Abstract

In single particle spectroscopy, the degree of observed fluorescence anti-bunching in a second-order cross correlation experiment is indicative of its bi-exciton quantum yield and whether or not a particle is well isolated. Advances in quantum dot synthesis have produced single particles with bi-exciton quantum yields approaching unity. Consequently, this creates uncertainty as to whether a particle has a high bi-exciton quantum yield or if it exists as a cluster. We report on a time-gated anti-bunching technique capable of determining the relative contributions of both multi-exciton emission and clustering effects. In this way, we can now unambiguously determine if a particle is single. Additionally, this time-gated anti-bunching approach provides an accurate way for the determination of bi-exciton lifetime with minimal contribution from higher order multi-exciton states.

© 2013 OSA

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    [CrossRef] [PubMed]
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  22. R. D. Schaller and V. I. Klimov, “High efficiency carrier multiplication in PbSe nanocrystals: Implications for solar energy conversion,” Phys. Rev. Lett.92(18), 186601 (2004).
    [CrossRef] [PubMed]
  23. A. Muller, W. Fang, J. Lawall, and G. S. Solomon, “Creating polarization-entangled photon pairs from a semiconductor quantum dot using the optical Stark effect,” Phys. Rev. Lett.103(21), 217402 (2009).
    [CrossRef] [PubMed]
  24. R. M. Stevenson, R. J. Young, P. Atkinson, K. Cooper, D. A. Ritchie, and A. J. Shields, “A semiconductor source of triggered entangled photon pairs,” Nature439(7073), 179–182 (2006).
    [CrossRef] [PubMed]
  25. M. Nirmal, B. O. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, “Fluorescence intermittency in single cadmium selenide nanocrystals,” Nature383(6603), 802–804 (1996).
    [CrossRef]
  26. M. Kuno, D. P. Fromm, H. F. Hamann, A. Gallagher, and D. J. Nesbitt, “Nonexponential “blinking” kinetics of single CdSe quantum dots: A universal power law behavior,” J. Chem. Phys.112(7), 3117–3120 (2000).
    [CrossRef]
  27. C. Galland, Y. Ghosh, A. Steinbrück, M. Sykora, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots,” Nature479(7372), 203–207 (2011).
    [CrossRef] [PubMed]
  28. S. Jander, A. Kornowski, and H. Weller, “Energy transfer from CdSe/CdS nanorods to amorphous carbon,” Nano Lett.11(12), 5179–5183 (2011).
    [CrossRef] [PubMed]
  29. J. Zhao, G. Nair, B. R. Fisher, and M. G. Bawendi, “Challenge to the charging model of semiconductor-nanocrystal fluorescence intermittency from off-state quantum yields and multiexciton blinking,” Phys. Rev. Lett.104(15), 157403 (2010).
    [CrossRef] [PubMed]
  30. Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, ““Giant” multishell CdSe nanocrystal quantum dots with suppressed blinking,” J. Am. Chem. Soc.130(15), 5026–5027 (2008).
    [CrossRef] [PubMed]
  31. V. I. Klimov, A. A. Mikhailovsky, D. W. McBranch, C. A. Leatherdale, and M. G. Bawendi, “Quantization of multiparticle Auger rates in semiconductor quantum dots,” Science287(5455), 1011–1013 (2000).
    [CrossRef] [PubMed]
  32. F. García-Santamaría, Y. Chen, J. Vela, R. D. Schaller, J. A. Hollingsworth, and V. I. Klimov, “Suppressed Auger recombination in “giant” nanocrystals boosts optical gain performance,” Nano Lett.9(10), 3482–3488 (2009).
    [CrossRef] [PubMed]
  33. D. Canneson, I. Mallek-Zouari, S. Buil, X. Quelin, C. Javaux, B. Dubertret, and J.-P. Hermier, “Enhancing the fluorescence of individual thick shell CdSe/CdS Nanocrystals by coupling to gold structures,” New J. Phys.14(6), 063035 (2012).
    [CrossRef]
  34. Due to very high QBX, then second g-NQD shows a bi-exponential decay even at very low pump power. The fast time constant of the PL decay 23.78 ns is in good agreement with 22.9ns τBX extracted from the decay of RTG.”
  35. Y. Ghosh, B. D. Mangum, J. L. Casson, D. J. Williams, H. Htoon, and J. A. Hollingsworth, “New insights into the complexities of shell growth and the strong influence of particle volume in nonblinking “giant” core/shell nanocrystal quantum dots,” J. Am. Chem. Soc.134(23), 9634–9643 (2012).
    [CrossRef] [PubMed]

2012 (2)

D. Canneson, I. Mallek-Zouari, S. Buil, X. Quelin, C. Javaux, B. Dubertret, and J.-P. Hermier, “Enhancing the fluorescence of individual thick shell CdSe/CdS Nanocrystals by coupling to gold structures,” New J. Phys.14(6), 063035 (2012).
[CrossRef]

Y. Ghosh, B. D. Mangum, J. L. Casson, D. J. Williams, H. Htoon, and J. A. Hollingsworth, “New insights into the complexities of shell growth and the strong influence of particle volume in nonblinking “giant” core/shell nanocrystal quantum dots,” J. Am. Chem. Soc.134(23), 9634–9643 (2012).
[CrossRef] [PubMed]

2011 (5)

G. Nair, J. Zhao, and M. G. Bawendi, “Biexciton quantum yield of single semiconductor nanocrystals from photon statistics,” Nano Lett.11(3), 1136–1140 (2011).
[CrossRef] [PubMed]

Y. S. Park, A. V. Malko, J. Vela, Y. Chen, Y. Ghosh, F. García-Santamaría, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Near-unity quantum yields of biexciton emission from CdSe/CdS nanocrystals measured using single-particle spectroscopy,” Phys. Rev. Lett.106(18), 187401 (2011).
[CrossRef] [PubMed]

Y. Louyer, L. Biadala, J. B. Trebbia, M. J. Fernée, P. Tamarat, and B. Lounis, “Efficient biexciton emission in elongated CdSe/ZnS nanocrystals,” Nano Lett.11(10), 4370–4375 (2011).
[CrossRef] [PubMed]

C. Galland, Y. Ghosh, A. Steinbrück, M. Sykora, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots,” Nature479(7372), 203–207 (2011).
[CrossRef] [PubMed]

S. Jander, A. Kornowski, and H. Weller, “Energy transfer from CdSe/CdS nanorods to amorphous carbon,” Nano Lett.11(12), 5179–5183 (2011).
[CrossRef] [PubMed]

2010 (1)

J. Zhao, G. Nair, B. R. Fisher, and M. G. Bawendi, “Challenge to the charging model of semiconductor-nanocrystal fluorescence intermittency from off-state quantum yields and multiexciton blinking,” Phys. Rev. Lett.104(15), 157403 (2010).
[CrossRef] [PubMed]

2009 (3)

A. Muller, W. Fang, J. Lawall, and G. S. Solomon, “Creating polarization-entangled photon pairs from a semiconductor quantum dot using the optical Stark effect,” Phys. Rev. Lett.103(21), 217402 (2009).
[CrossRef] [PubMed]

R. Osovsky, D. Cheskis, V. Kloper, A. Sashchiuk, M. Kroner, and E. Lifshitz, “Continuous-wave pumping of multiexciton bands in the photoluminescence spectrum of a single CdTe-CdSe core-shell colloidal quantum dot,” Phys. Rev. Lett.102(19), 197401 (2009).
[CrossRef] [PubMed]

F. García-Santamaría, Y. Chen, J. Vela, R. D. Schaller, J. A. Hollingsworth, and V. I. Klimov, “Suppressed Auger recombination in “giant” nanocrystals boosts optical gain performance,” Nano Lett.9(10), 3482–3488 (2009).
[CrossRef] [PubMed]

2008 (2)

A. Högele, C. Galland, M. Winger, and A. Imamoğlu, “Photon antibunching in the photoluminescence spectra of a single carbon nanotube,” Phys. Rev. Lett.100(21), 217401 (2008).
[CrossRef] [PubMed]

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, ““Giant” multishell CdSe nanocrystal quantum dots with suppressed blinking,” J. Am. Chem. Soc.130(15), 5026–5027 (2008).
[CrossRef] [PubMed]

2006 (2)

R. M. Stevenson, R. J. Young, P. Atkinson, K. Cooper, D. A. Ritchie, and A. J. Shields, “A semiconductor source of triggered entangled photon pairs,” Nature439(7073), 179–182 (2006).
[CrossRef] [PubMed]

A. Shabaev, A. L. Efros, and A. J. Nozik, “Multiexciton generation by a single photon in nanocrystals,” Nano Lett.6(12), 2856–2863 (2006).
[CrossRef] [PubMed]

2005 (1)

B. Fisher, J. M. Caruge, D. Zehnder, and M. Bawendi, “Room-temperature ordered photon emission from multiexciton states in single CdSe core-shell nanocrystals,” Phys. Rev. Lett.94(8), 087403 (2005).
[CrossRef] [PubMed]

2004 (1)

R. D. Schaller and V. I. Klimov, “High efficiency carrier multiplication in PbSe nanocrystals: Implications for solar energy conversion,” Phys. Rev. Lett.92(18), 186601 (2004).
[CrossRef] [PubMed]

2002 (1)

K. D. Weston, M. Dyck, P. Tinnefeld, C. Müller, D. P. Herten, and M. Sauer, “Measuring the number of independent emitters in single-molecule fluorescence images and trajectories using coincident photons,” Anal. Chem.74(20), 5342–5349 (2002).
[CrossRef] [PubMed]

2001 (4)

P. Tinnefeld, C. Müller, and M. Sauer, “Time-varying photon probability distribution of individual molecules at room temperature,” Chem. Phys. Lett.345(3-4), 252–258 (2001).
[CrossRef]

E. Moreau, I. Robert, L. Manin, V. Thierry-Mieg, J. M. Gérard, and I. Abram, “Quantum cascade of photons in semiconductor quantum dots,” Phys. Rev. Lett.87(18), 183601 (2001).
[CrossRef]

F. Treussart, A. Clouqueur, C. Grossman, and J.-F. Roch, “Photon antibunching in the fluorescence of a single dye molecule embedded in a thin polymer film,” Opt. Lett.26(19), 1504–1506 (2001).
[CrossRef] [PubMed]

A. Beveratos, R. Brouri, T. Gacoin, J.-P. Poizat, and P. Grangier, “Nonclassical radiation from diamond nanocrystals,” Phys. Rev. A64(6), 061802 (2001).
[CrossRef]

2000 (9)

R. Brouri, A. Beveratos, J.-P. Poizat, and P. Grangier, “Photon antibunching in the fluorescence of individual color centers in diamond,” Opt. Lett.25(17), 1294–1296 (2000).
[CrossRef] [PubMed]

M. Kuno, D. P. Fromm, H. F. Hamann, A. Gallagher, and D. J. Nesbitt, “Nonexponential “blinking” kinetics of single CdSe quantum dots: A universal power law behavior,” J. Chem. Phys.112(7), 3117–3120 (2000).
[CrossRef]

C. Kurtsiefer, S. Mayer, P. Zarda, and H. Weinfurter, “Stable solid-state source of single photons,” Phys. Rev. Lett.85(2), 290–293 (2000).
[CrossRef] [PubMed]

B. Lounis and W. E. Moerner, “Single photons on demand from a single molecule at room temperature,” Nature407(6803), 491–493 (2000).
[CrossRef] [PubMed]

P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, “A quantum dot single-photon turnstile device,” Science290(5500), 2282–2285 (2000).
[CrossRef] [PubMed]

P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and S. K. Buratto, “Quantum correlation among photons from a single quantum dot at room temperature,” Nature406(6799), 968–970 (2000).
[CrossRef] [PubMed]

E. Dekel, D. V. Regelman, D. Gershoni, E. Ehrenfreund, W. V. Schoenfeld, and P. M. Petroff, “Cascade evolution and radiative recombination of quantum dot multiexcitons studied by time-resolved spectroscopy,” Phys. Rev. B62(16), 11038–11045 (2000).
[CrossRef]

V. I. Klimov, A. A. Mikhailovsky, S. Xu, A. Malko, J. A. Hollingsworth, C. A. Leatherdale, H.-J. Eisler, and M. G. Bawendi, “Optical gain and stimulated emission in nanocrystal quantum dots,” Science290(5490), 314–317 (2000).
[CrossRef] [PubMed]

V. I. Klimov, A. A. Mikhailovsky, D. W. McBranch, C. A. Leatherdale, and M. G. Bawendi, “Quantization of multiparticle Auger rates in semiconductor quantum dots,” Science287(5455), 1011–1013 (2000).
[CrossRef] [PubMed]

1996 (1)

M. Nirmal, B. O. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, “Fluorescence intermittency in single cadmium selenide nanocrystals,” Nature383(6603), 802–804 (1996).
[CrossRef]

1992 (1)

T. Basché, W. E. Moerner, M. Orrit, and H. Talon, “Photon antibunching in the fluorescence of a single dye molecule trapped in a solid,” Phys. Rev. Lett.69(10), 1516–1519 (1992).
[CrossRef] [PubMed]

Abram, I.

E. Moreau, I. Robert, L. Manin, V. Thierry-Mieg, J. M. Gérard, and I. Abram, “Quantum cascade of photons in semiconductor quantum dots,” Phys. Rev. Lett.87(18), 183601 (2001).
[CrossRef]

Atkinson, P.

R. M. Stevenson, R. J. Young, P. Atkinson, K. Cooper, D. A. Ritchie, and A. J. Shields, “A semiconductor source of triggered entangled photon pairs,” Nature439(7073), 179–182 (2006).
[CrossRef] [PubMed]

Basché, T.

T. Basché, W. E. Moerner, M. Orrit, and H. Talon, “Photon antibunching in the fluorescence of a single dye molecule trapped in a solid,” Phys. Rev. Lett.69(10), 1516–1519 (1992).
[CrossRef] [PubMed]

Bawendi, M.

B. Fisher, J. M. Caruge, D. Zehnder, and M. Bawendi, “Room-temperature ordered photon emission from multiexciton states in single CdSe core-shell nanocrystals,” Phys. Rev. Lett.94(8), 087403 (2005).
[CrossRef] [PubMed]

Bawendi, M. G.

G. Nair, J. Zhao, and M. G. Bawendi, “Biexciton quantum yield of single semiconductor nanocrystals from photon statistics,” Nano Lett.11(3), 1136–1140 (2011).
[CrossRef] [PubMed]

J. Zhao, G. Nair, B. R. Fisher, and M. G. Bawendi, “Challenge to the charging model of semiconductor-nanocrystal fluorescence intermittency from off-state quantum yields and multiexciton blinking,” Phys. Rev. Lett.104(15), 157403 (2010).
[CrossRef] [PubMed]

V. I. Klimov, A. A. Mikhailovsky, S. Xu, A. Malko, J. A. Hollingsworth, C. A. Leatherdale, H.-J. Eisler, and M. G. Bawendi, “Optical gain and stimulated emission in nanocrystal quantum dots,” Science290(5490), 314–317 (2000).
[CrossRef] [PubMed]

V. I. Klimov, A. A. Mikhailovsky, D. W. McBranch, C. A. Leatherdale, and M. G. Bawendi, “Quantization of multiparticle Auger rates in semiconductor quantum dots,” Science287(5455), 1011–1013 (2000).
[CrossRef] [PubMed]

M. Nirmal, B. O. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, “Fluorescence intermittency in single cadmium selenide nanocrystals,” Nature383(6603), 802–804 (1996).
[CrossRef]

Becher, C.

P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, “A quantum dot single-photon turnstile device,” Science290(5500), 2282–2285 (2000).
[CrossRef] [PubMed]

Beveratos, A.

A. Beveratos, R. Brouri, T. Gacoin, J.-P. Poizat, and P. Grangier, “Nonclassical radiation from diamond nanocrystals,” Phys. Rev. A64(6), 061802 (2001).
[CrossRef]

R. Brouri, A. Beveratos, J.-P. Poizat, and P. Grangier, “Photon antibunching in the fluorescence of individual color centers in diamond,” Opt. Lett.25(17), 1294–1296 (2000).
[CrossRef] [PubMed]

Biadala, L.

Y. Louyer, L. Biadala, J. B. Trebbia, M. J. Fernée, P. Tamarat, and B. Lounis, “Efficient biexciton emission in elongated CdSe/ZnS nanocrystals,” Nano Lett.11(10), 4370–4375 (2011).
[CrossRef] [PubMed]

Brouri, R.

A. Beveratos, R. Brouri, T. Gacoin, J.-P. Poizat, and P. Grangier, “Nonclassical radiation from diamond nanocrystals,” Phys. Rev. A64(6), 061802 (2001).
[CrossRef]

R. Brouri, A. Beveratos, J.-P. Poizat, and P. Grangier, “Photon antibunching in the fluorescence of individual color centers in diamond,” Opt. Lett.25(17), 1294–1296 (2000).
[CrossRef] [PubMed]

Brus, L. E.

M. Nirmal, B. O. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, “Fluorescence intermittency in single cadmium selenide nanocrystals,” Nature383(6603), 802–804 (1996).
[CrossRef]

Buil, S.

D. Canneson, I. Mallek-Zouari, S. Buil, X. Quelin, C. Javaux, B. Dubertret, and J.-P. Hermier, “Enhancing the fluorescence of individual thick shell CdSe/CdS Nanocrystals by coupling to gold structures,” New J. Phys.14(6), 063035 (2012).
[CrossRef]

Buratto, S. K.

P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and S. K. Buratto, “Quantum correlation among photons from a single quantum dot at room temperature,” Nature406(6799), 968–970 (2000).
[CrossRef] [PubMed]

Bussian, D. A.

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, ““Giant” multishell CdSe nanocrystal quantum dots with suppressed blinking,” J. Am. Chem. Soc.130(15), 5026–5027 (2008).
[CrossRef] [PubMed]

Canneson, D.

D. Canneson, I. Mallek-Zouari, S. Buil, X. Quelin, C. Javaux, B. Dubertret, and J.-P. Hermier, “Enhancing the fluorescence of individual thick shell CdSe/CdS Nanocrystals by coupling to gold structures,” New J. Phys.14(6), 063035 (2012).
[CrossRef]

Carson, P. J.

P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and S. K. Buratto, “Quantum correlation among photons from a single quantum dot at room temperature,” Nature406(6799), 968–970 (2000).
[CrossRef] [PubMed]

Caruge, J. M.

B. Fisher, J. M. Caruge, D. Zehnder, and M. Bawendi, “Room-temperature ordered photon emission from multiexciton states in single CdSe core-shell nanocrystals,” Phys. Rev. Lett.94(8), 087403 (2005).
[CrossRef] [PubMed]

Casson, J. L.

Y. Ghosh, B. D. Mangum, J. L. Casson, D. J. Williams, H. Htoon, and J. A. Hollingsworth, “New insights into the complexities of shell growth and the strong influence of particle volume in nonblinking “giant” core/shell nanocrystal quantum dots,” J. Am. Chem. Soc.134(23), 9634–9643 (2012).
[CrossRef] [PubMed]

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, ““Giant” multishell CdSe nanocrystal quantum dots with suppressed blinking,” J. Am. Chem. Soc.130(15), 5026–5027 (2008).
[CrossRef] [PubMed]

Chen, Y.

Y. S. Park, A. V. Malko, J. Vela, Y. Chen, Y. Ghosh, F. García-Santamaría, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Near-unity quantum yields of biexciton emission from CdSe/CdS nanocrystals measured using single-particle spectroscopy,” Phys. Rev. Lett.106(18), 187401 (2011).
[CrossRef] [PubMed]

F. García-Santamaría, Y. Chen, J. Vela, R. D. Schaller, J. A. Hollingsworth, and V. I. Klimov, “Suppressed Auger recombination in “giant” nanocrystals boosts optical gain performance,” Nano Lett.9(10), 3482–3488 (2009).
[CrossRef] [PubMed]

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, ““Giant” multishell CdSe nanocrystal quantum dots with suppressed blinking,” J. Am. Chem. Soc.130(15), 5026–5027 (2008).
[CrossRef] [PubMed]

Cheskis, D.

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V. I. Klimov, A. A. Mikhailovsky, S. Xu, A. Malko, J. A. Hollingsworth, C. A. Leatherdale, H.-J. Eisler, and M. G. Bawendi, “Optical gain and stimulated emission in nanocrystal quantum dots,” Science290(5490), 314–317 (2000).
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A. Muller, W. Fang, J. Lawall, and G. S. Solomon, “Creating polarization-entangled photon pairs from a semiconductor quantum dot using the optical Stark effect,” Phys. Rev. Lett.103(21), 217402 (2009).
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Y. Louyer, L. Biadala, J. B. Trebbia, M. J. Fernée, P. Tamarat, and B. Lounis, “Efficient biexciton emission in elongated CdSe/ZnS nanocrystals,” Nano Lett.11(10), 4370–4375 (2011).
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J. Zhao, G. Nair, B. R. Fisher, and M. G. Bawendi, “Challenge to the charging model of semiconductor-nanocrystal fluorescence intermittency from off-state quantum yields and multiexciton blinking,” Phys. Rev. Lett.104(15), 157403 (2010).
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Y. S. Park, A. V. Malko, J. Vela, Y. Chen, Y. Ghosh, F. García-Santamaría, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Near-unity quantum yields of biexciton emission from CdSe/CdS nanocrystals measured using single-particle spectroscopy,” Phys. Rev. Lett.106(18), 187401 (2011).
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F. García-Santamaría, Y. Chen, J. Vela, R. D. Schaller, J. A. Hollingsworth, and V. I. Klimov, “Suppressed Auger recombination in “giant” nanocrystals boosts optical gain performance,” Nano Lett.9(10), 3482–3488 (2009).
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E. Moreau, I. Robert, L. Manin, V. Thierry-Mieg, J. M. Gérard, and I. Abram, “Quantum cascade of photons in semiconductor quantum dots,” Phys. Rev. Lett.87(18), 183601 (2001).
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E. Dekel, D. V. Regelman, D. Gershoni, E. Ehrenfreund, W. V. Schoenfeld, and P. M. Petroff, “Cascade evolution and radiative recombination of quantum dot multiexcitons studied by time-resolved spectroscopy,” Phys. Rev. B62(16), 11038–11045 (2000).
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Y. Ghosh, B. D. Mangum, J. L. Casson, D. J. Williams, H. Htoon, and J. A. Hollingsworth, “New insights into the complexities of shell growth and the strong influence of particle volume in nonblinking “giant” core/shell nanocrystal quantum dots,” J. Am. Chem. Soc.134(23), 9634–9643 (2012).
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Y. S. Park, A. V. Malko, J. Vela, Y. Chen, Y. Ghosh, F. García-Santamaría, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Near-unity quantum yields of biexciton emission from CdSe/CdS nanocrystals measured using single-particle spectroscopy,” Phys. Rev. Lett.106(18), 187401 (2011).
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C. Galland, Y. Ghosh, A. Steinbrück, M. Sykora, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots,” Nature479(7372), 203–207 (2011).
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A. Beveratos, R. Brouri, T. Gacoin, J.-P. Poizat, and P. Grangier, “Nonclassical radiation from diamond nanocrystals,” Phys. Rev. A64(6), 061802 (2001).
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R. Brouri, A. Beveratos, J.-P. Poizat, and P. Grangier, “Photon antibunching in the fluorescence of individual color centers in diamond,” Opt. Lett.25(17), 1294–1296 (2000).
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Hamann, H. F.

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[CrossRef]

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M. Nirmal, B. O. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, “Fluorescence intermittency in single cadmium selenide nanocrystals,” Nature383(6603), 802–804 (1996).
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D. Canneson, I. Mallek-Zouari, S. Buil, X. Quelin, C. Javaux, B. Dubertret, and J.-P. Hermier, “Enhancing the fluorescence of individual thick shell CdSe/CdS Nanocrystals by coupling to gold structures,” New J. Phys.14(6), 063035 (2012).
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K. D. Weston, M. Dyck, P. Tinnefeld, C. Müller, D. P. Herten, and M. Sauer, “Measuring the number of independent emitters in single-molecule fluorescence images and trajectories using coincident photons,” Anal. Chem.74(20), 5342–5349 (2002).
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A. Högele, C. Galland, M. Winger, and A. Imamoğlu, “Photon antibunching in the photoluminescence spectra of a single carbon nanotube,” Phys. Rev. Lett.100(21), 217401 (2008).
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Y. Ghosh, B. D. Mangum, J. L. Casson, D. J. Williams, H. Htoon, and J. A. Hollingsworth, “New insights into the complexities of shell growth and the strong influence of particle volume in nonblinking “giant” core/shell nanocrystal quantum dots,” J. Am. Chem. Soc.134(23), 9634–9643 (2012).
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Y. S. Park, A. V. Malko, J. Vela, Y. Chen, Y. Ghosh, F. García-Santamaría, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Near-unity quantum yields of biexciton emission from CdSe/CdS nanocrystals measured using single-particle spectroscopy,” Phys. Rev. Lett.106(18), 187401 (2011).
[CrossRef] [PubMed]

C. Galland, Y. Ghosh, A. Steinbrück, M. Sykora, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots,” Nature479(7372), 203–207 (2011).
[CrossRef] [PubMed]

F. García-Santamaría, Y. Chen, J. Vela, R. D. Schaller, J. A. Hollingsworth, and V. I. Klimov, “Suppressed Auger recombination in “giant” nanocrystals boosts optical gain performance,” Nano Lett.9(10), 3482–3488 (2009).
[CrossRef] [PubMed]

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, ““Giant” multishell CdSe nanocrystal quantum dots with suppressed blinking,” J. Am. Chem. Soc.130(15), 5026–5027 (2008).
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V. I. Klimov, A. A. Mikhailovsky, S. Xu, A. Malko, J. A. Hollingsworth, C. A. Leatherdale, H.-J. Eisler, and M. G. Bawendi, “Optical gain and stimulated emission in nanocrystal quantum dots,” Science290(5490), 314–317 (2000).
[CrossRef] [PubMed]

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Y. Ghosh, B. D. Mangum, J. L. Casson, D. J. Williams, H. Htoon, and J. A. Hollingsworth, “New insights into the complexities of shell growth and the strong influence of particle volume in nonblinking “giant” core/shell nanocrystal quantum dots,” J. Am. Chem. Soc.134(23), 9634–9643 (2012).
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Y. S. Park, A. V. Malko, J. Vela, Y. Chen, Y. Ghosh, F. García-Santamaría, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Near-unity quantum yields of biexciton emission from CdSe/CdS nanocrystals measured using single-particle spectroscopy,” Phys. Rev. Lett.106(18), 187401 (2011).
[CrossRef] [PubMed]

C. Galland, Y. Ghosh, A. Steinbrück, M. Sykora, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots,” Nature479(7372), 203–207 (2011).
[CrossRef] [PubMed]

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, ““Giant” multishell CdSe nanocrystal quantum dots with suppressed blinking,” J. Am. Chem. Soc.130(15), 5026–5027 (2008).
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P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, “A quantum dot single-photon turnstile device,” Science290(5500), 2282–2285 (2000).
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A. Högele, C. Galland, M. Winger, and A. Imamoğlu, “Photon antibunching in the photoluminescence spectra of a single carbon nanotube,” Phys. Rev. Lett.100(21), 217401 (2008).
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P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, “A quantum dot single-photon turnstile device,” Science290(5500), 2282–2285 (2000).
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P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and S. K. Buratto, “Quantum correlation among photons from a single quantum dot at room temperature,” Nature406(6799), 968–970 (2000).
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C. Galland, Y. Ghosh, A. Steinbrück, M. Sykora, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots,” Nature479(7372), 203–207 (2011).
[CrossRef] [PubMed]

Y. S. Park, A. V. Malko, J. Vela, Y. Chen, Y. Ghosh, F. García-Santamaría, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Near-unity quantum yields of biexciton emission from CdSe/CdS nanocrystals measured using single-particle spectroscopy,” Phys. Rev. Lett.106(18), 187401 (2011).
[CrossRef] [PubMed]

F. García-Santamaría, Y. Chen, J. Vela, R. D. Schaller, J. A. Hollingsworth, and V. I. Klimov, “Suppressed Auger recombination in “giant” nanocrystals boosts optical gain performance,” Nano Lett.9(10), 3482–3488 (2009).
[CrossRef] [PubMed]

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, ““Giant” multishell CdSe nanocrystal quantum dots with suppressed blinking,” J. Am. Chem. Soc.130(15), 5026–5027 (2008).
[CrossRef] [PubMed]

R. D. Schaller and V. I. Klimov, “High efficiency carrier multiplication in PbSe nanocrystals: Implications for solar energy conversion,” Phys. Rev. Lett.92(18), 186601 (2004).
[CrossRef] [PubMed]

V. I. Klimov, A. A. Mikhailovsky, S. Xu, A. Malko, J. A. Hollingsworth, C. A. Leatherdale, H.-J. Eisler, and M. G. Bawendi, “Optical gain and stimulated emission in nanocrystal quantum dots,” Science290(5490), 314–317 (2000).
[CrossRef] [PubMed]

V. I. Klimov, A. A. Mikhailovsky, D. W. McBranch, C. A. Leatherdale, and M. G. Bawendi, “Quantization of multiparticle Auger rates in semiconductor quantum dots,” Science287(5455), 1011–1013 (2000).
[CrossRef] [PubMed]

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R. Osovsky, D. Cheskis, V. Kloper, A. Sashchiuk, M. Kroner, and E. Lifshitz, “Continuous-wave pumping of multiexciton bands in the photoluminescence spectrum of a single CdTe-CdSe core-shell colloidal quantum dot,” Phys. Rev. Lett.102(19), 197401 (2009).
[CrossRef] [PubMed]

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S. Jander, A. Kornowski, and H. Weller, “Energy transfer from CdSe/CdS nanorods to amorphous carbon,” Nano Lett.11(12), 5179–5183 (2011).
[CrossRef] [PubMed]

Kroner, M.

R. Osovsky, D. Cheskis, V. Kloper, A. Sashchiuk, M. Kroner, and E. Lifshitz, “Continuous-wave pumping of multiexciton bands in the photoluminescence spectrum of a single CdTe-CdSe core-shell colloidal quantum dot,” Phys. Rev. Lett.102(19), 197401 (2009).
[CrossRef] [PubMed]

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M. Kuno, D. P. Fromm, H. F. Hamann, A. Gallagher, and D. J. Nesbitt, “Nonexponential “blinking” kinetics of single CdSe quantum dots: A universal power law behavior,” J. Chem. Phys.112(7), 3117–3120 (2000).
[CrossRef]

Kurtsiefer, C.

C. Kurtsiefer, S. Mayer, P. Zarda, and H. Weinfurter, “Stable solid-state source of single photons,” Phys. Rev. Lett.85(2), 290–293 (2000).
[CrossRef] [PubMed]

Lawall, J.

A. Muller, W. Fang, J. Lawall, and G. S. Solomon, “Creating polarization-entangled photon pairs from a semiconductor quantum dot using the optical Stark effect,” Phys. Rev. Lett.103(21), 217402 (2009).
[CrossRef] [PubMed]

Leatherdale, C. A.

V. I. Klimov, A. A. Mikhailovsky, S. Xu, A. Malko, J. A. Hollingsworth, C. A. Leatherdale, H.-J. Eisler, and M. G. Bawendi, “Optical gain and stimulated emission in nanocrystal quantum dots,” Science290(5490), 314–317 (2000).
[CrossRef] [PubMed]

V. I. Klimov, A. A. Mikhailovsky, D. W. McBranch, C. A. Leatherdale, and M. G. Bawendi, “Quantization of multiparticle Auger rates in semiconductor quantum dots,” Science287(5455), 1011–1013 (2000).
[CrossRef] [PubMed]

Lifshitz, E.

R. Osovsky, D. Cheskis, V. Kloper, A. Sashchiuk, M. Kroner, and E. Lifshitz, “Continuous-wave pumping of multiexciton bands in the photoluminescence spectrum of a single CdTe-CdSe core-shell colloidal quantum dot,” Phys. Rev. Lett.102(19), 197401 (2009).
[CrossRef] [PubMed]

Lounis, B.

Y. Louyer, L. Biadala, J. B. Trebbia, M. J. Fernée, P. Tamarat, and B. Lounis, “Efficient biexciton emission in elongated CdSe/ZnS nanocrystals,” Nano Lett.11(10), 4370–4375 (2011).
[CrossRef] [PubMed]

B. Lounis and W. E. Moerner, “Single photons on demand from a single molecule at room temperature,” Nature407(6803), 491–493 (2000).
[CrossRef] [PubMed]

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Y. Louyer, L. Biadala, J. B. Trebbia, M. J. Fernée, P. Tamarat, and B. Lounis, “Efficient biexciton emission in elongated CdSe/ZnS nanocrystals,” Nano Lett.11(10), 4370–4375 (2011).
[CrossRef] [PubMed]

Macklin, J. J.

M. Nirmal, B. O. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, “Fluorescence intermittency in single cadmium selenide nanocrystals,” Nature383(6603), 802–804 (1996).
[CrossRef]

Malko, A.

V. I. Klimov, A. A. Mikhailovsky, S. Xu, A. Malko, J. A. Hollingsworth, C. A. Leatherdale, H.-J. Eisler, and M. G. Bawendi, “Optical gain and stimulated emission in nanocrystal quantum dots,” Science290(5490), 314–317 (2000).
[CrossRef] [PubMed]

Malko, A. V.

Y. S. Park, A. V. Malko, J. Vela, Y. Chen, Y. Ghosh, F. García-Santamaría, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Near-unity quantum yields of biexciton emission from CdSe/CdS nanocrystals measured using single-particle spectroscopy,” Phys. Rev. Lett.106(18), 187401 (2011).
[CrossRef] [PubMed]

Mallek-Zouari, I.

D. Canneson, I. Mallek-Zouari, S. Buil, X. Quelin, C. Javaux, B. Dubertret, and J.-P. Hermier, “Enhancing the fluorescence of individual thick shell CdSe/CdS Nanocrystals by coupling to gold structures,” New J. Phys.14(6), 063035 (2012).
[CrossRef]

Mangum, B. D.

Y. Ghosh, B. D. Mangum, J. L. Casson, D. J. Williams, H. Htoon, and J. A. Hollingsworth, “New insights into the complexities of shell growth and the strong influence of particle volume in nonblinking “giant” core/shell nanocrystal quantum dots,” J. Am. Chem. Soc.134(23), 9634–9643 (2012).
[CrossRef] [PubMed]

Manin, L.

E. Moreau, I. Robert, L. Manin, V. Thierry-Mieg, J. M. Gérard, and I. Abram, “Quantum cascade of photons in semiconductor quantum dots,” Phys. Rev. Lett.87(18), 183601 (2001).
[CrossRef]

Mason, M. D.

P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and S. K. Buratto, “Quantum correlation among photons from a single quantum dot at room temperature,” Nature406(6799), 968–970 (2000).
[CrossRef] [PubMed]

Mayer, S.

C. Kurtsiefer, S. Mayer, P. Zarda, and H. Weinfurter, “Stable solid-state source of single photons,” Phys. Rev. Lett.85(2), 290–293 (2000).
[CrossRef] [PubMed]

McBranch, D. W.

V. I. Klimov, A. A. Mikhailovsky, D. W. McBranch, C. A. Leatherdale, and M. G. Bawendi, “Quantization of multiparticle Auger rates in semiconductor quantum dots,” Science287(5455), 1011–1013 (2000).
[CrossRef] [PubMed]

Michler, P.

P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and S. K. Buratto, “Quantum correlation among photons from a single quantum dot at room temperature,” Nature406(6799), 968–970 (2000).
[CrossRef] [PubMed]

P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, “A quantum dot single-photon turnstile device,” Science290(5500), 2282–2285 (2000).
[CrossRef] [PubMed]

Mikhailovsky, A. A.

V. I. Klimov, A. A. Mikhailovsky, D. W. McBranch, C. A. Leatherdale, and M. G. Bawendi, “Quantization of multiparticle Auger rates in semiconductor quantum dots,” Science287(5455), 1011–1013 (2000).
[CrossRef] [PubMed]

V. I. Klimov, A. A. Mikhailovsky, S. Xu, A. Malko, J. A. Hollingsworth, C. A. Leatherdale, H.-J. Eisler, and M. G. Bawendi, “Optical gain and stimulated emission in nanocrystal quantum dots,” Science290(5490), 314–317 (2000).
[CrossRef] [PubMed]

Moerner, W. E.

B. Lounis and W. E. Moerner, “Single photons on demand from a single molecule at room temperature,” Nature407(6803), 491–493 (2000).
[CrossRef] [PubMed]

T. Basché, W. E. Moerner, M. Orrit, and H. Talon, “Photon antibunching in the fluorescence of a single dye molecule trapped in a solid,” Phys. Rev. Lett.69(10), 1516–1519 (1992).
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E. Moreau, I. Robert, L. Manin, V. Thierry-Mieg, J. M. Gérard, and I. Abram, “Quantum cascade of photons in semiconductor quantum dots,” Phys. Rev. Lett.87(18), 183601 (2001).
[CrossRef]

Muller, A.

A. Muller, W. Fang, J. Lawall, and G. S. Solomon, “Creating polarization-entangled photon pairs from a semiconductor quantum dot using the optical Stark effect,” Phys. Rev. Lett.103(21), 217402 (2009).
[CrossRef] [PubMed]

Müller, C.

K. D. Weston, M. Dyck, P. Tinnefeld, C. Müller, D. P. Herten, and M. Sauer, “Measuring the number of independent emitters in single-molecule fluorescence images and trajectories using coincident photons,” Anal. Chem.74(20), 5342–5349 (2002).
[CrossRef] [PubMed]

P. Tinnefeld, C. Müller, and M. Sauer, “Time-varying photon probability distribution of individual molecules at room temperature,” Chem. Phys. Lett.345(3-4), 252–258 (2001).
[CrossRef]

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G. Nair, J. Zhao, and M. G. Bawendi, “Biexciton quantum yield of single semiconductor nanocrystals from photon statistics,” Nano Lett.11(3), 1136–1140 (2011).
[CrossRef] [PubMed]

J. Zhao, G. Nair, B. R. Fisher, and M. G. Bawendi, “Challenge to the charging model of semiconductor-nanocrystal fluorescence intermittency from off-state quantum yields and multiexciton blinking,” Phys. Rev. Lett.104(15), 157403 (2010).
[CrossRef] [PubMed]

Nesbitt, D. J.

M. Kuno, D. P. Fromm, H. F. Hamann, A. Gallagher, and D. J. Nesbitt, “Nonexponential “blinking” kinetics of single CdSe quantum dots: A universal power law behavior,” J. Chem. Phys.112(7), 3117–3120 (2000).
[CrossRef]

Nirmal, M.

M. Nirmal, B. O. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, “Fluorescence intermittency in single cadmium selenide nanocrystals,” Nature383(6603), 802–804 (1996).
[CrossRef]

Nozik, A. J.

A. Shabaev, A. L. Efros, and A. J. Nozik, “Multiexciton generation by a single photon in nanocrystals,” Nano Lett.6(12), 2856–2863 (2006).
[CrossRef] [PubMed]

Orrit, M.

T. Basché, W. E. Moerner, M. Orrit, and H. Talon, “Photon antibunching in the fluorescence of a single dye molecule trapped in a solid,” Phys. Rev. Lett.69(10), 1516–1519 (1992).
[CrossRef] [PubMed]

Osovsky, R.

R. Osovsky, D. Cheskis, V. Kloper, A. Sashchiuk, M. Kroner, and E. Lifshitz, “Continuous-wave pumping of multiexciton bands in the photoluminescence spectrum of a single CdTe-CdSe core-shell colloidal quantum dot,” Phys. Rev. Lett.102(19), 197401 (2009).
[CrossRef] [PubMed]

Park, Y. S.

Y. S. Park, A. V. Malko, J. Vela, Y. Chen, Y. Ghosh, F. García-Santamaría, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Near-unity quantum yields of biexciton emission from CdSe/CdS nanocrystals measured using single-particle spectroscopy,” Phys. Rev. Lett.106(18), 187401 (2011).
[CrossRef] [PubMed]

Petroff, P. M.

E. Dekel, D. V. Regelman, D. Gershoni, E. Ehrenfreund, W. V. Schoenfeld, and P. M. Petroff, “Cascade evolution and radiative recombination of quantum dot multiexcitons studied by time-resolved spectroscopy,” Phys. Rev. B62(16), 11038–11045 (2000).
[CrossRef]

P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, “A quantum dot single-photon turnstile device,” Science290(5500), 2282–2285 (2000).
[CrossRef] [PubMed]

Poizat, J.-P.

A. Beveratos, R. Brouri, T. Gacoin, J.-P. Poizat, and P. Grangier, “Nonclassical radiation from diamond nanocrystals,” Phys. Rev. A64(6), 061802 (2001).
[CrossRef]

R. Brouri, A. Beveratos, J.-P. Poizat, and P. Grangier, “Photon antibunching in the fluorescence of individual color centers in diamond,” Opt. Lett.25(17), 1294–1296 (2000).
[CrossRef] [PubMed]

Quelin, X.

D. Canneson, I. Mallek-Zouari, S. Buil, X. Quelin, C. Javaux, B. Dubertret, and J.-P. Hermier, “Enhancing the fluorescence of individual thick shell CdSe/CdS Nanocrystals by coupling to gold structures,” New J. Phys.14(6), 063035 (2012).
[CrossRef]

Regelman, D. V.

E. Dekel, D. V. Regelman, D. Gershoni, E. Ehrenfreund, W. V. Schoenfeld, and P. M. Petroff, “Cascade evolution and radiative recombination of quantum dot multiexcitons studied by time-resolved spectroscopy,” Phys. Rev. B62(16), 11038–11045 (2000).
[CrossRef]

Ritchie, D. A.

R. M. Stevenson, R. J. Young, P. Atkinson, K. Cooper, D. A. Ritchie, and A. J. Shields, “A semiconductor source of triggered entangled photon pairs,” Nature439(7073), 179–182 (2006).
[CrossRef] [PubMed]

Robert, I.

E. Moreau, I. Robert, L. Manin, V. Thierry-Mieg, J. M. Gérard, and I. Abram, “Quantum cascade of photons in semiconductor quantum dots,” Phys. Rev. Lett.87(18), 183601 (2001).
[CrossRef]

Roch, J.-F.

Sashchiuk, A.

R. Osovsky, D. Cheskis, V. Kloper, A. Sashchiuk, M. Kroner, and E. Lifshitz, “Continuous-wave pumping of multiexciton bands in the photoluminescence spectrum of a single CdTe-CdSe core-shell colloidal quantum dot,” Phys. Rev. Lett.102(19), 197401 (2009).
[CrossRef] [PubMed]

Sauer, M.

K. D. Weston, M. Dyck, P. Tinnefeld, C. Müller, D. P. Herten, and M. Sauer, “Measuring the number of independent emitters in single-molecule fluorescence images and trajectories using coincident photons,” Anal. Chem.74(20), 5342–5349 (2002).
[CrossRef] [PubMed]

P. Tinnefeld, C. Müller, and M. Sauer, “Time-varying photon probability distribution of individual molecules at room temperature,” Chem. Phys. Lett.345(3-4), 252–258 (2001).
[CrossRef]

Schaller, R. D.

F. García-Santamaría, Y. Chen, J. Vela, R. D. Schaller, J. A. Hollingsworth, and V. I. Klimov, “Suppressed Auger recombination in “giant” nanocrystals boosts optical gain performance,” Nano Lett.9(10), 3482–3488 (2009).
[CrossRef] [PubMed]

R. D. Schaller and V. I. Klimov, “High efficiency carrier multiplication in PbSe nanocrystals: Implications for solar energy conversion,” Phys. Rev. Lett.92(18), 186601 (2004).
[CrossRef] [PubMed]

Schoenfeld, W. V.

E. Dekel, D. V. Regelman, D. Gershoni, E. Ehrenfreund, W. V. Schoenfeld, and P. M. Petroff, “Cascade evolution and radiative recombination of quantum dot multiexcitons studied by time-resolved spectroscopy,” Phys. Rev. B62(16), 11038–11045 (2000).
[CrossRef]

P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, “A quantum dot single-photon turnstile device,” Science290(5500), 2282–2285 (2000).
[CrossRef] [PubMed]

Shabaev, A.

A. Shabaev, A. L. Efros, and A. J. Nozik, “Multiexciton generation by a single photon in nanocrystals,” Nano Lett.6(12), 2856–2863 (2006).
[CrossRef] [PubMed]

Shields, A. J.

R. M. Stevenson, R. J. Young, P. Atkinson, K. Cooper, D. A. Ritchie, and A. J. Shields, “A semiconductor source of triggered entangled photon pairs,” Nature439(7073), 179–182 (2006).
[CrossRef] [PubMed]

Solomon, G. S.

A. Muller, W. Fang, J. Lawall, and G. S. Solomon, “Creating polarization-entangled photon pairs from a semiconductor quantum dot using the optical Stark effect,” Phys. Rev. Lett.103(21), 217402 (2009).
[CrossRef] [PubMed]

Steinbrück, A.

C. Galland, Y. Ghosh, A. Steinbrück, M. Sykora, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots,” Nature479(7372), 203–207 (2011).
[CrossRef] [PubMed]

Stevenson, R. M.

R. M. Stevenson, R. J. Young, P. Atkinson, K. Cooper, D. A. Ritchie, and A. J. Shields, “A semiconductor source of triggered entangled photon pairs,” Nature439(7073), 179–182 (2006).
[CrossRef] [PubMed]

Strouse, G. F.

P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and S. K. Buratto, “Quantum correlation among photons from a single quantum dot at room temperature,” Nature406(6799), 968–970 (2000).
[CrossRef] [PubMed]

Sykora, M.

C. Galland, Y. Ghosh, A. Steinbrück, M. Sykora, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots,” Nature479(7372), 203–207 (2011).
[CrossRef] [PubMed]

Talon, H.

T. Basché, W. E. Moerner, M. Orrit, and H. Talon, “Photon antibunching in the fluorescence of a single dye molecule trapped in a solid,” Phys. Rev. Lett.69(10), 1516–1519 (1992).
[CrossRef] [PubMed]

Tamarat, P.

Y. Louyer, L. Biadala, J. B. Trebbia, M. J. Fernée, P. Tamarat, and B. Lounis, “Efficient biexciton emission in elongated CdSe/ZnS nanocrystals,” Nano Lett.11(10), 4370–4375 (2011).
[CrossRef] [PubMed]

Thierry-Mieg, V.

E. Moreau, I. Robert, L. Manin, V. Thierry-Mieg, J. M. Gérard, and I. Abram, “Quantum cascade of photons in semiconductor quantum dots,” Phys. Rev. Lett.87(18), 183601 (2001).
[CrossRef]

Tinnefeld, P.

K. D. Weston, M. Dyck, P. Tinnefeld, C. Müller, D. P. Herten, and M. Sauer, “Measuring the number of independent emitters in single-molecule fluorescence images and trajectories using coincident photons,” Anal. Chem.74(20), 5342–5349 (2002).
[CrossRef] [PubMed]

P. Tinnefeld, C. Müller, and M. Sauer, “Time-varying photon probability distribution of individual molecules at room temperature,” Chem. Phys. Lett.345(3-4), 252–258 (2001).
[CrossRef]

Trautman, J. K.

M. Nirmal, B. O. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, “Fluorescence intermittency in single cadmium selenide nanocrystals,” Nature383(6603), 802–804 (1996).
[CrossRef]

Trebbia, J. B.

Y. Louyer, L. Biadala, J. B. Trebbia, M. J. Fernée, P. Tamarat, and B. Lounis, “Efficient biexciton emission in elongated CdSe/ZnS nanocrystals,” Nano Lett.11(10), 4370–4375 (2011).
[CrossRef] [PubMed]

Treussart, F.

Vela, J.

Y. S. Park, A. V. Malko, J. Vela, Y. Chen, Y. Ghosh, F. García-Santamaría, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Near-unity quantum yields of biexciton emission from CdSe/CdS nanocrystals measured using single-particle spectroscopy,” Phys. Rev. Lett.106(18), 187401 (2011).
[CrossRef] [PubMed]

F. García-Santamaría, Y. Chen, J. Vela, R. D. Schaller, J. A. Hollingsworth, and V. I. Klimov, “Suppressed Auger recombination in “giant” nanocrystals boosts optical gain performance,” Nano Lett.9(10), 3482–3488 (2009).
[CrossRef] [PubMed]

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, ““Giant” multishell CdSe nanocrystal quantum dots with suppressed blinking,” J. Am. Chem. Soc.130(15), 5026–5027 (2008).
[CrossRef] [PubMed]

Weinfurter, H.

C. Kurtsiefer, S. Mayer, P. Zarda, and H. Weinfurter, “Stable solid-state source of single photons,” Phys. Rev. Lett.85(2), 290–293 (2000).
[CrossRef] [PubMed]

Weller, H.

S. Jander, A. Kornowski, and H. Weller, “Energy transfer from CdSe/CdS nanorods to amorphous carbon,” Nano Lett.11(12), 5179–5183 (2011).
[CrossRef] [PubMed]

Werder, D. J.

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, ““Giant” multishell CdSe nanocrystal quantum dots with suppressed blinking,” J. Am. Chem. Soc.130(15), 5026–5027 (2008).
[CrossRef] [PubMed]

Weston, K. D.

K. D. Weston, M. Dyck, P. Tinnefeld, C. Müller, D. P. Herten, and M. Sauer, “Measuring the number of independent emitters in single-molecule fluorescence images and trajectories using coincident photons,” Anal. Chem.74(20), 5342–5349 (2002).
[CrossRef] [PubMed]

Williams, D. J.

Y. Ghosh, B. D. Mangum, J. L. Casson, D. J. Williams, H. Htoon, and J. A. Hollingsworth, “New insights into the complexities of shell growth and the strong influence of particle volume in nonblinking “giant” core/shell nanocrystal quantum dots,” J. Am. Chem. Soc.134(23), 9634–9643 (2012).
[CrossRef] [PubMed]

Winger, M.

A. Högele, C. Galland, M. Winger, and A. Imamoğlu, “Photon antibunching in the photoluminescence spectra of a single carbon nanotube,” Phys. Rev. Lett.100(21), 217401 (2008).
[CrossRef] [PubMed]

Xu, S.

V. I. Klimov, A. A. Mikhailovsky, S. Xu, A. Malko, J. A. Hollingsworth, C. A. Leatherdale, H.-J. Eisler, and M. G. Bawendi, “Optical gain and stimulated emission in nanocrystal quantum dots,” Science290(5490), 314–317 (2000).
[CrossRef] [PubMed]

Young, R. J.

R. M. Stevenson, R. J. Young, P. Atkinson, K. Cooper, D. A. Ritchie, and A. J. Shields, “A semiconductor source of triggered entangled photon pairs,” Nature439(7073), 179–182 (2006).
[CrossRef] [PubMed]

Zarda, P.

C. Kurtsiefer, S. Mayer, P. Zarda, and H. Weinfurter, “Stable solid-state source of single photons,” Phys. Rev. Lett.85(2), 290–293 (2000).
[CrossRef] [PubMed]

Zehnder, D.

B. Fisher, J. M. Caruge, D. Zehnder, and M. Bawendi, “Room-temperature ordered photon emission from multiexciton states in single CdSe core-shell nanocrystals,” Phys. Rev. Lett.94(8), 087403 (2005).
[CrossRef] [PubMed]

Zhang, L.

P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, “A quantum dot single-photon turnstile device,” Science290(5500), 2282–2285 (2000).
[CrossRef] [PubMed]

Zhao, J.

G. Nair, J. Zhao, and M. G. Bawendi, “Biexciton quantum yield of single semiconductor nanocrystals from photon statistics,” Nano Lett.11(3), 1136–1140 (2011).
[CrossRef] [PubMed]

J. Zhao, G. Nair, B. R. Fisher, and M. G. Bawendi, “Challenge to the charging model of semiconductor-nanocrystal fluorescence intermittency from off-state quantum yields and multiexciton blinking,” Phys. Rev. Lett.104(15), 157403 (2010).
[CrossRef] [PubMed]

Anal. Chem. (1)

K. D. Weston, M. Dyck, P. Tinnefeld, C. Müller, D. P. Herten, and M. Sauer, “Measuring the number of independent emitters in single-molecule fluorescence images and trajectories using coincident photons,” Anal. Chem.74(20), 5342–5349 (2002).
[CrossRef] [PubMed]

Chem. Phys. Lett. (1)

P. Tinnefeld, C. Müller, and M. Sauer, “Time-varying photon probability distribution of individual molecules at room temperature,” Chem. Phys. Lett.345(3-4), 252–258 (2001).
[CrossRef]

J. Am. Chem. Soc. (2)

Y. Chen, J. Vela, H. Htoon, J. L. Casson, D. J. Werder, D. A. Bussian, V. I. Klimov, and J. A. Hollingsworth, ““Giant” multishell CdSe nanocrystal quantum dots with suppressed blinking,” J. Am. Chem. Soc.130(15), 5026–5027 (2008).
[CrossRef] [PubMed]

Y. Ghosh, B. D. Mangum, J. L. Casson, D. J. Williams, H. Htoon, and J. A. Hollingsworth, “New insights into the complexities of shell growth and the strong influence of particle volume in nonblinking “giant” core/shell nanocrystal quantum dots,” J. Am. Chem. Soc.134(23), 9634–9643 (2012).
[CrossRef] [PubMed]

J. Chem. Phys. (1)

M. Kuno, D. P. Fromm, H. F. Hamann, A. Gallagher, and D. J. Nesbitt, “Nonexponential “blinking” kinetics of single CdSe quantum dots: A universal power law behavior,” J. Chem. Phys.112(7), 3117–3120 (2000).
[CrossRef]

Nano Lett. (5)

S. Jander, A. Kornowski, and H. Weller, “Energy transfer from CdSe/CdS nanorods to amorphous carbon,” Nano Lett.11(12), 5179–5183 (2011).
[CrossRef] [PubMed]

A. Shabaev, A. L. Efros, and A. J. Nozik, “Multiexciton generation by a single photon in nanocrystals,” Nano Lett.6(12), 2856–2863 (2006).
[CrossRef] [PubMed]

F. García-Santamaría, Y. Chen, J. Vela, R. D. Schaller, J. A. Hollingsworth, and V. I. Klimov, “Suppressed Auger recombination in “giant” nanocrystals boosts optical gain performance,” Nano Lett.9(10), 3482–3488 (2009).
[CrossRef] [PubMed]

G. Nair, J. Zhao, and M. G. Bawendi, “Biexciton quantum yield of single semiconductor nanocrystals from photon statistics,” Nano Lett.11(3), 1136–1140 (2011).
[CrossRef] [PubMed]

Y. Louyer, L. Biadala, J. B. Trebbia, M. J. Fernée, P. Tamarat, and B. Lounis, “Efficient biexciton emission in elongated CdSe/ZnS nanocrystals,” Nano Lett.11(10), 4370–4375 (2011).
[CrossRef] [PubMed]

Nature (5)

B. Lounis and W. E. Moerner, “Single photons on demand from a single molecule at room temperature,” Nature407(6803), 491–493 (2000).
[CrossRef] [PubMed]

P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and S. K. Buratto, “Quantum correlation among photons from a single quantum dot at room temperature,” Nature406(6799), 968–970 (2000).
[CrossRef] [PubMed]

R. M. Stevenson, R. J. Young, P. Atkinson, K. Cooper, D. A. Ritchie, and A. J. Shields, “A semiconductor source of triggered entangled photon pairs,” Nature439(7073), 179–182 (2006).
[CrossRef] [PubMed]

M. Nirmal, B. O. Dabbousi, M. G. Bawendi, J. J. Macklin, J. K. Trautman, T. D. Harris, and L. E. Brus, “Fluorescence intermittency in single cadmium selenide nanocrystals,” Nature383(6603), 802–804 (1996).
[CrossRef]

C. Galland, Y. Ghosh, A. Steinbrück, M. Sykora, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots,” Nature479(7372), 203–207 (2011).
[CrossRef] [PubMed]

New J. Phys. (1)

D. Canneson, I. Mallek-Zouari, S. Buil, X. Quelin, C. Javaux, B. Dubertret, and J.-P. Hermier, “Enhancing the fluorescence of individual thick shell CdSe/CdS Nanocrystals by coupling to gold structures,” New J. Phys.14(6), 063035 (2012).
[CrossRef]

Opt. Lett. (2)

Phys. Rev. A (1)

A. Beveratos, R. Brouri, T. Gacoin, J.-P. Poizat, and P. Grangier, “Nonclassical radiation from diamond nanocrystals,” Phys. Rev. A64(6), 061802 (2001).
[CrossRef]

Phys. Rev. B (1)

E. Dekel, D. V. Regelman, D. Gershoni, E. Ehrenfreund, W. V. Schoenfeld, and P. M. Petroff, “Cascade evolution and radiative recombination of quantum dot multiexcitons studied by time-resolved spectroscopy,” Phys. Rev. B62(16), 11038–11045 (2000).
[CrossRef]

Phys. Rev. Lett. (10)

B. Fisher, J. M. Caruge, D. Zehnder, and M. Bawendi, “Room-temperature ordered photon emission from multiexciton states in single CdSe core-shell nanocrystals,” Phys. Rev. Lett.94(8), 087403 (2005).
[CrossRef] [PubMed]

Y. S. Park, A. V. Malko, J. Vela, Y. Chen, Y. Ghosh, F. García-Santamaría, J. A. Hollingsworth, V. I. Klimov, and H. Htoon, “Near-unity quantum yields of biexciton emission from CdSe/CdS nanocrystals measured using single-particle spectroscopy,” Phys. Rev. Lett.106(18), 187401 (2011).
[CrossRef] [PubMed]

R. Osovsky, D. Cheskis, V. Kloper, A. Sashchiuk, M. Kroner, and E. Lifshitz, “Continuous-wave pumping of multiexciton bands in the photoluminescence spectrum of a single CdTe-CdSe core-shell colloidal quantum dot,” Phys. Rev. Lett.102(19), 197401 (2009).
[CrossRef] [PubMed]

E. Moreau, I. Robert, L. Manin, V. Thierry-Mieg, J. M. Gérard, and I. Abram, “Quantum cascade of photons in semiconductor quantum dots,” Phys. Rev. Lett.87(18), 183601 (2001).
[CrossRef]

T. Basché, W. E. Moerner, M. Orrit, and H. Talon, “Photon antibunching in the fluorescence of a single dye molecule trapped in a solid,” Phys. Rev. Lett.69(10), 1516–1519 (1992).
[CrossRef] [PubMed]

A. Högele, C. Galland, M. Winger, and A. Imamoğlu, “Photon antibunching in the photoluminescence spectra of a single carbon nanotube,” Phys. Rev. Lett.100(21), 217401 (2008).
[CrossRef] [PubMed]

C. Kurtsiefer, S. Mayer, P. Zarda, and H. Weinfurter, “Stable solid-state source of single photons,” Phys. Rev. Lett.85(2), 290–293 (2000).
[CrossRef] [PubMed]

J. Zhao, G. Nair, B. R. Fisher, and M. G. Bawendi, “Challenge to the charging model of semiconductor-nanocrystal fluorescence intermittency from off-state quantum yields and multiexciton blinking,” Phys. Rev. Lett.104(15), 157403 (2010).
[CrossRef] [PubMed]

R. D. Schaller and V. I. Klimov, “High efficiency carrier multiplication in PbSe nanocrystals: Implications for solar energy conversion,” Phys. Rev. Lett.92(18), 186601 (2004).
[CrossRef] [PubMed]

A. Muller, W. Fang, J. Lawall, and G. S. Solomon, “Creating polarization-entangled photon pairs from a semiconductor quantum dot using the optical Stark effect,” Phys. Rev. Lett.103(21), 217402 (2009).
[CrossRef] [PubMed]

Science (3)

V. I. Klimov, A. A. Mikhailovsky, D. W. McBranch, C. A. Leatherdale, and M. G. Bawendi, “Quantization of multiparticle Auger rates in semiconductor quantum dots,” Science287(5455), 1011–1013 (2000).
[CrossRef] [PubMed]

P. Michler, A. Kiraz, C. Becher, W. V. Schoenfeld, P. M. Petroff, L. Zhang, E. Hu, and A. Imamoglu, “A quantum dot single-photon turnstile device,” Science290(5500), 2282–2285 (2000).
[CrossRef] [PubMed]

V. I. Klimov, A. A. Mikhailovsky, S. Xu, A. Malko, J. A. Hollingsworth, C. A. Leatherdale, H.-J. Eisler, and M. G. Bawendi, “Optical gain and stimulated emission in nanocrystal quantum dots,” Science290(5490), 314–317 (2000).
[CrossRef] [PubMed]

Other (2)

W. Becker, Advanced Time-Correlated Single Photon Counting Techniques Chemical Physics (Springer, 2005).

Due to very high QBX, then second g-NQD shows a bi-exponential decay even at very low pump power. The fast time constant of the PL decay 23.78 ns is in good agreement with 22.9ns τBX extracted from the decay of RTG.”

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Figures (3)

Fig. 1
Fig. 1

Schematic of TCSPC implementations. (a) TCSPC setup allowing for hardware-implemented time-gating. (b) TCSPC setup allowing for software-implemented time-gating. (c) Details of TCSPC calculations. Photon arrival times are indicated by red circles while laser pulses are denoted by blue stars. PL lifetimes are determined by histogramming t values. Time-gating is implemented by using only photons arriving within the time-gated region, depicted by the yellow boxes. The gate-delay time (GDT) is also indicated. Anti-bunching plots are built up by histogramming the time differences, ΔT, between photons arriving on opposing channels.

Fig. 2
Fig. 2

Single NQD data. Panels (a)-(d) and (e)-(h) correspond to different measurements/data sets. (a) PL lifetime from a single detector channel. Dash line: single exponential fit with time constant of 124 ns. (b) Standard g(2) plot before time-gating. R = 0.50 (c) Plot of RTG vs. GDT. Notice that the first 25 ns (before t = 0) are flat, this corresponds to the time before the sync pulse, due to the electronic delay in the system as is also seen in all lifetime plots. (d) g(2) plot after time gating has been applied (GDT = 75 ns, RTG(75) = 0.05). Note that most if this is due to cross-talk (sharp central spikes). (e) PL lifetime from a single detector channel. Dash line: double exponential fit with time constant of 23.7 and 110.5 ns. (f) Standard g(2) plot before time-gating. R = 0.73 (g) Plot of RTG as a function of GDT. (h) g(2) plot after time gating has been applied (GDT = 75 ns, RTG(7 5) = 0.13).

Fig. 3
Fig. 3

Single NQD data. (a) PL lifetime from a single detector channel. (b) Standard g(2) plot, no time gating (R = 0.73). (c) Plot of RTG vs. GDT. (d) g(2) plot after time gating has been applied (GDT = 75 ns, RTG(75) = 0.28).

Equations (5)

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

R= ( m1 ) Q X + Q BX m Q X .
lim GDT R TG = ( m1 ) m .
R TG ( GDT )=R e ( GDT α )
1/α =1/ τ BX 2/ τ X ,
R TG ( GDT )=R e ( GDT β τ X ) ,

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