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Sub-Microscopic Probing of Intrinsic and Extrinsic Enhancement of Second Harmonic Generation of Nano-Structured Gold Surfaces

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Organic Nanophotonics

Part of the book series: NATO Science Series ((NAII,volume 100))

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Abstract

This paper describes the local enhancement of quadratic nonlinear optical properties of granular gold nano-structures and their effect on nonlinear molecules deposited on them. A two-photon excitation microscope has been employed in order to detect second harmonic generation with a sub-microscopic resolution. Surface-SHG from the gold granular structures exhibits intense signals in sub-micrometer sized regions randomly localized on the surface. The spatial distribution and polarization state of these signals provides significant information on the underlying physics of the local enhancement effect. We show furthermore that the signal from nonlinear chromophores deposited on these substrates is strongly enhanced with factors up to 2×103, before decaying within a few seconds. Quantitative measurements indicate a significant local electromagnetic contribution to the molecular enhancement. Molecular damage and possible metal-molecule interactions are analyzed in order to explain the magnitude and the fast decay of this effect.

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References

  1. Oldenburg, S.J., Averitt, R.D., Westcott, S.L. and Halas, N.J. (1998) Nanoengineering of optical resonances, Chem. Phys. Lett. 288, 243–7.

    Article  ADS  Google Scholar 

  2. Doremus, R.H. (1964) Optical properties of small gold nanoparticles, Journ. Chem. Phys. 40, 2389–96.

    Article  ADS  Google Scholar 

  3. Kreibig, U. and Vollmer, M. (1995). Optical Properties of Metal Clusters Springer Verlag

    Book  Google Scholar 

  4. Chang, R.K. and Furtark, T.E. (1982). Surface Enhanced Raman Scattering, New York Plenum Press

    Book  Google Scholar 

  5. Golab, J.T., Sprague, J.R., Carron, K.T., Schatz, G.C. and Van Duyne, R.P. (1988) A surface enhanced hyper-Raman scattering study of pyridine adsorbed onto silver: Experiment and theory, J. Chem. Phys. 88, 7942.

    Article  ADS  Google Scholar 

  6. Andrews, M., Kusyk, M.G. and Ghebremichael, F. (1993) Local field enhancement of the cubic optical nonlinearity in fractal silver nanosphere/poly(methylmetacrylate) composite, Nonlinear Optics 6, 103–12.

    Google Scholar 

  7. Zhang, J., Zhao, J., He, H., Zhang, H., Li, H. and Liu, Z. (1998) Studies on the surface enhanced infrared spectroscopy of Langmuir-Blodgett monolayers of azobenzene carboxylic acid on silver island films, Langmuir 14, 5521–5.

    Article  Google Scholar 

  8. Kneipp, K., Wang, Y., Kneipp, H., Perelman, L.T., Itzkan, I., Dasari, R.R. and Feld, M.S. (1997) Single Molecule Detection using Surface-Enhanced Raman Scattering, Phys. Rev. Lett. 78, 1667.

    Article  ADS  Google Scholar 

  9. Nie, S. and Emory, S. (1997) Science 275, 110–1106.

    Article  Google Scholar 

  10. Delvin, J.P. and Consani, K. (1981) J. Phys. Chem. 85, 2597.

    Article  Google Scholar 

  11. Maxwell, D.J., Emory, S. and Nie, S. (2001) Nanostructured thin-film materials with surface-enhanced optical properties, Chem. Mater. 13, 1082–8.

    Article  Google Scholar 

  12. Shalaev, V.M. and Sarychev, A.K. (1998) Nonlinear optics of random metal-dielectric films, Physical Review B 57, 13265–88.

    Article  ADS  Google Scholar 

  13. Grésillon, S., Aigouy, L., Boccara, A.C., Rivoal, J.C., Quélin, X., Desmarest, C., Gadenne, P., Shubin, V.A., Sarychev, A.K. and Shalaev, V.M. (1999) Experimental Observation of Localized Optical Excitations in Random Metal-Dielectric Films, Phys. Rev. Lett. 82, 4520–3.

    Article  ADS  Google Scholar 

  14. Guyot-Sionnest, P., Chen, W. and Shen, Y.R. (1986) General considerations on optical second-harmonic from surfaces and interfaces, Phys. Rev. B. 33, 8254–63.

    Article  ADS  Google Scholar 

  15. Bloembergen, N., Chang, R.K., Jha, S.S. and Lee, C.H. (1968) Optical second-harmonic generation in reflection from media with inversion symmetry, Phys. Rev. 174, 813.

    Article  ADS  Google Scholar 

  16. Chang, C.S. and Lue, J.T. (1997) Optical second harmonic generation from thin silver films, Surface Science 393, 232–9.

    Article  ADS  Google Scholar 

  17. Pluchery, O., Zheng, W.Q., Marin, T. and Tadjeddine, A. (1999) Study of the absorption of 4-cyanopyridine on Au(lll) using sum frequency generation nonlinear spectroscopy, Physica Status Solidi A 175, 145–51.

    Article  ADS  Google Scholar 

  18. Aktsipetrov, O.A., Keller, O., Pedersen, K., Nikulin, A.A., Novikova, N.N. and Fedyanin, A.A. (1993) Surface-enhanced second harmonic generation in C60-coated silver island films, Phys. Lett. A 179, 149–53.

    Article  ADS  Google Scholar 

  19. Manaka, T. and Manaka, I. (2001) Enhancement of second harmonic generation from phtalocyanine Langmuir-Blodgett films on metal electrodes, Thin Solid Films 393, 119–23.

    Article  ADS  Google Scholar 

  20. Jha, S.S. (1965) Phys. Rev. A 140, 2020.

    ADS  Google Scholar 

  21. Rudnick, J. and Stern, E.A. (1971) Second-harmonic radiation from metal surfaces, Phys. Rev. B 4, 4274–90.

    Article  ADS  Google Scholar 

  22. Weber, M. and Liebsch, A. (1987) Density-functional theory appraoch to second-harmonic generation at metal surfaces, Phys. Rev. B 35, 7411–6.

    Article  ADS  Google Scholar 

  23. Boyd, G.T., Rasing, T., Leite, J.R.R. and Shen, Y.R. (1984) Local-field enhancement on rough surfaces of metals, semimetals, and semiconductors with the use of optical second-harmonic generation, Phys. Rev. B. 30, 519–26.

    Article  ADS  Google Scholar 

  24. Van Driel, H.M. (1994) Second-harmonic generation from metal surfaces: beyond jellium, Appl. Phys. A 59, 545–52.

    Article  ADS  Google Scholar 

  25. Chen, C.K., Castro, A.R.B. and Shen, Y.R. (1981) Surface-Enhanced Second-Harmonic Generation, Phys. Rev. Lett. 46, 145–8.

    Article  ADS  Google Scholar 

  26. Poliakov, E.Y., Markel, V.A., Shalaev, V.M. and Botet, R. (1998) Nonlinear optical phenomena on rough surfaces of metal thin films, Phys. Rev. B 57, 14901–13.

    Article  ADS  Google Scholar 

  27. Podolskiy, V.A., Sarychev, A.K. and Shalaev, V.M. (2002) Temporal Dynamics of Local Optical Responses and Sub-fs Pulse Generation in Semicontinuous Metal Films, Laser Physics 12, 292–9.

    Google Scholar 

  28. Zayats, A.V., Smolyaninov, I.I. and Davis, C.C. (1999) Observation of localized plasmonic excitations in thin metal films with near-field second harmonic microscopy, Opt. Comm. 169, 93–6.

    Article  ADS  Google Scholar 

  29. Breit, M., Podolsky, V.A., Grésillon, S., Von Plessen, G., Feldmann, J., Rivoal, J.C., Gadenne, P., Sarychev, A.K. and Shalaev, V.M. (2001) Experimental observation of percolation-enhanced non-linear scattering from semi-continuous gold films, Phys. Rev. B. 64, 106.

    Article  Google Scholar 

  30. Ducourtieux, S., Grésillon, S., Boccara, A.C., Rivoal, J.C., Quélin, X., Gadenne, P., Drachev, V.P., Bragg, W.D., Safonov, V.P., Podolskiy, V.A., Ying, Z.C., Armstrong, R.L. and Shalaev, V.M. (2000) Percolation and Fractal composites: Optical Studies, Jour.Nonlinear Opt. Phys. Mat. 9, 105.

    ADS  Google Scholar 

  31. Anceau, C., Brasselet, S., Gadenne, P. and Zyss, J. (2002) Local second harmonic generation enhancement on gold nanostructures probed by 2-photon microscopy, submitted

    Google Scholar 

  32. Safonov, V.P., Shalaev, V.M., Markel, V.A., Danilova, Y.E., Lepeshkin, N.N., Kim, W., Rautan, S.G. and Armstrong, R.L. (1998) Spectral dependance of selective photomodification in fractal aggregates of colloidal particules, Phys. Rev. Lett. 80, 1102–5.

    Article  ADS  Google Scholar 

  33. Stockman, M.I. (2000) Giant attosecond fluctuations of local optical fields in disordered nanostructured media, Phys. Rev. B 62, 10494–7.

    Article  ADS  Google Scholar 

  34. Ducourtieux, S., Podolskiy, V.A., Grésillon, S., Buil, S., Bérini, B. and Gadenne, P. (2001) Near-field optical studies of semi-continuous metal films, Phys. Rev. B 64, 1554.

    Article  Google Scholar 

  35. Shen, Y.R. (1994) Nonlinear optical studies of surfaces, Appl. Physics A 59, 541–3.

    Article  ADS  Google Scholar 

  36. Aroca, R.F. and Constantino, C.J.L. (2000) Surface-enhanced Raman scattering: imaging and mapping of Langmuir-Blodgett monolayers physically adsorbed onto siver island films, Langmuir 16, 5425–9.

    Article  Google Scholar 

  37. Simpson, G.J. and Rowlen, K.L. (2000) Measurement of Orientation in Organic Thin Films, Acc. Chem. Res. 33, 781–9.

    Article  Google Scholar 

  38. Zhang, Z.J., Verma, A.L., Tamai, N., Nakashima, K., Yoneyama, M., Iriyama, K. and Ozaki, Y. (1998) Excitation energy transfer in Langmuir-Blodgett films of 5-(4-N-octadecylpyridyl)-10, 15, 20-tri-tolyporphyrin on gold-evaporated surfaces studied by time-resolved fluorescence spectroscopy, Thin Solid Films 333, 1–4.

    Article  ADS  Google Scholar 

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Author information

Authors and Affiliations

  1. Laboratoire de Photonique Quantique et Moléculaire, Ecole Normale Supérieure de Cachan, 94235, Cachan, France

    S. Brasselet, C. Anceau & J. Zyss

  2. Laboratoire de Magnétisme et d’Optique de Versailles, Université de Versailles Saint-Quentin en Yvelines, 78035, Versailles Cedex, France

    C. Anceau & P. Gadenne

Authors
  1. S. Brasselet
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  2. C. Anceau
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  3. P. Gadenne
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  4. J. Zyss
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Editor information

Editors and Affiliations

  1. Direction for Matter Sciences (DSM), Atomic Energy Commission, Saclay, France

    Fabrice Charra

  2. Institute of Spectroscopy, Russian Academy of Sciences, Troisk, Russia

    Vladimir M. Agranovich

  3. Direction for Technological Research (DRT), Atomic Energy Commission (CEA), Saclay, France

    François Kajzar

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© 2003 Springer Science+Business Media Dordrecht

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Brasselet, S., Anceau, C., Gadenne, P., Zyss, J. (2003). Sub-Microscopic Probing of Intrinsic and Extrinsic Enhancement of Second Harmonic Generation of Nano-Structured Gold Surfaces. In: Charra, F., Agranovich, V.M., Kajzar, F. (eds) Organic Nanophotonics. NATO Science Series, vol 100. Springer, Dordrecht. https://doi.org/10.1007/978-94-010-0103-8_29

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  • DOI: https://doi.org/10.1007/978-94-010-0103-8_29

  • Publisher Name: Springer, Dordrecht

  • Print ISBN: 978-1-4020-1280-8

  • Online ISBN: 978-94-010-0103-8

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