In this paper, we developed a novel and efficient method of deterministically organizing colloidal particles on structured surfaces over macroscopic areas. Our approach utilizes integrated solution-based processes of dielectric encapsulation and electrostatic-force-mediated self-assembly, which allow precisely controlled placement of sub-10nm sized particles at single particle resolution. As a specific demonstration, motivated by application to single photon sources, highly ordered 2D arrays of single II–VI semiconductor colloidal quantum dots (QDs) were created by this method. Individually, the QDs display triggered single photon emission at room temperature with characteristic photon antibunching statistics, suggesting a pathway to scalable quantum optical radiative systems.

© 2008 Optical Society of America

1. Y. N. Xia, B. Gates, and S. H. Park, "Fabrication of three-dimensional photonic crystals for use in the spectral region from ultraviolet to near-infrared," J. Lightwave Technol. 17, 1956-1962 (1999). [CrossRef]
2. S. Coe, W.-K. Woo, M. Bawendi, and V. Bulovi, "Electroluminescence from single monolayers of nanocrystals in molecular organic devices," Nature 420, 800-803 (2002). [CrossRef] [PubMed]
3. S.-W. Chung, D. S. Ginger, M. W. Morales, Z. Zhang, V. Chandrasekhar, M. A. Ratner, and C. A. Mirkin, "Top-down meets bottom-up: dip-pen nanolithography and DNA-directed assembly of nanoscale electrical circuits," Small 1, 64-69 (2005). [CrossRef]
4. R. J. Tseng, C. Tsai, L. Ma, J. Ouyang, C. S. Ozkan, and Y. Yang, "Digital memory device based on tobacco mosaic virus conjugated with nanoparticles," Nature Nanotech. 1, 72-77 (2006). [CrossRef]
5. S. Sun, C. B. Murray, D. Weller, L. Folks, and A. Moser, "Monodisperse FePt nanoparticles and ferromagnetic FePt nanocrystal superlattices," Science 287, 1989-1992 (2000). [CrossRef] [PubMed]
6. M. F. Ali,  et al. "DNA hybridization and discrimination of single-nucleotide mismatches using chip-based microbead arrays," Anal. Chem. 75, 4732-4739 (2003). [CrossRef] [PubMed]
7. B. Lounis and M. Orrit, "Single-photon sources," Rep. Prog. Phys. 68, 1129-1179 (2005). [CrossRef]
8. A. J. Shields, "Semiconductor quantum light sources," Nature Photon. 1, 215-223 (2007). [CrossRef]
9. P. Michler, "A quantum dot single-photon turnstile device," Science 290, 2282-2285 (2000). [CrossRef] [PubMed]
10. S. Strauf, P. Michler, M. Klude, D. Hommel, G. Bacher, and A. Forchel, "Quantum optical studies on individual acceptor bound excitons in a semiconductor," Phys. Rev. Lett. 89, 177403 (2002). [CrossRef] [PubMed]
11. C. Kurtsiefer, S. Mayer, P. Zarda, and H. Weinfurter, "Stable solid-state source of single photons," Phys. Rev. Lett. 85, 290-293 (2000). [CrossRef] [PubMed]
12. P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and F. K. Buratoo, "Quantum correlation among photons from a single quantum dot at room temperature," Nature 406, 968-970 (2000). [CrossRef] [PubMed]
13. C. B. Murray, D. J. Norris, and M. G. Bawendi, "Synthesis and characterization of nearly monodisperse CdE (E = S, Se, Te) semiconductor nanocrystallites," J. Am. Chem. Soc. 115, 8706-8715 (1993). [CrossRef]
14. 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," Science 287, 1011-1013 (2000). [CrossRef] [PubMed]
15. L.-W. Wang, M. Califano, A. Zunger, and A. Franceschetti, "Pseudopotential theory of Auger processes in CdSe quantum dots," Phys. Rev. Lett. 91, 056404 (2003). [CrossRef] [PubMed]
16. B. Lounis, H. A. Bechtel, D. Gerion, P. Alivisatos, and W. W. Moerner, "Photon antibunching in single CdSe/ZnS quantum dot fluorescence," Chem. Phys. Lett. 329, 399-404 (2000). [CrossRef]
17. X. Brokmann, E. Giacobino, M. Dahan, and J. P. Hermierb, "Highly efficient triggered emission of single photons by colloidal CdSe/ZnS nanocrystals," Appl. Phys. Lett. 85, 712-714 (2004). [CrossRef]
18. Y. Min, M. Akbulut, K. Kristiansen, Y. Golan, and J. Israelachvili, "The role of interparticle and external forces in nanoparticle assembly," Nature Mater. 7, 527-538 (2008). [CrossRef]
19. Y. Yin, Y. Lu, B. Gates, and Y. Xia, "Template-assisted self-assembly: a practical route to complex aggregates of monodispersed colloids with well-defined sizes, shapes, and structures," J. Am. Chem. Soc. 123, 8718-8729 (2001). [CrossRef] [PubMed]
20. Y. Cui, M. T. Björk, J. A. Liddle, C. Sönnichsen, B. Boussert, and A. P. Alivisatos, "Integration of colloidal nanocrystals into lithographically patterned devices," Nano. Lett.,  4, 1093-1098 (2004). [CrossRef]
21. T. Kraus, L. Malaquin, H. Schmid, W. Riess, N. D. Spencer, and H. Wolf, "Nanoparticle printing with single-particle resolution," Nature Nanotech. 2, 570-576 (2007). [CrossRef]
22. R. Xie, U. Kolb, J. Li, T. Basche, and A. Mews, "Synthesis and Characterization of Highly Luminescent CdSe-Core CdS/Zn0.5Cd0.5S/ZnS Multishell Nanocrystals," J. Am. Chem. Soc. 127, 7480-7488 (2005). [CrossRef] [PubMed]
23. J. J. Li, Y. A. Wang, W. Z. Guo, J. C. Keay, T. D. Mishima, M. B. Johnson, and X. P. Peng, "Large-scale synthesis of nearly monodisperse CdSe/CdS core/shell nanocrystals using air-stable reagents via successive ion layer adsorption and reaction," J. Am. Chem. Soc. 125, 12567-12575 (2003). [CrossRef] [PubMed]
24. B. Mahler, P. Spinicelli, S. Buil, X. Quelin, J.-P. Hermier, and B. Dubertret, "Towards non-blinking colloidal quantum dots," Nature Mater. 7, 659-664 (2008). [CrossRef]
25. F. J. Arriagada and K. Osseo-Asare, "Synthesis of nanosize silica in a nonionic water-in-oil microemulsion: effects of the water/surfactant molar ratio and ammonia concentration," J. Colloid Interface Sci. 211, 210-220 (1999). [CrossRef] [PubMed]
26. P. L. Luisi, and B. E. Straub, Reverse Micelles (Plenum, New York, 1984).
27. S. T. Selvan, T. T. Tan, and J. Y. Ying, "Robust, non-cytotoxic, silica-coated CdSe quantum dots with efficient photoluminescence," Adv. Mater. 17, 1620-1625 (2005). [CrossRef]
28. M. Darbandi, R. Thomann, and T. Nann, "Single quantum dots in silica spheres by microemulsion synthesis," Chem. Mater. 17, 5720-5725 (2005). [CrossRef]
29. D. K. Yi, S. S. Lee, G. C. Papaefthymiou, and J. Y. Ying, "Nanoparticle architectures templated by SiO2/Fe2O3 nanocomposites," Chem. Mater. 18, 614-619 (2006). [CrossRef]
30. J. Aizenberg, P. V. Braun, and P. Wiltzius, "Patterned colloidal deposition controlled by electrostatic and capillary forces," Phys. Rev. Lett. 84, 2997-3000 (2000). [CrossRef] [PubMed]
31. R. J. Mashl, N. Grǿnbech-Jensen, M. R. Fitzsimmons, M. Lütt, and D. Li, "Theoretical and experimental adsorption studies of polyelectrolytes on an oppositely charged surface," J. Chem. Phys. 110, 2219-2225 (1999). [CrossRef]
32. S. A. Empedocles, R. Neuhauser, K. Shimizu, and M. G. Bawendi, "Photoluminescence from single semiconductor nanostructures," Adv. Mater. 11, 1243-1256 (1999). [CrossRef]

Adv. Mater.

• S. T. Selvan, T. T. Tan, and J. Y. Ying, "Robust, non-cytotoxic, silica-coated CdSe quantum dots with efficient photoluminescence," Adv. Mater. 17, 1620-1625 (2005). [CrossRef]
• S. A. Empedocles, R. Neuhauser, K. Shimizu, and M. G. Bawendi, "Photoluminescence from single semiconductor nanostructures," Adv. Mater. 11, 1243-1256 (1999). [CrossRef]

Anal. Chem.

• M. F. Ali,  et al. "DNA hybridization and discrimination of single-nucleotide mismatches using chip-based microbead arrays," Anal. Chem. 75, 4732-4739 (2003). [CrossRef] [PubMed]

Appl. Phys. Lett.

• X. Brokmann, E. Giacobino, M. Dahan, and J. P. Hermierb, "Highly efficient triggered emission of single photons by colloidal CdSe/ZnS nanocrystals," Appl. Phys. Lett. 85, 712-714 (2004). [CrossRef]

Chem. Mater.

• M. Darbandi, R. Thomann, and T. Nann, "Single quantum dots in silica spheres by microemulsion synthesis," Chem. Mater. 17, 5720-5725 (2005). [CrossRef]
• D. K. Yi, S. S. Lee, G. C. Papaefthymiou, and J. Y. Ying, "Nanoparticle architectures templated by SiO2/Fe2O3 nanocomposites," Chem. Mater. 18, 614-619 (2006). [CrossRef]

Chem. Phys. Lett.

• B. Lounis, H. A. Bechtel, D. Gerion, P. Alivisatos, and W. W. Moerner, "Photon antibunching in single CdSe/ZnS quantum dot fluorescence," Chem. Phys. Lett. 329, 399-404 (2000). [CrossRef]

J. Am. Chem. Soc.

• Y. Yin, Y. Lu, B. Gates, and Y. Xia, "Template-assisted self-assembly: a practical route to complex aggregates of monodispersed colloids with well-defined sizes, shapes, and structures," J. Am. Chem. Soc. 123, 8718-8729 (2001). [CrossRef] [PubMed]
• R. Xie, U. Kolb, J. Li, T. Basche, and A. Mews, "Synthesis and Characterization of Highly Luminescent CdSe-Core CdS/Zn0.5Cd0.5S/ZnS Multishell Nanocrystals," J. Am. Chem. Soc. 127, 7480-7488 (2005). [CrossRef] [PubMed]
• J. J. Li, Y. A. Wang, W. Z. Guo, J. C. Keay, T. D. Mishima, M. B. Johnson, and X. P. Peng, "Large-scale synthesis of nearly monodisperse CdSe/CdS core/shell nanocrystals using air-stable reagents via successive ion layer adsorption and reaction," J. Am. Chem. Soc. 125, 12567-12575 (2003). [CrossRef] [PubMed]
• C. B. Murray, D. J. Norris, and M. G. Bawendi, "Synthesis and characterization of nearly monodisperse CdE (E = S, Se, Te) semiconductor nanocrystallites," J. Am. Chem. Soc. 115, 8706-8715 (1993). [CrossRef]

J. Chem. Phys.

• R. J. Mashl, N. Grǿnbech-Jensen, M. R. Fitzsimmons, M. Lütt, and D. Li, "Theoretical and experimental adsorption studies of polyelectrolytes on an oppositely charged surface," J. Chem. Phys. 110, 2219-2225 (1999). [CrossRef]

J. Colloid Interface Sci.

• F. J. Arriagada and K. Osseo-Asare, "Synthesis of nanosize silica in a nonionic water-in-oil microemulsion: effects of the water/surfactant molar ratio and ammonia concentration," J. Colloid Interface Sci. 211, 210-220 (1999). [CrossRef] [PubMed]

J. Lightwave Technol.

• Y. N. Xia, B. Gates, and S. H. Park, "Fabrication of three-dimensional photonic crystals for use in the spectral region from ultraviolet to near-infrared," J. Lightwave Technol. 17, 1956-1962 (1999). [CrossRef]

Nano. Lett.

• Y. Cui, M. T. Björk, J. A. Liddle, C. Sönnichsen, B. Boussert, and A. P. Alivisatos, "Integration of colloidal nanocrystals into lithographically patterned devices," Nano. Lett.,  4, 1093-1098 (2004). [CrossRef]

Nature

• S. Coe, W.-K. Woo, M. Bawendi, and V. Bulovi, "Electroluminescence from single monolayers of nanocrystals in molecular organic devices," Nature 420, 800-803 (2002). [CrossRef] [PubMed]
• P. Michler, A. Imamoglu, M. D. Mason, P. J. Carson, G. F. Strouse, and F. K. Buratoo, "Quantum correlation among photons from a single quantum dot at room temperature," Nature 406, 968-970 (2000). [CrossRef] [PubMed]

Nature Mater.

• Y. Min, M. Akbulut, K. Kristiansen, Y. Golan, and J. Israelachvili, "The role of interparticle and external forces in nanoparticle assembly," Nature Mater. 7, 527-538 (2008). [CrossRef]
• B. Mahler, P. Spinicelli, S. Buil, X. Quelin, J.-P. Hermier, and B. Dubertret, "Towards non-blinking colloidal quantum dots," Nature Mater. 7, 659-664 (2008). [CrossRef]

Nature Nanotech.

• T. Kraus, L. Malaquin, H. Schmid, W. Riess, N. D. Spencer, and H. Wolf, "Nanoparticle printing with single-particle resolution," Nature Nanotech. 2, 570-576 (2007). [CrossRef]
• R. J. Tseng, C. Tsai, L. Ma, J. Ouyang, C. S. Ozkan, and Y. Yang, "Digital memory device based on tobacco mosaic virus conjugated with nanoparticles," Nature Nanotech. 1, 72-77 (2006). [CrossRef]

Nature Photon.

• A. J. Shields, "Semiconductor quantum light sources," Nature Photon. 1, 215-223 (2007). [CrossRef]

Phys. Rev. Lett.

• L.-W. Wang, M. Califano, A. Zunger, and A. Franceschetti, "Pseudopotential theory of Auger processes in CdSe quantum dots," Phys. Rev. Lett. 91, 056404 (2003). [CrossRef] [PubMed]
• S. Strauf, P. Michler, M. Klude, D. Hommel, G. Bacher, and A. Forchel, "Quantum optical studies on individual acceptor bound excitons in a semiconductor," Phys. Rev. Lett. 89, 177403 (2002). [CrossRef] [PubMed]
• C. Kurtsiefer, S. Mayer, P. Zarda, and H. Weinfurter, "Stable solid-state source of single photons," Phys. Rev. Lett. 85, 290-293 (2000). [CrossRef] [PubMed]
• J. Aizenberg, P. V. Braun, and P. Wiltzius, "Patterned colloidal deposition controlled by electrostatic and capillary forces," Phys. Rev. Lett. 84, 2997-3000 (2000). [CrossRef] [PubMed]

Rep. Prog. Phys.

• B. Lounis and M. Orrit, "Single-photon sources," Rep. Prog. Phys. 68, 1129-1179 (2005). [CrossRef]

Science

• P. Michler, "A quantum dot single-photon turnstile device," Science 290, 2282-2285 (2000). [CrossRef] [PubMed]
• S. Sun, C. B. Murray, D. Weller, L. Folks, and A. Moser, "Monodisperse FePt nanoparticles and ferromagnetic FePt nanocrystal superlattices," Science 287, 1989-1992 (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," Science 287, 1011-1013 (2000). [CrossRef] [PubMed]

Small

• S.-W. Chung, D. S. Ginger, M. W. Morales, Z. Zhang, V. Chandrasekhar, M. A. Ratner, and C. A. Mirkin, "Top-down meets bottom-up: dip-pen nanolithography and DNA-directed assembly of nanoscale electrical circuits," Small 1, 64-69 (2005). [CrossRef]

Other

• P. L. Luisi, and B. E. Straub, Reverse Micelles (Plenum, New York, 1984).

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