Abstract

The fluorescence of single-colloidal CdSe quantum dots is investigated at room temperature by means of the autocorrelation function over a time scale of almost 12 orders of magnitude. Over a short time scale, the autocorrelation function shows complete antibunching, indicating single-photon emission and atomiclike behavior. Over longer time scales (up to tens of seconds), we measure a bunching effect that is due to fluorescence intermittency and that cannot be described by fluctuations between two states with constant rates. The autocorrelation function also exhibits nonstationary behavior related to power-law distributions of on and off times.

© 2001 Optical Society of America

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  1. D. Bouwmeester, A. Ekert, and A. Zeilinger, The Physics of Quantum Information (Springer-Verlag, Berlin, 2000).
    [CrossRef]
  2. H. J. Kimble, M. Dagenais, and L. Mandel, Phys. Rev. Lett. 39, 691 (1977).
    [CrossRef]
  3. F. Diedrich and H. Walther, Phys. Rev. Lett. 58, 203 (1987).
    [CrossRef] [PubMed]
  4. T. Basche, W. E. Moerner, M. Orrit, and H. Talon, Phys. Rev. Lett. 69, 1516 (1992).
    [CrossRef]
  5. L. Fleury, J. M. Segura, G. Zumofen, B. Hecht, and U. P. Wild, Phys. Rev. Lett. 84, 1148 (2000).
    [CrossRef] [PubMed]
  6. B. Lounis and W. E. Moerner, Nature 407, 491 (2000).
    [CrossRef] [PubMed]
  7. P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, Science 290, 2282 (2000).
    [CrossRef] [PubMed]
  8. C. Santori, M. Pelton, G. Solomon, Y. Dale, and Y. Yamamoto, Phys. Rev. Lett. 86, 1502 (2001).
    [CrossRef] [PubMed]
  9. C. Kurtsiefer, S. Mayer, P. Zarda, and H. Weinfurter, Phys. Rev. Lett. 85, 290 (2000).
    [CrossRef] [PubMed]
  10. R. Brouri, A. Beveratos, J. P. Poizat, and P. Grangier, Opt. Lett. 25, 1294 (2000).
    [CrossRef]
  11. P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and S. K. Buratto, Nature 406, 968 (2000).
    [CrossRef] [PubMed]
  12. B. Lounis, H. A. Bechtel, D. Gerion, A. P. Alivisatos, and W. E. Moerner, Chem. Phys. Lett. 329, 399 (2000).
  13. M. Nirmal, B. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, Nature 383, 802 (1996).
    [CrossRef]
  14. A. L. Efros and M. Rosen, Phys. Rev. Lett. 78, 1110 (1997).
    [CrossRef]
  15. These data, not shown here, will be discussed and analyzed in detail in a forthcoming paper entitled “Lévy flight approach to fluorescence intermittency in semiconductor nanocrystals.”
  16. M. Kuno, D. P. Fromm, H. F. Hamann, A. Gallagher, and D. J. Nesbitt, J. Chem. Phys. 112, 3117 (2000).
  17. J. P. Bouchaud and A. Georges, Phys. Rep.195, 125 (1990).
    [CrossRef]
  18. F. Bardou, J. P. Bouchaud, A. Aspect, and C. Cohen-Tannoudji, Lévy Statistics and Laser Cooling (Cambridge U. Press, Cambridge, 2001).
    [CrossRef]
  19. C. Godreche and J. M. Luck, J. Stat. Phys. 104, 489 (2001).
    [CrossRef]

2001 (2)

C. Santori, M. Pelton, G. Solomon, Y. Dale, and Y. Yamamoto, Phys. Rev. Lett. 86, 1502 (2001).
[CrossRef] [PubMed]

C. Godreche and J. M. Luck, J. Stat. Phys. 104, 489 (2001).
[CrossRef]

2000 (8)

M. Kuno, D. P. Fromm, H. F. Hamann, A. Gallagher, and D. J. Nesbitt, J. Chem. Phys. 112, 3117 (2000).

C. Kurtsiefer, S. Mayer, P. Zarda, and H. Weinfurter, Phys. Rev. Lett. 85, 290 (2000).
[CrossRef] [PubMed]

R. Brouri, A. Beveratos, J. P. Poizat, and P. Grangier, Opt. Lett. 25, 1294 (2000).
[CrossRef]

P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and S. K. Buratto, Nature 406, 968 (2000).
[CrossRef] [PubMed]

B. Lounis, H. A. Bechtel, D. Gerion, A. P. Alivisatos, and W. E. Moerner, Chem. Phys. Lett. 329, 399 (2000).

L. Fleury, J. M. Segura, G. Zumofen, B. Hecht, and U. P. Wild, Phys. Rev. Lett. 84, 1148 (2000).
[CrossRef] [PubMed]

B. Lounis and W. E. Moerner, Nature 407, 491 (2000).
[CrossRef] [PubMed]

P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, Science 290, 2282 (2000).
[CrossRef] [PubMed]

1997 (1)

A. L. Efros and M. Rosen, Phys. Rev. Lett. 78, 1110 (1997).
[CrossRef]

1996 (1)

M. Nirmal, B. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, Nature 383, 802 (1996).
[CrossRef]

1992 (1)

T. Basche, W. E. Moerner, M. Orrit, and H. Talon, Phys. Rev. Lett. 69, 1516 (1992).
[CrossRef]

1987 (1)

F. Diedrich and H. Walther, Phys. Rev. Lett. 58, 203 (1987).
[CrossRef] [PubMed]

1977 (1)

H. J. Kimble, M. Dagenais, and L. Mandel, Phys. Rev. Lett. 39, 691 (1977).
[CrossRef]

Alivisatos, A. P.

B. Lounis, H. A. Bechtel, D. Gerion, A. P. Alivisatos, and W. E. Moerner, Chem. Phys. Lett. 329, 399 (2000).

Aspect, A.

F. Bardou, J. P. Bouchaud, A. Aspect, and C. Cohen-Tannoudji, Lévy Statistics and Laser Cooling (Cambridge U. Press, Cambridge, 2001).
[CrossRef]

Bardou, F.

F. Bardou, J. P. Bouchaud, A. Aspect, and C. Cohen-Tannoudji, Lévy Statistics and Laser Cooling (Cambridge U. Press, Cambridge, 2001).
[CrossRef]

Basche, T.

T. Basche, W. E. Moerner, M. Orrit, and H. Talon, Phys. Rev. Lett. 69, 1516 (1992).
[CrossRef]

Bawendi, M. G.

M. Nirmal, B. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, Nature 383, 802 (1996).
[CrossRef]

Becher, C.

P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, Science 290, 2282 (2000).
[CrossRef] [PubMed]

Bechtel, H. A.

B. Lounis, H. A. Bechtel, D. Gerion, A. P. Alivisatos, and W. E. Moerner, Chem. Phys. Lett. 329, 399 (2000).

Beveratos, A.

Bouchaud, J. P.

F. Bardou, J. P. Bouchaud, A. Aspect, and C. Cohen-Tannoudji, Lévy Statistics and Laser Cooling (Cambridge U. Press, Cambridge, 2001).
[CrossRef]

J. P. Bouchaud and A. Georges, Phys. Rep.195, 125 (1990).
[CrossRef]

Bouwmeester, D.

D. Bouwmeester, A. Ekert, and A. Zeilinger, The Physics of Quantum Information (Springer-Verlag, Berlin, 2000).
[CrossRef]

Brouri, R.

Brus, L. E.

M. Nirmal, B. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, Nature 383, 802 (1996).
[CrossRef]

Buratto, S. K.

P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and S. K. Buratto, Nature 406, 968 (2000).
[CrossRef] [PubMed]

Carson, P. J.

P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and S. K. Buratto, Nature 406, 968 (2000).
[CrossRef] [PubMed]

Cohen-Tannoudji, C.

F. Bardou, J. P. Bouchaud, A. Aspect, and C. Cohen-Tannoudji, Lévy Statistics and Laser Cooling (Cambridge U. Press, Cambridge, 2001).
[CrossRef]

Dabbousi, B.

M. Nirmal, B. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, Nature 383, 802 (1996).
[CrossRef]

Dagenais, M.

H. J. Kimble, M. Dagenais, and L. Mandel, Phys. Rev. Lett. 39, 691 (1977).
[CrossRef]

Dale, Y.

C. Santori, M. Pelton, G. Solomon, Y. Dale, and Y. Yamamoto, Phys. Rev. Lett. 86, 1502 (2001).
[CrossRef] [PubMed]

Diedrich, F.

F. Diedrich and H. Walther, Phys. Rev. Lett. 58, 203 (1987).
[CrossRef] [PubMed]

Efros, A. L.

A. L. Efros and M. Rosen, Phys. Rev. Lett. 78, 1110 (1997).
[CrossRef]

Ekert, A.

D. Bouwmeester, A. Ekert, and A. Zeilinger, The Physics of Quantum Information (Springer-Verlag, Berlin, 2000).
[CrossRef]

Fleury, L.

L. Fleury, J. M. Segura, G. Zumofen, B. Hecht, and U. P. Wild, Phys. Rev. Lett. 84, 1148 (2000).
[CrossRef] [PubMed]

Fromm, D. P.

M. Kuno, D. P. Fromm, H. F. Hamann, A. Gallagher, and D. J. Nesbitt, J. Chem. Phys. 112, 3117 (2000).

Gallagher, A.

M. Kuno, D. P. Fromm, H. F. Hamann, A. Gallagher, and D. J. Nesbitt, J. Chem. Phys. 112, 3117 (2000).

Georges, A.

J. P. Bouchaud and A. Georges, Phys. Rep.195, 125 (1990).
[CrossRef]

Gerion, D.

B. Lounis, H. A. Bechtel, D. Gerion, A. P. Alivisatos, and W. E. Moerner, Chem. Phys. Lett. 329, 399 (2000).

Godreche, C.

C. Godreche and J. M. Luck, J. Stat. Phys. 104, 489 (2001).
[CrossRef]

Grangier, P.

Hamann, H. F.

M. Kuno, D. P. Fromm, H. F. Hamann, A. Gallagher, and D. J. Nesbitt, J. Chem. Phys. 112, 3117 (2000).

Harris, T. D.

M. Nirmal, B. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, Nature 383, 802 (1996).
[CrossRef]

Hecht, B.

L. Fleury, J. M. Segura, G. Zumofen, B. Hecht, and U. P. Wild, Phys. Rev. Lett. 84, 1148 (2000).
[CrossRef] [PubMed]

Hu, E.

P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, Science 290, 2282 (2000).
[CrossRef] [PubMed]

Imamoglu, A.

P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, Science 290, 2282 (2000).
[CrossRef] [PubMed]

P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and S. K. Buratto, Nature 406, 968 (2000).
[CrossRef] [PubMed]

Kimble, H. J.

H. J. Kimble, M. Dagenais, and L. Mandel, Phys. Rev. Lett. 39, 691 (1977).
[CrossRef]

Kiraz, A.

P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, Science 290, 2282 (2000).
[CrossRef] [PubMed]

Kuno, M.

M. Kuno, D. P. Fromm, H. F. Hamann, A. Gallagher, and D. J. Nesbitt, J. Chem. Phys. 112, 3117 (2000).

Kurtsiefer, C.

C. Kurtsiefer, S. Mayer, P. Zarda, and H. Weinfurter, Phys. Rev. Lett. 85, 290 (2000).
[CrossRef] [PubMed]

Lounis, B.

B. Lounis and W. E. Moerner, Nature 407, 491 (2000).
[CrossRef] [PubMed]

B. Lounis, H. A. Bechtel, D. Gerion, A. P. Alivisatos, and W. E. Moerner, Chem. Phys. Lett. 329, 399 (2000).

Luck, J. M.

C. Godreche and J. M. Luck, J. Stat. Phys. 104, 489 (2001).
[CrossRef]

Macklin, J. J.

M. Nirmal, B. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, Nature 383, 802 (1996).
[CrossRef]

Mandel, L.

H. J. Kimble, M. Dagenais, and L. Mandel, Phys. Rev. Lett. 39, 691 (1977).
[CrossRef]

Mason, M. D.

P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and S. K. Buratto, Nature 406, 968 (2000).
[CrossRef] [PubMed]

Mayer, S.

C. Kurtsiefer, S. Mayer, P. Zarda, and H. Weinfurter, Phys. Rev. Lett. 85, 290 (2000).
[CrossRef] [PubMed]

Michler, P.

P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, Science 290, 2282 (2000).
[CrossRef] [PubMed]

P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and S. K. Buratto, Nature 406, 968 (2000).
[CrossRef] [PubMed]

Moerner, W. E.

B. Lounis, H. A. Bechtel, D. Gerion, A. P. Alivisatos, and W. E. Moerner, Chem. Phys. Lett. 329, 399 (2000).

B. Lounis and W. E. Moerner, Nature 407, 491 (2000).
[CrossRef] [PubMed]

T. Basche, W. E. Moerner, M. Orrit, and H. Talon, Phys. Rev. Lett. 69, 1516 (1992).
[CrossRef]

Nesbitt, D. J.

M. Kuno, D. P. Fromm, H. F. Hamann, A. Gallagher, and D. J. Nesbitt, J. Chem. Phys. 112, 3117 (2000).

Nirmal, M.

M. Nirmal, B. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, Nature 383, 802 (1996).
[CrossRef]

Orrit, M.

T. Basche, W. E. Moerner, M. Orrit, and H. Talon, Phys. Rev. Lett. 69, 1516 (1992).
[CrossRef]

Pelton, M.

C. Santori, M. Pelton, G. Solomon, Y. Dale, and Y. Yamamoto, Phys. Rev. Lett. 86, 1502 (2001).
[CrossRef] [PubMed]

Petroff, P. M.

P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, Science 290, 2282 (2000).
[CrossRef] [PubMed]

Poizat, J. P.

Rosen, M.

A. L. Efros and M. Rosen, Phys. Rev. Lett. 78, 1110 (1997).
[CrossRef]

Santori, C.

C. Santori, M. Pelton, G. Solomon, Y. Dale, and Y. Yamamoto, Phys. Rev. Lett. 86, 1502 (2001).
[CrossRef] [PubMed]

Schoenfeld, W. V.

P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, Science 290, 2282 (2000).
[CrossRef] [PubMed]

Segura, J. M.

L. Fleury, J. M. Segura, G. Zumofen, B. Hecht, and U. P. Wild, Phys. Rev. Lett. 84, 1148 (2000).
[CrossRef] [PubMed]

Solomon, G.

C. Santori, M. Pelton, G. Solomon, Y. Dale, and Y. Yamamoto, Phys. Rev. Lett. 86, 1502 (2001).
[CrossRef] [PubMed]

Strouse, G. F.

P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and S. K. Buratto, Nature 406, 968 (2000).
[CrossRef] [PubMed]

Talon, H.

T. Basche, W. E. Moerner, M. Orrit, and H. Talon, Phys. Rev. Lett. 69, 1516 (1992).
[CrossRef]

Trautman, J. K.

M. Nirmal, B. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, Nature 383, 802 (1996).
[CrossRef]

Walther, H.

F. Diedrich and H. Walther, Phys. Rev. Lett. 58, 203 (1987).
[CrossRef] [PubMed]

Weinfurter, H.

C. Kurtsiefer, S. Mayer, P. Zarda, and H. Weinfurter, Phys. Rev. Lett. 85, 290 (2000).
[CrossRef] [PubMed]

Wild, U. P.

L. Fleury, J. M. Segura, G. Zumofen, B. Hecht, and U. P. Wild, Phys. Rev. Lett. 84, 1148 (2000).
[CrossRef] [PubMed]

Yamamoto, Y.

C. Santori, M. Pelton, G. Solomon, Y. Dale, and Y. Yamamoto, Phys. Rev. Lett. 86, 1502 (2001).
[CrossRef] [PubMed]

Zarda, P.

C. Kurtsiefer, S. Mayer, P. Zarda, and H. Weinfurter, Phys. Rev. Lett. 85, 290 (2000).
[CrossRef] [PubMed]

Zeilinger, A.

D. Bouwmeester, A. Ekert, and A. Zeilinger, The Physics of Quantum Information (Springer-Verlag, Berlin, 2000).
[CrossRef]

Zhang, L.

P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, Science 290, 2282 (2000).
[CrossRef] [PubMed]

Zumofen, G.

L. Fleury, J. M. Segura, G. Zumofen, B. Hecht, and U. P. Wild, Phys. Rev. Lett. 84, 1148 (2000).
[CrossRef] [PubMed]

Chem. Phys. Lett. (1)

B. Lounis, H. A. Bechtel, D. Gerion, A. P. Alivisatos, and W. E. Moerner, Chem. Phys. Lett. 329, 399 (2000).

J. Chem. Phys. (1)

M. Kuno, D. P. Fromm, H. F. Hamann, A. Gallagher, and D. J. Nesbitt, J. Chem. Phys. 112, 3117 (2000).

J. Stat. Phys. (1)

C. Godreche and J. M. Luck, J. Stat. Phys. 104, 489 (2001).
[CrossRef]

Nature (3)

P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and S. K. Buratto, Nature 406, 968 (2000).
[CrossRef] [PubMed]

M. Nirmal, B. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, Nature 383, 802 (1996).
[CrossRef]

B. Lounis and W. E. Moerner, Nature 407, 491 (2000).
[CrossRef] [PubMed]

Opt. Lett. (1)

Phys. Rev. Lett. (7)

C. Santori, M. Pelton, G. Solomon, Y. Dale, and Y. Yamamoto, Phys. Rev. Lett. 86, 1502 (2001).
[CrossRef] [PubMed]

C. Kurtsiefer, S. Mayer, P. Zarda, and H. Weinfurter, Phys. Rev. Lett. 85, 290 (2000).
[CrossRef] [PubMed]

H. J. Kimble, M. Dagenais, and L. Mandel, Phys. Rev. Lett. 39, 691 (1977).
[CrossRef]

F. Diedrich and H. Walther, Phys. Rev. Lett. 58, 203 (1987).
[CrossRef] [PubMed]

T. Basche, W. E. Moerner, M. Orrit, and H. Talon, Phys. Rev. Lett. 69, 1516 (1992).
[CrossRef]

L. Fleury, J. M. Segura, G. Zumofen, B. Hecht, and U. P. Wild, Phys. Rev. Lett. 84, 1148 (2000).
[CrossRef] [PubMed]

A. L. Efros and M. Rosen, Phys. Rev. Lett. 78, 1110 (1997).
[CrossRef]

Science (1)

P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, Science 290, 2282 (2000).
[CrossRef] [PubMed]

Other (4)

These data, not shown here, will be discussed and analyzed in detail in a forthcoming paper entitled “Lévy flight approach to fluorescence intermittency in semiconductor nanocrystals.”

D. Bouwmeester, A. Ekert, and A. Zeilinger, The Physics of Quantum Information (Springer-Verlag, Berlin, 2000).
[CrossRef]

J. P. Bouchaud and A. Georges, Phys. Rep.195, 125 (1990).
[CrossRef]

F. Bardou, J. P. Bouchaud, A. Aspect, and C. Cohen-Tannoudji, Lévy Statistics and Laser Cooling (Cambridge U. Press, Cambridge, 2001).
[CrossRef]

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Figures (3)

Fig. 1
Fig. 1

Histograms of coincidence counts obtained from the PTA (time resolution, 600  ps) and corrected from the time delay. The solid curve is a fit by an exponential curve a1-bexp-τ/τ0, with a=577.5, b=0.95, and τ0=20.1 ns.

Fig. 2
Fig. 2

Normalized ACF from 1  ns to 100  s, measured by the PTA and the Malvern correlator (T=900 s, I=2 kW/cm2, anorm=1.4).

Fig. 3
Fig. 3

(a) Time trace of the fluorescence intensity for a single QD (excitation intensity, 0.25 kW/cm2). (b) Computations of the ACF for this trace. Curves (1), (2), and (3) correspond to time intervals of 18, 180, and 1800  s.

Equations (1)

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g2t,t+τ=ItIt+τItIt+τ,

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