Abstract

By detecting the transient four-wave mixing from gold nanoparticles in resonance with their surface plasmon, we demonstrate a multiphoton imaging modality suited for cell microscopy. Four-wave mixing is measured free from background using a three-beam excitation geometry and heterodyne detection. We achieve a spatial resolution of 140nm in-plane and 470nm in the axial direction, surpassing the one-photon diffraction limit. With this technique, high-contrast photostable imaging of Golgi structures is demonstrated in HepG2 cells labeled with gold nanoparticles of 10nm and 5nm diameter.

© 2009 Optical Society of America

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  1. H. Wang, T. B. Huff, D. A. Zweifel, W. He, P. S. Low, A. Wei, and J.-X. Cheng, Proc. Natl. Acad. Sci. USA 102, 15752 (2005).
    [CrossRef] [PubMed]
  2. D. Boyer, P. Tamarat, A. Maali, B. Lounis, and M. Orrit, Science 297, 1160 (2002).
    [CrossRef] [PubMed]
  3. M. A. van Dijk, A. L. Tchebotareva, M. Orrit, M. Lippitz, S. Berciaud, D. Lasne, L. Cognet, and B. Lounis, Phys. Chem. Chem. Phys. 8, 3486 (2006).
    [CrossRef] [PubMed]
  4. D. Lasne, G. A. Blab, F. D. Giorgi, F. Ichas, B. Lounis, and L. Cognet, Opt. Express 15, 14184 (2007), and references therein.
    [CrossRef] [PubMed]
  5. P. Borri, W. Langbein, S. Schneider, U. Woggon, R. L. Sellin, D. Ouyang, and D. Bimberg, Phys. Rev. Lett. 87, 157401 (2001).
    [CrossRef] [PubMed]
  6. P. Borri and W. Langbein, J. Phys. Condens. Matter 19, 295201 (2007).
    [CrossRef] [PubMed]
  7. F. Masia, W. Langbein, and P. Borri, Appl. Phys. Lett. 93, 021114 (2008).
    [CrossRef]
  8. F. Masia, W. Langbein, and P. Borri, Phys. Status Solidi C 6, 916 (2009).
    [CrossRef]

2009 (1)

F. Masia, W. Langbein, and P. Borri, Phys. Status Solidi C 6, 916 (2009).
[CrossRef]

2008 (1)

F. Masia, W. Langbein, and P. Borri, Appl. Phys. Lett. 93, 021114 (2008).
[CrossRef]

2007 (2)

2006 (1)

M. A. van Dijk, A. L. Tchebotareva, M. Orrit, M. Lippitz, S. Berciaud, D. Lasne, L. Cognet, and B. Lounis, Phys. Chem. Chem. Phys. 8, 3486 (2006).
[CrossRef] [PubMed]

2005 (1)

H. Wang, T. B. Huff, D. A. Zweifel, W. He, P. S. Low, A. Wei, and J.-X. Cheng, Proc. Natl. Acad. Sci. USA 102, 15752 (2005).
[CrossRef] [PubMed]

2002 (1)

D. Boyer, P. Tamarat, A. Maali, B. Lounis, and M. Orrit, Science 297, 1160 (2002).
[CrossRef] [PubMed]

2001 (1)

P. Borri, W. Langbein, S. Schneider, U. Woggon, R. L. Sellin, D. Ouyang, and D. Bimberg, Phys. Rev. Lett. 87, 157401 (2001).
[CrossRef] [PubMed]

Berciaud, S.

M. A. van Dijk, A. L. Tchebotareva, M. Orrit, M. Lippitz, S. Berciaud, D. Lasne, L. Cognet, and B. Lounis, Phys. Chem. Chem. Phys. 8, 3486 (2006).
[CrossRef] [PubMed]

Bimberg, D.

P. Borri, W. Langbein, S. Schneider, U. Woggon, R. L. Sellin, D. Ouyang, and D. Bimberg, Phys. Rev. Lett. 87, 157401 (2001).
[CrossRef] [PubMed]

Blab, G. A.

Borri, P.

F. Masia, W. Langbein, and P. Borri, Phys. Status Solidi C 6, 916 (2009).
[CrossRef]

F. Masia, W. Langbein, and P. Borri, Appl. Phys. Lett. 93, 021114 (2008).
[CrossRef]

P. Borri and W. Langbein, J. Phys. Condens. Matter 19, 295201 (2007).
[CrossRef] [PubMed]

P. Borri, W. Langbein, S. Schneider, U. Woggon, R. L. Sellin, D. Ouyang, and D. Bimberg, Phys. Rev. Lett. 87, 157401 (2001).
[CrossRef] [PubMed]

Boyer, D.

D. Boyer, P. Tamarat, A. Maali, B. Lounis, and M. Orrit, Science 297, 1160 (2002).
[CrossRef] [PubMed]

Cheng, J.-X.

H. Wang, T. B. Huff, D. A. Zweifel, W. He, P. S. Low, A. Wei, and J.-X. Cheng, Proc. Natl. Acad. Sci. USA 102, 15752 (2005).
[CrossRef] [PubMed]

Cognet, L.

D. Lasne, G. A. Blab, F. D. Giorgi, F. Ichas, B. Lounis, and L. Cognet, Opt. Express 15, 14184 (2007), and references therein.
[CrossRef] [PubMed]

M. A. van Dijk, A. L. Tchebotareva, M. Orrit, M. Lippitz, S. Berciaud, D. Lasne, L. Cognet, and B. Lounis, Phys. Chem. Chem. Phys. 8, 3486 (2006).
[CrossRef] [PubMed]

Giorgi, F. D.

He, W.

H. Wang, T. B. Huff, D. A. Zweifel, W. He, P. S. Low, A. Wei, and J.-X. Cheng, Proc. Natl. Acad. Sci. USA 102, 15752 (2005).
[CrossRef] [PubMed]

Huff, T. B.

H. Wang, T. B. Huff, D. A. Zweifel, W. He, P. S. Low, A. Wei, and J.-X. Cheng, Proc. Natl. Acad. Sci. USA 102, 15752 (2005).
[CrossRef] [PubMed]

Ichas, F.

Langbein, W.

F. Masia, W. Langbein, and P. Borri, Phys. Status Solidi C 6, 916 (2009).
[CrossRef]

F. Masia, W. Langbein, and P. Borri, Appl. Phys. Lett. 93, 021114 (2008).
[CrossRef]

P. Borri and W. Langbein, J. Phys. Condens. Matter 19, 295201 (2007).
[CrossRef] [PubMed]

P. Borri, W. Langbein, S. Schneider, U. Woggon, R. L. Sellin, D. Ouyang, and D. Bimberg, Phys. Rev. Lett. 87, 157401 (2001).
[CrossRef] [PubMed]

Lasne, D.

D. Lasne, G. A. Blab, F. D. Giorgi, F. Ichas, B. Lounis, and L. Cognet, Opt. Express 15, 14184 (2007), and references therein.
[CrossRef] [PubMed]

M. A. van Dijk, A. L. Tchebotareva, M. Orrit, M. Lippitz, S. Berciaud, D. Lasne, L. Cognet, and B. Lounis, Phys. Chem. Chem. Phys. 8, 3486 (2006).
[CrossRef] [PubMed]

Lippitz, M.

M. A. van Dijk, A. L. Tchebotareva, M. Orrit, M. Lippitz, S. Berciaud, D. Lasne, L. Cognet, and B. Lounis, Phys. Chem. Chem. Phys. 8, 3486 (2006).
[CrossRef] [PubMed]

Lounis, B.

D. Lasne, G. A. Blab, F. D. Giorgi, F. Ichas, B. Lounis, and L. Cognet, Opt. Express 15, 14184 (2007), and references therein.
[CrossRef] [PubMed]

M. A. van Dijk, A. L. Tchebotareva, M. Orrit, M. Lippitz, S. Berciaud, D. Lasne, L. Cognet, and B. Lounis, Phys. Chem. Chem. Phys. 8, 3486 (2006).
[CrossRef] [PubMed]

D. Boyer, P. Tamarat, A. Maali, B. Lounis, and M. Orrit, Science 297, 1160 (2002).
[CrossRef] [PubMed]

Low, P. S.

H. Wang, T. B. Huff, D. A. Zweifel, W. He, P. S. Low, A. Wei, and J.-X. Cheng, Proc. Natl. Acad. Sci. USA 102, 15752 (2005).
[CrossRef] [PubMed]

Maali, A.

D. Boyer, P. Tamarat, A. Maali, B. Lounis, and M. Orrit, Science 297, 1160 (2002).
[CrossRef] [PubMed]

Masia, F.

F. Masia, W. Langbein, and P. Borri, Phys. Status Solidi C 6, 916 (2009).
[CrossRef]

F. Masia, W. Langbein, and P. Borri, Appl. Phys. Lett. 93, 021114 (2008).
[CrossRef]

Orrit, M.

M. A. van Dijk, A. L. Tchebotareva, M. Orrit, M. Lippitz, S. Berciaud, D. Lasne, L. Cognet, and B. Lounis, Phys. Chem. Chem. Phys. 8, 3486 (2006).
[CrossRef] [PubMed]

D. Boyer, P. Tamarat, A. Maali, B. Lounis, and M. Orrit, Science 297, 1160 (2002).
[CrossRef] [PubMed]

Ouyang, D.

P. Borri, W. Langbein, S. Schneider, U. Woggon, R. L. Sellin, D. Ouyang, and D. Bimberg, Phys. Rev. Lett. 87, 157401 (2001).
[CrossRef] [PubMed]

Schneider, S.

P. Borri, W. Langbein, S. Schneider, U. Woggon, R. L. Sellin, D. Ouyang, and D. Bimberg, Phys. Rev. Lett. 87, 157401 (2001).
[CrossRef] [PubMed]

Sellin, R. L.

P. Borri, W. Langbein, S. Schneider, U. Woggon, R. L. Sellin, D. Ouyang, and D. Bimberg, Phys. Rev. Lett. 87, 157401 (2001).
[CrossRef] [PubMed]

Tamarat, P.

D. Boyer, P. Tamarat, A. Maali, B. Lounis, and M. Orrit, Science 297, 1160 (2002).
[CrossRef] [PubMed]

Tchebotareva, A. L.

M. A. van Dijk, A. L. Tchebotareva, M. Orrit, M. Lippitz, S. Berciaud, D. Lasne, L. Cognet, and B. Lounis, Phys. Chem. Chem. Phys. 8, 3486 (2006).
[CrossRef] [PubMed]

van Dijk, M. A.

M. A. van Dijk, A. L. Tchebotareva, M. Orrit, M. Lippitz, S. Berciaud, D. Lasne, L. Cognet, and B. Lounis, Phys. Chem. Chem. Phys. 8, 3486 (2006).
[CrossRef] [PubMed]

Wang, H.

H. Wang, T. B. Huff, D. A. Zweifel, W. He, P. S. Low, A. Wei, and J.-X. Cheng, Proc. Natl. Acad. Sci. USA 102, 15752 (2005).
[CrossRef] [PubMed]

Wei, A.

H. Wang, T. B. Huff, D. A. Zweifel, W. He, P. S. Low, A. Wei, and J.-X. Cheng, Proc. Natl. Acad. Sci. USA 102, 15752 (2005).
[CrossRef] [PubMed]

Woggon, U.

P. Borri, W. Langbein, S. Schneider, U. Woggon, R. L. Sellin, D. Ouyang, and D. Bimberg, Phys. Rev. Lett. 87, 157401 (2001).
[CrossRef] [PubMed]

Zweifel, D. A.

H. Wang, T. B. Huff, D. A. Zweifel, W. He, P. S. Low, A. Wei, and J.-X. Cheng, Proc. Natl. Acad. Sci. USA 102, 15752 (2005).
[CrossRef] [PubMed]

Appl. Phys. Lett. (1)

F. Masia, W. Langbein, and P. Borri, Appl. Phys. Lett. 93, 021114 (2008).
[CrossRef]

J. Phys. Condens. Matter (1)

P. Borri and W. Langbein, J. Phys. Condens. Matter 19, 295201 (2007).
[CrossRef] [PubMed]

Opt. Express (1)

Phys. Chem. Chem. Phys. (1)

M. A. van Dijk, A. L. Tchebotareva, M. Orrit, M. Lippitz, S. Berciaud, D. Lasne, L. Cognet, and B. Lounis, Phys. Chem. Chem. Phys. 8, 3486 (2006).
[CrossRef] [PubMed]

Phys. Rev. Lett. (1)

P. Borri, W. Langbein, S. Schneider, U. Woggon, R. L. Sellin, D. Ouyang, and D. Bimberg, Phys. Rev. Lett. 87, 157401 (2001).
[CrossRef] [PubMed]

Phys. Status Solidi C (1)

F. Masia, W. Langbein, and P. Borri, Phys. Status Solidi C 6, 916 (2009).
[CrossRef]

Proc. Natl. Acad. Sci. USA (1)

H. Wang, T. B. Huff, D. A. Zweifel, W. He, P. S. Low, A. Wei, and J.-X. Cheng, Proc. Natl. Acad. Sci. USA 102, 15752 (2005).
[CrossRef] [PubMed]

Science (1)

D. Boyer, P. Tamarat, A. Maali, B. Lounis, and M. Orrit, Science 297, 1160 (2002).
[CrossRef] [PubMed]

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Figures (3)

Fig. 1
Fig. 1

Sketch of the experimental setup. AOM, acousto-optic modulator; λ 2 , wave plate; Pol. polarizer; xyz, piezoelectric scanning stage; BS, 50:50 beam splitter; MO, microscope objective; BPD, balanced photodiodes.

Fig. 2
Fig. 2

FWM of a single GNP of 20 nm diameter. (a) FWM amplitude normalized to the excitation fields as a function of the total excitation intensity. (b) Axial ( x z ) scan indicating the spatial resolution (point spread function) of the FWM imaging. Solid curves are intensity profiles from which a lateral (axial) resolution of 140 nm ( 470 nm ) FWHM is measured.

Fig. 3
Fig. 3

Images of HepG2 cells having the Golgi apparatus immunostained with GM130-Alexa488 fluorophores and GNPs of 10 nm [(a), (b)] and 5 nm [(c)–(e)] diameter. Scale bars are given. (a), (c) Overlay of phase-contrast microscopy and epifluorescence. Equal scale. (b), (d), FWM intensity of the Golgi region indicated by the white dashed squares in (a) and (c), respectively. Pixel size 50 × 50 nm 2 , time/pixel 30 ms . (e) y z section (axial scan) FWM intensity at x indicated by the dashed line in part (d). Dashed line indicates z of part (d). Equal scale as (d).

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