne, “Nanosphere lithography: a versatile nanofabrication tool for studies of size-dependent nanoparticle optics,” J. Phys. Chem. B 105, 5599-5611 (2001).
[CrossRef]

T. R. Jensen, M. D. Malinsky, C. L. Haynes, and R. P. Van Duyne, “Nanosphere lithography: tunable localized surface plasmon resonance spectra of silver nanoparticles,” J. Phys. Chem. B 104, 10549-10556 (2000).
[CrossRef]

Langmuir (2)

J. R. Heflin, M. T. Guzy, P. J. Neyman, K. J. Gaskins, C. Brands, Z. Wang, H. W. Gibson, R. M. Davis, and K. E. Van Cott, “Efficient, thermally stable, second-order nonlinear optical response in organic hybrid covalent/ionic self-assembled films,” Langmuir 22, 5723-5727 (2006).
[CrossRef] [PubMed]

B. G. Prevo and O. D. Velev, “Controlled, rapid deposition of structured coatings from micro- and nanoparticle suspensions,” Langmuir 20, 2099-2107 (2004).
[CrossRef]

Nano Lett. (4)

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, 1027-1030 (2006).
[CrossRef]

K. Chen, C. Durak, J. R. Heflin, and H. D. Robinson, “Plasmon-enhanced second-harmonic generation from ionic self-assembled multilayer films,” Nano Lett. 7, 254-258 (2007).
[CrossRef] [PubMed]

D. A. Genov, A. K. Sarychev, V. M. Shalaev, and A. Wei, “Resonant field enhancements from metal nanoparticle arrays,” Nano Lett. 4, 153-158 (2003).
[CrossRef]

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

Opt. Express (1)

Opt. Lett. (1)

Phys. Rev. Lett. (1)

K. Kneipp, Y. Wang, H. Kneipp, L. T. Perelman, I. Itzkan, R. Dasari, and M. S. Feld, “Single molecule detection using surface-enhanced Raman scattering (SERS),” Phys. Rev. Lett. 78, 1667-1670 (1997).
[CrossRef]

Science (2)

S. Nie and S. R. Emory, “Probing single molecules and single nanoparticles by surface-enhanced Raman scattering,” Science 275, 1102-1106 (1997).
[CrossRef] [PubMed]

G. Decher, “Fuzzy nanoassemblies: toward layered polymeric multicomposites,” Science 277, 1232-1237 (1997).
[CrossRef]

Semicond. Int. (1)

W. Kern, “Purifying Si and SiO2 surfaces with hydrogen peroxide,” Semicond. Int. 7, 94-99 (1984).

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Figures (7)

Fig. 1
Fig. 1

Illustration of the structures of (a) ISAM films, where cationic and anionic polyelectrolytes are arranged in a layered structure, and (b) HCISAM films, where the cationic layer consists of monomers (in this case Procion Brown) that are covalently bound to the underlying polycation (PAH).

Fig. 2
Fig. 2

Absorption spectrum of a 2-bilayer PAH/PCBS ISAM film decorated with triangular Ag nanoparticles fabricated through nanosphere lithography (shown in inset). The noise around 800 nm is due the change of gratings and detectors inside the spectrometer.

Fig. 3
Fig. 3

SHG intensity as a function of film thickness for conventional PAH/PCBS and PAH/PB films (crossed circles and empty diamonds, respectively) and for the same films as modified by Ag nanoparticles (solid circles and crossed diamonds). The dash-dotted line indicates SHG intensity from Ag nanoparticles in the absence of an ISAM film.

Fig. 4
Fig. 4

Square root of the SHG intensity from PAH/PCBS ISAM films as a function of thickness with and without ten NLO-inactive PAH/PAA buffers. The addition of the buffers eliminates the interface contribution (y intercept) to the SHG signal. The lines are a guide to the eye.

Fig. 5
Fig. 5

Schemes of the four different configurations: (a) film only, (b) film–buffer, (c) buffer–film, (d) buffer–film–buffer. The films are NLO-active 1-bilayer or 3-bilayer PAH/PCBS or PAH/PB films, while each buffer consists of 10 bilayers of NLO-inactive PAH/PAA.

Fig. 6
Fig. 6

Linear (absorption) and nonlinear (SHG) optical properties of films with or without buffer layers in the four different film/buffer combinations sketched in Fig. 3. (a), (b) Film absorption. (c), (d) Square root of SHG intensity. (e), (f) Square root of SHG intensity divided by absorption; used as a figure of merit of film performance.

Fig. 7
Fig. 7

Comparison of SHG signal from freshly made PAH/PB HCISAM film with the signal from films that are several months old. For the aged films, the SHG intensity is smaller from the thinnest films, and the minimum in the signal is shifted towards lower film thickness. The lines are mainly guides to the eye, as no formal fittings have been attempted to the data. However, the lines represent the expected functional dependence of a constant interface SHG out of phase with a bulk SHG that varies as the square of the number of bilayers.

Tables (2)

Tables Icon

Table 1 Deposition Conditions for PAH/PCBS and PAH/PB ISAM Films

Tables Icon

Table 2 Effective χ ( 2 ) Values for PAH/PCBS and PAH/PB Films as Derived by Least-squared Fit from the Data Compared to Bulk χ ( 2 ) Values from a Single ISAM Bilayer a

Equations (1)

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

χ eff ( 2 ) = g + a + γ b l ,

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