Abstract

Nonlinear plasmonics opens up for wavelength conversion, reduced interaction/emission volumes, and nonlinear enhancement effects at the nanoscale with many compelling nanophotonic applications foreseen. We investigate nonlinear plasmonic responses of nanoholes in thin gold films by exciting the holes individually with tightly focused laser beams, employing a degenerated pump/probe and Stokes excitation scheme. Excitation of the holes results in efficient generation of both narrowband four-wave mixing (FWM) and broadband multiphoton excited luminescence, blueshifted relative to the excitation beams. Clear enhancements were observed when matching the pump/probe wavelength with the hole plasmon resonance. These observations show that the FWM generation is locally excited by nanoholes and has a resonant behavior primarily governed by the dimensions of the individual holes.

© 2014 Optical Society of America

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2012 (1)

2011 (3)

X. Liu, Y. Wang, and E. O. Potma, Opt. Lett. 36, 2348 (2011).
[CrossRef]

T. Sannomiya, O. Scholder, K. Jefimovs, C. Hafner, and A. B. Dahlin, Small 7, 1653 (2011).
[CrossRef]

C. Steuwe, C. F. Kaminski, J. J. Baumberg, and S. Mahajan, Nano Lett. 11, 5339 (2011).
[CrossRef]

2010 (2)

P. Genevet, J.-P. Tetienne, E. Gatzogiannis, R. Blanchard, M. A. Kats, M. O. Scully, and F. Capasso, Nano Lett. 10, 4880 (2010).
[CrossRef]

A. Enejder, C. Brackmann, and F. Svedberg, IEEE J. Sel. Top. Quantum Electron. 16, 506 (2010).
[CrossRef]

2009 (2)

J. Renger, R. Quidant, N. van Hulst, S. Palomba, and L. Novotny, Phys. Rev. Lett. 103, 266802 (2009).
[CrossRef]

A. B. Dahlin, S. Chen, M. P. Jonsson, L. Gunnarsson, M. Kall, and F. Hook, Anal. Chem. 81, 6572 (2009).
[CrossRef]

2008 (6)

S. Palomba and L. Novotny, Phys. Rev. Lett. 101, 056802 (2008).
[CrossRef]

H. Kim, D. K. Taggart, C. X. Xiang, R. M. Penner, and E. O. Potma, Nano Lett. 8, 2373 (2008).
[CrossRef]

S. Kim, J. Jin, Y.-J. Kim, I.-Y. Park, Y. Kim, and S.-W. Kim, Nature 453, 757 (2008).
[CrossRef]

M. P. Jonsson, A. B. Dahlin, P. Jonsson, and F. Hook, Biointerphases 3, Fd30 (2008).
[CrossRef]

J. Alegret, P. Johansson, and M. Kall, New J. Phys. 10, 105004 (2008).
[CrossRef]

T. H. Park, N. Mirin, J. B. Lassiter, C. L. Nehl, N. J. Halas, and P. Nordlander, ACS Nano 2, 25 (2008).
[CrossRef]

2006 (1)

A. Lesuffleur, L. K. S. Kumar, and R. Gordon, Appl. Phys. Lett. 88, 261104 (2006).
[CrossRef]

2005 (6)

M. Lippitz, M. A. van Dijk, and M. Orrit, Nano Lett. 5, 799 (2005).
[CrossRef]

R. A. Farrer, F. L. Butterfield, V. W. Chen, and J. T. Fourkas, Nano Lett. 5, 1139 (2005).
[CrossRef]

P. Muhlschlegel, H. J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, Science 308, 1607 (2005).
[CrossRef]

S. I. Bozhevolnyi, V. S. Volkov, E. Devaux, and T. W. Ebbesen, Phys. Rev. Lett. 95, 046802 (2005).
[CrossRef]

H. Ditlbacher, A. Hohenau, D. Wagner, U. Kreibig, M. Rogers, F. Hofer, F. R. Aussenegg, and J. R. Krenn, Phys. Rev. Lett. 95, 257403 (2005).
[CrossRef]

T. Rindzevicius, Y. Alaverdyan, A. Dahlin, F. Hook, D. S. Sutherland, and M. Kall, Nano Lett. 5, 2335 (2005).
[CrossRef]

2003 (4)

P. Hanarp, D. S. Sutherland, J. Gold, and B. Kasemo, Colloids Surf. A 214, 23 (2003).
[CrossRef]

A. Bouhelier, M. Beversluis, A. Hartschuh, and L. Novotny, Phys. Rev. Lett. 90, 013903 (2003).
[CrossRef]

A. D. McFarland and R. P. Van Duyne, Nano Lett. 3, 1057 (2003).
[CrossRef]

S. I. Bozhevolnyi, J. Beermann, and V. Coello, Phys. Rev. Lett. 90, 197403 (2003).
[CrossRef]

Afanasiev, A. E.

Alaverdyan, Y.

T. Rindzevicius, Y. Alaverdyan, A. Dahlin, F. Hook, D. S. Sutherland, and M. Kall, Nano Lett. 5, 2335 (2005).
[CrossRef]

Alegret, J.

J. Alegret, P. Johansson, and M. Kall, New J. Phys. 10, 105004 (2008).
[CrossRef]

Aussenegg, F. R.

H. Ditlbacher, A. Hohenau, D. Wagner, U. Kreibig, M. Rogers, F. Hofer, F. R. Aussenegg, and J. R. Krenn, Phys. Rev. Lett. 95, 257403 (2005).
[CrossRef]

Balykin, V. I.

Baturin, A. S.

Baumberg, J. J.

C. Steuwe, C. F. Kaminski, J. J. Baumberg, and S. Mahajan, Nano Lett. 11, 5339 (2011).
[CrossRef]

Beermann, J.

S. I. Bozhevolnyi, J. Beermann, and V. Coello, Phys. Rev. Lett. 90, 197403 (2003).
[CrossRef]

Beversluis, M.

A. Bouhelier, M. Beversluis, A. Hartschuh, and L. Novotny, Phys. Rev. Lett. 90, 013903 (2003).
[CrossRef]

Blanchard, R.

P. Genevet, J.-P. Tetienne, E. Gatzogiannis, R. Blanchard, M. A. Kats, M. O. Scully, and F. Capasso, Nano Lett. 10, 4880 (2010).
[CrossRef]

Bouhelier, A.

A. Bouhelier, M. Beversluis, A. Hartschuh, and L. Novotny, Phys. Rev. Lett. 90, 013903 (2003).
[CrossRef]

Bozhevolnyi, S. I.

S. I. Bozhevolnyi, V. S. Volkov, E. Devaux, and T. W. Ebbesen, Phys. Rev. Lett. 95, 046802 (2005).
[CrossRef]

S. I. Bozhevolnyi, J. Beermann, and V. Coello, Phys. Rev. Lett. 90, 197403 (2003).
[CrossRef]

Brackmann, C.

A. Enejder, C. Brackmann, and F. Svedberg, IEEE J. Sel. Top. Quantum Electron. 16, 506 (2010).
[CrossRef]

Butterfield, F. L.

R. A. Farrer, F. L. Butterfield, V. W. Chen, and J. T. Fourkas, Nano Lett. 5, 1139 (2005).
[CrossRef]

Capasso, F.

P. Genevet, J.-P. Tetienne, E. Gatzogiannis, R. Blanchard, M. A. Kats, M. O. Scully, and F. Capasso, Nano Lett. 10, 4880 (2010).
[CrossRef]

Chen, S.

A. B. Dahlin, S. Chen, M. P. Jonsson, L. Gunnarsson, M. Kall, and F. Hook, Anal. Chem. 81, 6572 (2009).
[CrossRef]

Chen, V. W.

R. A. Farrer, F. L. Butterfield, V. W. Chen, and J. T. Fourkas, Nano Lett. 5, 1139 (2005).
[CrossRef]

Cheng, J.-X.

J.-X. Cheng and X. S. Xie, Coherent Raman Scattering Microscopy (CRC Press, 2013).

Coello, V.

S. I. Bozhevolnyi, J. Beermann, and V. Coello, Phys. Rev. Lett. 90, 197403 (2003).
[CrossRef]

Dahlin, A.

T. Rindzevicius, Y. Alaverdyan, A. Dahlin, F. Hook, D. S. Sutherland, and M. Kall, Nano Lett. 5, 2335 (2005).
[CrossRef]

Dahlin, A. B.

T. Sannomiya, O. Scholder, K. Jefimovs, C. Hafner, and A. B. Dahlin, Small 7, 1653 (2011).
[CrossRef]

A. B. Dahlin, S. Chen, M. P. Jonsson, L. Gunnarsson, M. Kall, and F. Hook, Anal. Chem. 81, 6572 (2009).
[CrossRef]

M. P. Jonsson, A. B. Dahlin, P. Jonsson, and F. Hook, Biointerphases 3, Fd30 (2008).
[CrossRef]

Devaux, E.

S. I. Bozhevolnyi, V. S. Volkov, E. Devaux, and T. W. Ebbesen, Phys. Rev. Lett. 95, 046802 (2005).
[CrossRef]

Ditlbacher, H.

H. Ditlbacher, A. Hohenau, D. Wagner, U. Kreibig, M. Rogers, F. Hofer, F. R. Aussenegg, and J. R. Krenn, Phys. Rev. Lett. 95, 257403 (2005).
[CrossRef]

Ebbesen, T. W.

S. I. Bozhevolnyi, V. S. Volkov, E. Devaux, and T. W. Ebbesen, Phys. Rev. Lett. 95, 046802 (2005).
[CrossRef]

Eisler, H. J.

P. Muhlschlegel, H. J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, Science 308, 1607 (2005).
[CrossRef]

Enejder, A.

A. Enejder, C. Brackmann, and F. Svedberg, IEEE J. Sel. Top. Quantum Electron. 16, 506 (2010).
[CrossRef]

Farrer, R. A.

R. A. Farrer, F. L. Butterfield, V. W. Chen, and J. T. Fourkas, Nano Lett. 5, 1139 (2005).
[CrossRef]

Fourkas, J. T.

R. A. Farrer, F. L. Butterfield, V. W. Chen, and J. T. Fourkas, Nano Lett. 5, 1139 (2005).
[CrossRef]

Gatzogiannis, E.

P. Genevet, J.-P. Tetienne, E. Gatzogiannis, R. Blanchard, M. A. Kats, M. O. Scully, and F. Capasso, Nano Lett. 10, 4880 (2010).
[CrossRef]

Genevet, P.

P. Genevet, J.-P. Tetienne, E. Gatzogiannis, R. Blanchard, M. A. Kats, M. O. Scully, and F. Capasso, Nano Lett. 10, 4880 (2010).
[CrossRef]

Gold, J.

P. Hanarp, D. S. Sutherland, J. Gold, and B. Kasemo, Colloids Surf. A 214, 23 (2003).
[CrossRef]

Gordon, R.

A. Lesuffleur, L. K. S. Kumar, and R. Gordon, Appl. Phys. Lett. 88, 261104 (2006).
[CrossRef]

Gunnarsson, L.

A. B. Dahlin, S. Chen, M. P. Jonsson, L. Gunnarsson, M. Kall, and F. Hook, Anal. Chem. 81, 6572 (2009).
[CrossRef]

Hafner, C.

T. Sannomiya, O. Scholder, K. Jefimovs, C. Hafner, and A. B. Dahlin, Small 7, 1653 (2011).
[CrossRef]

Halas, N. J.

T. H. Park, N. Mirin, J. B. Lassiter, C. L. Nehl, N. J. Halas, and P. Nordlander, ACS Nano 2, 25 (2008).
[CrossRef]

Hanarp, P.

P. Hanarp, D. S. Sutherland, J. Gold, and B. Kasemo, Colloids Surf. A 214, 23 (2003).
[CrossRef]

Hartschuh, A.

A. Bouhelier, M. Beversluis, A. Hartschuh, and L. Novotny, Phys. Rev. Lett. 90, 013903 (2003).
[CrossRef]

Hecht, B.

P. Muhlschlegel, H. J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, Science 308, 1607 (2005).
[CrossRef]

Hofer, F.

H. Ditlbacher, A. Hohenau, D. Wagner, U. Kreibig, M. Rogers, F. Hofer, F. R. Aussenegg, and J. R. Krenn, Phys. Rev. Lett. 95, 257403 (2005).
[CrossRef]

Hohenau, A.

H. Ditlbacher, A. Hohenau, D. Wagner, U. Kreibig, M. Rogers, F. Hofer, F. R. Aussenegg, and J. R. Krenn, Phys. Rev. Lett. 95, 257403 (2005).
[CrossRef]

Hook, F.

A. B. Dahlin, S. Chen, M. P. Jonsson, L. Gunnarsson, M. Kall, and F. Hook, Anal. Chem. 81, 6572 (2009).
[CrossRef]

M. P. Jonsson, A. B. Dahlin, P. Jonsson, and F. Hook, Biointerphases 3, Fd30 (2008).
[CrossRef]

T. Rindzevicius, Y. Alaverdyan, A. Dahlin, F. Hook, D. S. Sutherland, and M. Kall, Nano Lett. 5, 2335 (2005).
[CrossRef]

Jefimovs, K.

T. Sannomiya, O. Scholder, K. Jefimovs, C. Hafner, and A. B. Dahlin, Small 7, 1653 (2011).
[CrossRef]

Jin, J.

S. Kim, J. Jin, Y.-J. Kim, I.-Y. Park, Y. Kim, and S.-W. Kim, Nature 453, 757 (2008).
[CrossRef]

Johansson, P.

J. Alegret, P. Johansson, and M. Kall, New J. Phys. 10, 105004 (2008).
[CrossRef]

Jonsson, M. P.

A. B. Dahlin, S. Chen, M. P. Jonsson, L. Gunnarsson, M. Kall, and F. Hook, Anal. Chem. 81, 6572 (2009).
[CrossRef]

M. P. Jonsson, A. B. Dahlin, P. Jonsson, and F. Hook, Biointerphases 3, Fd30 (2008).
[CrossRef]

Jonsson, P.

M. P. Jonsson, A. B. Dahlin, P. Jonsson, and F. Hook, Biointerphases 3, Fd30 (2008).
[CrossRef]

Kall, M.

A. B. Dahlin, S. Chen, M. P. Jonsson, L. Gunnarsson, M. Kall, and F. Hook, Anal. Chem. 81, 6572 (2009).
[CrossRef]

J. Alegret, P. Johansson, and M. Kall, New J. Phys. 10, 105004 (2008).
[CrossRef]

T. Rindzevicius, Y. Alaverdyan, A. Dahlin, F. Hook, D. S. Sutherland, and M. Kall, Nano Lett. 5, 2335 (2005).
[CrossRef]

Kaminski, C. F.

C. Steuwe, C. F. Kaminski, J. J. Baumberg, and S. Mahajan, Nano Lett. 11, 5339 (2011).
[CrossRef]

Kasemo, B.

P. Hanarp, D. S. Sutherland, J. Gold, and B. Kasemo, Colloids Surf. A 214, 23 (2003).
[CrossRef]

Kats, M. A.

P. Genevet, J.-P. Tetienne, E. Gatzogiannis, R. Blanchard, M. A. Kats, M. O. Scully, and F. Capasso, Nano Lett. 10, 4880 (2010).
[CrossRef]

Kim, H.

H. Kim, D. K. Taggart, C. X. Xiang, R. M. Penner, and E. O. Potma, Nano Lett. 8, 2373 (2008).
[CrossRef]

Kim, S.

S. Kim, J. Jin, Y.-J. Kim, I.-Y. Park, Y. Kim, and S.-W. Kim, Nature 453, 757 (2008).
[CrossRef]

Kim, S.-W.

S. Kim, J. Jin, Y.-J. Kim, I.-Y. Park, Y. Kim, and S.-W. Kim, Nature 453, 757 (2008).
[CrossRef]

Kim, Y.

S. Kim, J. Jin, Y.-J. Kim, I.-Y. Park, Y. Kim, and S.-W. Kim, Nature 453, 757 (2008).
[CrossRef]

Kim, Y.-J.

S. Kim, J. Jin, Y.-J. Kim, I.-Y. Park, Y. Kim, and S.-W. Kim, Nature 453, 757 (2008).
[CrossRef]

Konstantinova, T. V.

Kreibig, U.

H. Ditlbacher, A. Hohenau, D. Wagner, U. Kreibig, M. Rogers, F. Hofer, F. R. Aussenegg, and J. R. Krenn, Phys. Rev. Lett. 95, 257403 (2005).
[CrossRef]

Krenn, J. R.

H. Ditlbacher, A. Hohenau, D. Wagner, U. Kreibig, M. Rogers, F. Hofer, F. R. Aussenegg, and J. R. Krenn, Phys. Rev. Lett. 95, 257403 (2005).
[CrossRef]

Kumar, L. K. S.

A. Lesuffleur, L. K. S. Kumar, and R. Gordon, Appl. Phys. Lett. 88, 261104 (2006).
[CrossRef]

Kuzin, A. A.

Lassiter, J. B.

T. H. Park, N. Mirin, J. B. Lassiter, C. L. Nehl, N. J. Halas, and P. Nordlander, ACS Nano 2, 25 (2008).
[CrossRef]

Lesuffleur, A.

A. Lesuffleur, L. K. S. Kumar, and R. Gordon, Appl. Phys. Lett. 88, 261104 (2006).
[CrossRef]

Lippitz, M.

M. Lippitz, M. A. van Dijk, and M. Orrit, Nano Lett. 5, 799 (2005).
[CrossRef]

Liu, X.

Mahajan, S.

C. Steuwe, C. F. Kaminski, J. J. Baumberg, and S. Mahajan, Nano Lett. 11, 5339 (2011).
[CrossRef]

Martin, O. J. F.

P. Muhlschlegel, H. J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, Science 308, 1607 (2005).
[CrossRef]

McFarland, A. D.

A. D. McFarland and R. P. Van Duyne, Nano Lett. 3, 1057 (2003).
[CrossRef]

Melentiev, P. N.

Mirin, N.

T. H. Park, N. Mirin, J. B. Lassiter, C. L. Nehl, N. J. Halas, and P. Nordlander, ACS Nano 2, 25 (2008).
[CrossRef]

Muhlschlegel, P.

P. Muhlschlegel, H. J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, Science 308, 1607 (2005).
[CrossRef]

Nehl, C. L.

T. H. Park, N. Mirin, J. B. Lassiter, C. L. Nehl, N. J. Halas, and P. Nordlander, ACS Nano 2, 25 (2008).
[CrossRef]

Nordlander, P.

T. H. Park, N. Mirin, J. B. Lassiter, C. L. Nehl, N. J. Halas, and P. Nordlander, ACS Nano 2, 25 (2008).
[CrossRef]

Novotny, L.

J. Renger, R. Quidant, N. van Hulst, S. Palomba, and L. Novotny, Phys. Rev. Lett. 103, 266802 (2009).
[CrossRef]

S. Palomba and L. Novotny, Phys. Rev. Lett. 101, 056802 (2008).
[CrossRef]

A. Bouhelier, M. Beversluis, A. Hartschuh, and L. Novotny, Phys. Rev. Lett. 90, 013903 (2003).
[CrossRef]

Orrit, M.

M. Lippitz, M. A. van Dijk, and M. Orrit, Nano Lett. 5, 799 (2005).
[CrossRef]

Palomba, S.

J. Renger, R. Quidant, N. van Hulst, S. Palomba, and L. Novotny, Phys. Rev. Lett. 103, 266802 (2009).
[CrossRef]

S. Palomba and L. Novotny, Phys. Rev. Lett. 101, 056802 (2008).
[CrossRef]

Park, I.-Y.

S. Kim, J. Jin, Y.-J. Kim, I.-Y. Park, Y. Kim, and S.-W. Kim, Nature 453, 757 (2008).
[CrossRef]

Park, T. H.

T. H. Park, N. Mirin, J. B. Lassiter, C. L. Nehl, N. J. Halas, and P. Nordlander, ACS Nano 2, 25 (2008).
[CrossRef]

Penner, R. M.

H. Kim, D. K. Taggart, C. X. Xiang, R. M. Penner, and E. O. Potma, Nano Lett. 8, 2373 (2008).
[CrossRef]

Pohl, D. W.

P. Muhlschlegel, H. J. Eisler, O. J. F. Martin, B. Hecht, and D. W. Pohl, Science 308, 1607 (2005).
[CrossRef]

Potma, E. O.

X. Liu, Y. Wang, and E. O. Potma, Opt. Lett. 36, 2348 (2011).
[CrossRef]

H. Kim, D. K. Taggart, C. X. Xiang, R. M. Penner, and E. O. Potma, Nano Lett. 8, 2373 (2008).
[CrossRef]

Quidant, R.

J. Renger, R. Quidant, N. van Hulst, S. Palomba, and L. Novotny, Phys. Rev. Lett. 103, 266802 (2009).
[CrossRef]

Renger, J.

J. Renger, R. Quidant, N. van Hulst, S. Palomba, and L. Novotny, Phys. Rev. Lett. 103, 266802 (2009).
[CrossRef]

Rindzevicius, T.

T. Rindzevicius, Y. Alaverdyan, A. Dahlin, F. Hook, D. S. Sutherland, and M. Kall, Nano Lett. 5, 2335 (2005).
[CrossRef]

Rogers, M.

H. Ditlbacher, A. Hohenau, D. Wagner, U. Kreibig, M. Rogers, F. Hofer, F. R. Aussenegg, and J. R. Krenn, Phys. Rev. Lett. 95, 257403 (2005).
[CrossRef]

Sannomiya, T.

T. Sannomiya, O. Scholder, K. Jefimovs, C. Hafner, and A. B. Dahlin, Small 7, 1653 (2011).
[CrossRef]

Scholder, O.

T. Sannomiya, O. Scholder, K. Jefimovs, C. Hafner, and A. B. Dahlin, Small 7, 1653 (2011).
[CrossRef]

Scully, M. O.

P. Genevet, J.-P. Tetienne, E. Gatzogiannis, R. Blanchard, M. A. Kats, M. O. Scully, and F. Capasso, Nano Lett. 10, 4880 (2010).
[CrossRef]

Steuwe, C.

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Figures (3)

Fig. 1.
Fig. 1.

(a) Energy level diagram of the FWM process. (b) Schematic of the excitation geometry. (c) SEM image of a gold film with a high density of holes; diameter here 140 nm.

Fig. 2.
Fig. 2.

Images of thin gold films with nanoholes (λ1=817nm, λ2=1064nm, λFWM=663nm, detection at 663±20nm). FWM signal collected from the low hole-density film (D: 150 nm) in (a) epi and (b) forward. (c) Corresponding MPEL image (epi, excitation only λ1). (d) FWM image of the high-density film shown in Fig. 1 (epi). (e) Spectrum from the high-density gold film in (d). Inset: Output powers versus input powers on log-log scale (blue: Stokes beam, slope=1.05, red: pump/probe, slope=1.96). (f) Intensity profile plots over a single hole [dashed line in (a)]. (g) Lateral and axial profiles of a single hole, indicating the corresponding resolutions (0.3 and 0.9 μm). (h) Lateral profile for two adjacent holes. In (f)–(h), dashed lines are Gaussian fits.

Fig. 3.
Fig. 3.

(a) Extinction spectra for the five hole diameters. Circles indicate the extinction minimum (λHPR). (b) Normalized FWM intensities versus hole diameter for three λ1 (legend: λ1/λFWM). (c) Relation between λHPR and hole diameter. (d) The sets of (λ1, λ2, and λFWM) are plotted at the hole diameter where highest FWM conversion efficiency was obtained. The center wavelength of the HPR and the BW-SPPs are shown as a dashed line and as crosses, respectively. (e) and (f) MPEL emission versus hole diameter, excited by 817 and 883 nm, respectively. For each λ1, the MPEL is measured at two wavelength regions for a series of hole diameters. Dashed line indicated FWM for the same λ1, showing clear similarities between FWM and MPEL in dependence on hole diameter. All results were acquired with the high hole density films.

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