Abstract

We present a novel process for the production of three-layer Composite Nanoparticles (CNPs) in the size range 100–300 nm with an up-converting phosphor interior, a coating of porphyrin photosensitizer, and a biocompatible PEG outer layer to prevent clearance by the reticuloendothelial system. We show that these CNPs produce millimolar amounts of singlet oxygen at NIR intensities far less than other two-photon techniques.

© 2009 Optical Society of America

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  1. S. Heer, K. Kompe, H. U. Gudel, and M. Haase, "Highly efficient multicolour upconversion emission in transparent colloids of lanthanide-doped NaYF4 nanocrystals," Adv. Mat. 16, 2102-+ (2004).
    [CrossRef]
  2. K. Kuningas, T. Rantanen, U. Karhunen, T. Lovgren, and T. Soukka, "Simultaneous use of time-resolved fluorescence and anti-stokes photoluminescence in a bioaffinity assay," Anal. Chem. 77, 2826-2834 (2005).
    [CrossRef] [PubMed]
  3. K. van de Rijke, H. Zijlmans, S. V. Li, T. A. K. Raap, R. S. Niedbala, and H. J. Tanke, "Up-converting phosphor reporters for nucleic acid microarrays," Nature Biotech. 19, 273-276 (2001).
    [CrossRef]
  4. M. Zuiderwijk, H. J. Tanke, R. S. Niedbala, and P. Corstjens, "An amplification-free hybridization-based DNA assay to detect Streptococcus pneumoniae utilizing the up-conversion phosphor technology," Clin. Biochem. 36, 401-403 (2003).
    [CrossRef] [PubMed]
  5. S. F. Lim, R. Riehn, W. S. Ryu, N. Khanarian, C. K. Tung, D. Tank, and R. H. Austin, "In vivo and scanning electron microscopy imaging of upconverting nanophosphors in Caenorhabditis elegans," Nano Lett.6-2 (2006).
  6. V. P. Torchilin, and V. S. Trubetskoy, "Which Polymers Can Make Nanoparticulate Drug Carriers Long-Circulating," Adv. Drug Del. Rev. 16, 141-155 (1995).
    [CrossRef]
  7. J. Shan and Y. G. Ju, "Synthesis, characterization and SiO2 coating of NaF4Y:Er3+ upconversion nanophosphors using high temperature ligands," Adv. Mat.Submitted (2007).
  8. B. K. Johnson and R. K. Prud'homme, "Flash NanoPrecipitation of organic actives and block copolymers using a confined impinging jets mixer," Australian J. Chem. 56, 1021-1024 (2003).
    [CrossRef]
  9. F. Auzel, "Upconversion and anti-stokes processes with f and d ions in solids," Chem. Rev. 104, 139-173 (2004).
    [CrossRef] [PubMed]
  10. M. J. Moreno, E. Monson, R. G. Reddy, A. Rehemtulla, B. D. Ross, M. Philbert, R. J. Schneider, and R. Kopelman, "Production of singlet oxygen by Ru(dpp(SO3)(2))(3) incorporated in polyacrylamide PEBBLES," Sens. Actuat. B-Chem. 90, 82-89 (2003).
    [CrossRef]
  11. B. A. Lindig, M. A. J. Rodgers, and A. P. Schaap, "Determination of the Lifetime of Singlet Oxygen in D2o Using 9,10-Anthracenedipropionic Acid, a Water-Soluble Probe," J. Am. Chem. Soc. 102, 5590-5593 (1980).
    [CrossRef]
  12. D. K. Chatterjee and Z. Yong, "Upconverting nanoparticles as nanotransducers for photodynamic therapy in cancer cells," Nanomed. 3, 73-82 (2008).
    [CrossRef]
  13. S. M. Ansell, S. A. Johnstone, P. G. Tardi, L. Lo, S. W. Xie, Y. Shu, T. O. Harasym, N. L. Harasym, L. Williams, D. Bermudes, B. D. Liboiron, W. Saad, R. K. Prud'homme, and L. D. Mayer, "Modulating the therapeutic activity of nanoparticle delivered paclitaxel by manipulating the hydrophobicity of prodrug conjugates," J. Med. Chem. 51, 3288-3296 (2008).
    [CrossRef] [PubMed]
  14. P. Zhang, W. Steelant, M. Kumar, and M. Scholfield, "Versatile photosensitizers for photodynamic therapy at infrared excitation," J. Am. Chem. Soc. 129, 4526 (2007).
    [CrossRef] [PubMed]
  15. H. Maeda, J. Fang, T. Inutsuka, and Y. Kitamoto, "Vascular permeability enhancement in solid tumor: various factors, mechanisms involved and its implications," Int. Immunopharm. 3, 319-328 (2003).
    [CrossRef]
  16. M. E. Gindy, S. Ji, T. R. Hoye, A. Z. Panagiotopoulos, and R. K. Prud’homme, "Preparation of Poly(ethylene glycol) Protected Nanoparticles with Variable Bioconjugate Ligand Density," Biomacromol. 9, 2705-2711 (2008).
    [CrossRef]
  17. M. E. Gindy, A. Z. Panagiotopoulos, and R. K. Prud'homme, "Composite block copolymer stabilized nanoparticles: Simultaneous encapsulation of organic actives and inorganic nanostructures," Langmuir 24, 83-90 (2008).
    [CrossRef]
  18. Y. Liu, K. Kathan, W. Saad, and R. K. Prud'homme, "Ostwald ripening of beta-carotene nanoparticles," Phys. Rev. Lett. 98 (2007).
    [PubMed]

2008

D. K. Chatterjee and Z. Yong, "Upconverting nanoparticles as nanotransducers for photodynamic therapy in cancer cells," Nanomed. 3, 73-82 (2008).
[CrossRef]

S. M. Ansell, S. A. Johnstone, P. G. Tardi, L. Lo, S. W. Xie, Y. Shu, T. O. Harasym, N. L. Harasym, L. Williams, D. Bermudes, B. D. Liboiron, W. Saad, R. K. Prud'homme, and L. D. Mayer, "Modulating the therapeutic activity of nanoparticle delivered paclitaxel by manipulating the hydrophobicity of prodrug conjugates," J. Med. Chem. 51, 3288-3296 (2008).
[CrossRef] [PubMed]

M. E. Gindy, S. Ji, T. R. Hoye, A. Z. Panagiotopoulos, and R. K. Prud’homme, "Preparation of Poly(ethylene glycol) Protected Nanoparticles with Variable Bioconjugate Ligand Density," Biomacromol. 9, 2705-2711 (2008).
[CrossRef]

M. E. Gindy, A. Z. Panagiotopoulos, and R. K. Prud'homme, "Composite block copolymer stabilized nanoparticles: Simultaneous encapsulation of organic actives and inorganic nanostructures," Langmuir 24, 83-90 (2008).
[CrossRef]

2007

Y. Liu, K. Kathan, W. Saad, and R. K. Prud'homme, "Ostwald ripening of beta-carotene nanoparticles," Phys. Rev. Lett. 98 (2007).
[PubMed]

P. Zhang, W. Steelant, M. Kumar, and M. Scholfield, "Versatile photosensitizers for photodynamic therapy at infrared excitation," J. Am. Chem. Soc. 129, 4526 (2007).
[CrossRef] [PubMed]

J. Shan and Y. G. Ju, "Synthesis, characterization and SiO2 coating of NaF4Y:Er3+ upconversion nanophosphors using high temperature ligands," Adv. Mat.Submitted (2007).

2006

S. F. Lim, R. Riehn, W. S. Ryu, N. Khanarian, C. K. Tung, D. Tank, and R. H. Austin, "In vivo and scanning electron microscopy imaging of upconverting nanophosphors in Caenorhabditis elegans," Nano Lett.6-2 (2006).

2005

K. Kuningas, T. Rantanen, U. Karhunen, T. Lovgren, and T. Soukka, "Simultaneous use of time-resolved fluorescence and anti-stokes photoluminescence in a bioaffinity assay," Anal. Chem. 77, 2826-2834 (2005).
[CrossRef] [PubMed]

2004

S. Heer, K. Kompe, H. U. Gudel, and M. Haase, "Highly efficient multicolour upconversion emission in transparent colloids of lanthanide-doped NaYF4 nanocrystals," Adv. Mat. 16, 2102-+ (2004).
[CrossRef]

F. Auzel, "Upconversion and anti-stokes processes with f and d ions in solids," Chem. Rev. 104, 139-173 (2004).
[CrossRef] [PubMed]

2003

M. J. Moreno, E. Monson, R. G. Reddy, A. Rehemtulla, B. D. Ross, M. Philbert, R. J. Schneider, and R. Kopelman, "Production of singlet oxygen by Ru(dpp(SO3)(2))(3) incorporated in polyacrylamide PEBBLES," Sens. Actuat. B-Chem. 90, 82-89 (2003).
[CrossRef]

H. Maeda, J. Fang, T. Inutsuka, and Y. Kitamoto, "Vascular permeability enhancement in solid tumor: various factors, mechanisms involved and its implications," Int. Immunopharm. 3, 319-328 (2003).
[CrossRef]

M. Zuiderwijk, H. J. Tanke, R. S. Niedbala, and P. Corstjens, "An amplification-free hybridization-based DNA assay to detect Streptococcus pneumoniae utilizing the up-conversion phosphor technology," Clin. Biochem. 36, 401-403 (2003).
[CrossRef] [PubMed]

B. K. Johnson and R. K. Prud'homme, "Flash NanoPrecipitation of organic actives and block copolymers using a confined impinging jets mixer," Australian J. Chem. 56, 1021-1024 (2003).
[CrossRef]

2001

K. van de Rijke, H. Zijlmans, S. V. Li, T. A. K. Raap, R. S. Niedbala, and H. J. Tanke, "Up-converting phosphor reporters for nucleic acid microarrays," Nature Biotech. 19, 273-276 (2001).
[CrossRef]

1995

V. P. Torchilin, and V. S. Trubetskoy, "Which Polymers Can Make Nanoparticulate Drug Carriers Long-Circulating," Adv. Drug Del. Rev. 16, 141-155 (1995).
[CrossRef]

1980

B. A. Lindig, M. A. J. Rodgers, and A. P. Schaap, "Determination of the Lifetime of Singlet Oxygen in D2o Using 9,10-Anthracenedipropionic Acid, a Water-Soluble Probe," J. Am. Chem. Soc. 102, 5590-5593 (1980).
[CrossRef]

Ansell, S. M.

S. M. Ansell, S. A. Johnstone, P. G. Tardi, L. Lo, S. W. Xie, Y. Shu, T. O. Harasym, N. L. Harasym, L. Williams, D. Bermudes, B. D. Liboiron, W. Saad, R. K. Prud'homme, and L. D. Mayer, "Modulating the therapeutic activity of nanoparticle delivered paclitaxel by manipulating the hydrophobicity of prodrug conjugates," J. Med. Chem. 51, 3288-3296 (2008).
[CrossRef] [PubMed]

Austin, R. H.

S. F. Lim, R. Riehn, W. S. Ryu, N. Khanarian, C. K. Tung, D. Tank, and R. H. Austin, "In vivo and scanning electron microscopy imaging of upconverting nanophosphors in Caenorhabditis elegans," Nano Lett.6-2 (2006).

Auzel, F.

F. Auzel, "Upconversion and anti-stokes processes with f and d ions in solids," Chem. Rev. 104, 139-173 (2004).
[CrossRef] [PubMed]

Bermudes, D.

S. M. Ansell, S. A. Johnstone, P. G. Tardi, L. Lo, S. W. Xie, Y. Shu, T. O. Harasym, N. L. Harasym, L. Williams, D. Bermudes, B. D. Liboiron, W. Saad, R. K. Prud'homme, and L. D. Mayer, "Modulating the therapeutic activity of nanoparticle delivered paclitaxel by manipulating the hydrophobicity of prodrug conjugates," J. Med. Chem. 51, 3288-3296 (2008).
[CrossRef] [PubMed]

Chatterjee, D. K.

D. K. Chatterjee and Z. Yong, "Upconverting nanoparticles as nanotransducers for photodynamic therapy in cancer cells," Nanomed. 3, 73-82 (2008).
[CrossRef]

Corstjens, P.

M. Zuiderwijk, H. J. Tanke, R. S. Niedbala, and P. Corstjens, "An amplification-free hybridization-based DNA assay to detect Streptococcus pneumoniae utilizing the up-conversion phosphor technology," Clin. Biochem. 36, 401-403 (2003).
[CrossRef] [PubMed]

Fang, J.

H. Maeda, J. Fang, T. Inutsuka, and Y. Kitamoto, "Vascular permeability enhancement in solid tumor: various factors, mechanisms involved and its implications," Int. Immunopharm. 3, 319-328 (2003).
[CrossRef]

Gindy, M. E.

M. E. Gindy, S. Ji, T. R. Hoye, A. Z. Panagiotopoulos, and R. K. Prud’homme, "Preparation of Poly(ethylene glycol) Protected Nanoparticles with Variable Bioconjugate Ligand Density," Biomacromol. 9, 2705-2711 (2008).
[CrossRef]

M. E. Gindy, A. Z. Panagiotopoulos, and R. K. Prud'homme, "Composite block copolymer stabilized nanoparticles: Simultaneous encapsulation of organic actives and inorganic nanostructures," Langmuir 24, 83-90 (2008).
[CrossRef]

Gudel, H. U.

S. Heer, K. Kompe, H. U. Gudel, and M. Haase, "Highly efficient multicolour upconversion emission in transparent colloids of lanthanide-doped NaYF4 nanocrystals," Adv. Mat. 16, 2102-+ (2004).
[CrossRef]

Haase, M.

S. Heer, K. Kompe, H. U. Gudel, and M. Haase, "Highly efficient multicolour upconversion emission in transparent colloids of lanthanide-doped NaYF4 nanocrystals," Adv. Mat. 16, 2102-+ (2004).
[CrossRef]

Harasym, N. L.

S. M. Ansell, S. A. Johnstone, P. G. Tardi, L. Lo, S. W. Xie, Y. Shu, T. O. Harasym, N. L. Harasym, L. Williams, D. Bermudes, B. D. Liboiron, W. Saad, R. K. Prud'homme, and L. D. Mayer, "Modulating the therapeutic activity of nanoparticle delivered paclitaxel by manipulating the hydrophobicity of prodrug conjugates," J. Med. Chem. 51, 3288-3296 (2008).
[CrossRef] [PubMed]

Harasym, T. O.

S. M. Ansell, S. A. Johnstone, P. G. Tardi, L. Lo, S. W. Xie, Y. Shu, T. O. Harasym, N. L. Harasym, L. Williams, D. Bermudes, B. D. Liboiron, W. Saad, R. K. Prud'homme, and L. D. Mayer, "Modulating the therapeutic activity of nanoparticle delivered paclitaxel by manipulating the hydrophobicity of prodrug conjugates," J. Med. Chem. 51, 3288-3296 (2008).
[CrossRef] [PubMed]

Heer, S.

S. Heer, K. Kompe, H. U. Gudel, and M. Haase, "Highly efficient multicolour upconversion emission in transparent colloids of lanthanide-doped NaYF4 nanocrystals," Adv. Mat. 16, 2102-+ (2004).
[CrossRef]

Hoye, T. R.

M. E. Gindy, S. Ji, T. R. Hoye, A. Z. Panagiotopoulos, and R. K. Prud’homme, "Preparation of Poly(ethylene glycol) Protected Nanoparticles with Variable Bioconjugate Ligand Density," Biomacromol. 9, 2705-2711 (2008).
[CrossRef]

Inutsuka, T.

H. Maeda, J. Fang, T. Inutsuka, and Y. Kitamoto, "Vascular permeability enhancement in solid tumor: various factors, mechanisms involved and its implications," Int. Immunopharm. 3, 319-328 (2003).
[CrossRef]

Ji, S.

M. E. Gindy, S. Ji, T. R. Hoye, A. Z. Panagiotopoulos, and R. K. Prud’homme, "Preparation of Poly(ethylene glycol) Protected Nanoparticles with Variable Bioconjugate Ligand Density," Biomacromol. 9, 2705-2711 (2008).
[CrossRef]

Johnson, B. K.

B. K. Johnson and R. K. Prud'homme, "Flash NanoPrecipitation of organic actives and block copolymers using a confined impinging jets mixer," Australian J. Chem. 56, 1021-1024 (2003).
[CrossRef]

Johnstone, S. A.

S. M. Ansell, S. A. Johnstone, P. G. Tardi, L. Lo, S. W. Xie, Y. Shu, T. O. Harasym, N. L. Harasym, L. Williams, D. Bermudes, B. D. Liboiron, W. Saad, R. K. Prud'homme, and L. D. Mayer, "Modulating the therapeutic activity of nanoparticle delivered paclitaxel by manipulating the hydrophobicity of prodrug conjugates," J. Med. Chem. 51, 3288-3296 (2008).
[CrossRef] [PubMed]

Ju, Y. G.

J. Shan and Y. G. Ju, "Synthesis, characterization and SiO2 coating of NaF4Y:Er3+ upconversion nanophosphors using high temperature ligands," Adv. Mat.Submitted (2007).

Karhunen, U.

K. Kuningas, T. Rantanen, U. Karhunen, T. Lovgren, and T. Soukka, "Simultaneous use of time-resolved fluorescence and anti-stokes photoluminescence in a bioaffinity assay," Anal. Chem. 77, 2826-2834 (2005).
[CrossRef] [PubMed]

Kathan, K.

Y. Liu, K. Kathan, W. Saad, and R. K. Prud'homme, "Ostwald ripening of beta-carotene nanoparticles," Phys. Rev. Lett. 98 (2007).
[PubMed]

Khanarian, N.

S. F. Lim, R. Riehn, W. S. Ryu, N. Khanarian, C. K. Tung, D. Tank, and R. H. Austin, "In vivo and scanning electron microscopy imaging of upconverting nanophosphors in Caenorhabditis elegans," Nano Lett.6-2 (2006).

Kitamoto, Y.

H. Maeda, J. Fang, T. Inutsuka, and Y. Kitamoto, "Vascular permeability enhancement in solid tumor: various factors, mechanisms involved and its implications," Int. Immunopharm. 3, 319-328 (2003).
[CrossRef]

Kompe, K.

S. Heer, K. Kompe, H. U. Gudel, and M. Haase, "Highly efficient multicolour upconversion emission in transparent colloids of lanthanide-doped NaYF4 nanocrystals," Adv. Mat. 16, 2102-+ (2004).
[CrossRef]

Kopelman, R.

M. J. Moreno, E. Monson, R. G. Reddy, A. Rehemtulla, B. D. Ross, M. Philbert, R. J. Schneider, and R. Kopelman, "Production of singlet oxygen by Ru(dpp(SO3)(2))(3) incorporated in polyacrylamide PEBBLES," Sens. Actuat. B-Chem. 90, 82-89 (2003).
[CrossRef]

Kumar, M.

P. Zhang, W. Steelant, M. Kumar, and M. Scholfield, "Versatile photosensitizers for photodynamic therapy at infrared excitation," J. Am. Chem. Soc. 129, 4526 (2007).
[CrossRef] [PubMed]

Kuningas, K.

K. Kuningas, T. Rantanen, U. Karhunen, T. Lovgren, and T. Soukka, "Simultaneous use of time-resolved fluorescence and anti-stokes photoluminescence in a bioaffinity assay," Anal. Chem. 77, 2826-2834 (2005).
[CrossRef] [PubMed]

Li, S. V.

K. van de Rijke, H. Zijlmans, S. V. Li, T. A. K. Raap, R. S. Niedbala, and H. J. Tanke, "Up-converting phosphor reporters for nucleic acid microarrays," Nature Biotech. 19, 273-276 (2001).
[CrossRef]

Liboiron, B. D.

S. M. Ansell, S. A. Johnstone, P. G. Tardi, L. Lo, S. W. Xie, Y. Shu, T. O. Harasym, N. L. Harasym, L. Williams, D. Bermudes, B. D. Liboiron, W. Saad, R. K. Prud'homme, and L. D. Mayer, "Modulating the therapeutic activity of nanoparticle delivered paclitaxel by manipulating the hydrophobicity of prodrug conjugates," J. Med. Chem. 51, 3288-3296 (2008).
[CrossRef] [PubMed]

Lim, S. F.

S. F. Lim, R. Riehn, W. S. Ryu, N. Khanarian, C. K. Tung, D. Tank, and R. H. Austin, "In vivo and scanning electron microscopy imaging of upconverting nanophosphors in Caenorhabditis elegans," Nano Lett.6-2 (2006).

Lindig, B. A.

B. A. Lindig, M. A. J. Rodgers, and A. P. Schaap, "Determination of the Lifetime of Singlet Oxygen in D2o Using 9,10-Anthracenedipropionic Acid, a Water-Soluble Probe," J. Am. Chem. Soc. 102, 5590-5593 (1980).
[CrossRef]

Liu, Y.

Y. Liu, K. Kathan, W. Saad, and R. K. Prud'homme, "Ostwald ripening of beta-carotene nanoparticles," Phys. Rev. Lett. 98 (2007).
[PubMed]

Lo, L.

S. M. Ansell, S. A. Johnstone, P. G. Tardi, L. Lo, S. W. Xie, Y. Shu, T. O. Harasym, N. L. Harasym, L. Williams, D. Bermudes, B. D. Liboiron, W. Saad, R. K. Prud'homme, and L. D. Mayer, "Modulating the therapeutic activity of nanoparticle delivered paclitaxel by manipulating the hydrophobicity of prodrug conjugates," J. Med. Chem. 51, 3288-3296 (2008).
[CrossRef] [PubMed]

Lovgren, T.

K. Kuningas, T. Rantanen, U. Karhunen, T. Lovgren, and T. Soukka, "Simultaneous use of time-resolved fluorescence and anti-stokes photoluminescence in a bioaffinity assay," Anal. Chem. 77, 2826-2834 (2005).
[CrossRef] [PubMed]

Maeda, H.

H. Maeda, J. Fang, T. Inutsuka, and Y. Kitamoto, "Vascular permeability enhancement in solid tumor: various factors, mechanisms involved and its implications," Int. Immunopharm. 3, 319-328 (2003).
[CrossRef]

Mayer, L. D.

S. M. Ansell, S. A. Johnstone, P. G. Tardi, L. Lo, S. W. Xie, Y. Shu, T. O. Harasym, N. L. Harasym, L. Williams, D. Bermudes, B. D. Liboiron, W. Saad, R. K. Prud'homme, and L. D. Mayer, "Modulating the therapeutic activity of nanoparticle delivered paclitaxel by manipulating the hydrophobicity of prodrug conjugates," J. Med. Chem. 51, 3288-3296 (2008).
[CrossRef] [PubMed]

Monson, E.

M. J. Moreno, E. Monson, R. G. Reddy, A. Rehemtulla, B. D. Ross, M. Philbert, R. J. Schneider, and R. Kopelman, "Production of singlet oxygen by Ru(dpp(SO3)(2))(3) incorporated in polyacrylamide PEBBLES," Sens. Actuat. B-Chem. 90, 82-89 (2003).
[CrossRef]

Moreno, M. J.

M. J. Moreno, E. Monson, R. G. Reddy, A. Rehemtulla, B. D. Ross, M. Philbert, R. J. Schneider, and R. Kopelman, "Production of singlet oxygen by Ru(dpp(SO3)(2))(3) incorporated in polyacrylamide PEBBLES," Sens. Actuat. B-Chem. 90, 82-89 (2003).
[CrossRef]

Niedbala, R. S.

M. Zuiderwijk, H. J. Tanke, R. S. Niedbala, and P. Corstjens, "An amplification-free hybridization-based DNA assay to detect Streptococcus pneumoniae utilizing the up-conversion phosphor technology," Clin. Biochem. 36, 401-403 (2003).
[CrossRef] [PubMed]

K. van de Rijke, H. Zijlmans, S. V. Li, T. A. K. Raap, R. S. Niedbala, and H. J. Tanke, "Up-converting phosphor reporters for nucleic acid microarrays," Nature Biotech. 19, 273-276 (2001).
[CrossRef]

Panagiotopoulos, A. Z.

M. E. Gindy, S. Ji, T. R. Hoye, A. Z. Panagiotopoulos, and R. K. Prud’homme, "Preparation of Poly(ethylene glycol) Protected Nanoparticles with Variable Bioconjugate Ligand Density," Biomacromol. 9, 2705-2711 (2008).
[CrossRef]

M. E. Gindy, A. Z. Panagiotopoulos, and R. K. Prud'homme, "Composite block copolymer stabilized nanoparticles: Simultaneous encapsulation of organic actives and inorganic nanostructures," Langmuir 24, 83-90 (2008).
[CrossRef]

Philbert, M.

M. J. Moreno, E. Monson, R. G. Reddy, A. Rehemtulla, B. D. Ross, M. Philbert, R. J. Schneider, and R. Kopelman, "Production of singlet oxygen by Ru(dpp(SO3)(2))(3) incorporated in polyacrylamide PEBBLES," Sens. Actuat. B-Chem. 90, 82-89 (2003).
[CrossRef]

Prud’homme, R. K.

M. E. Gindy, S. Ji, T. R. Hoye, A. Z. Panagiotopoulos, and R. K. Prud’homme, "Preparation of Poly(ethylene glycol) Protected Nanoparticles with Variable Bioconjugate Ligand Density," Biomacromol. 9, 2705-2711 (2008).
[CrossRef]

Prud'homme, R. K.

M. E. Gindy, A. Z. Panagiotopoulos, and R. K. Prud'homme, "Composite block copolymer stabilized nanoparticles: Simultaneous encapsulation of organic actives and inorganic nanostructures," Langmuir 24, 83-90 (2008).
[CrossRef]

S. M. Ansell, S. A. Johnstone, P. G. Tardi, L. Lo, S. W. Xie, Y. Shu, T. O. Harasym, N. L. Harasym, L. Williams, D. Bermudes, B. D. Liboiron, W. Saad, R. K. Prud'homme, and L. D. Mayer, "Modulating the therapeutic activity of nanoparticle delivered paclitaxel by manipulating the hydrophobicity of prodrug conjugates," J. Med. Chem. 51, 3288-3296 (2008).
[CrossRef] [PubMed]

Y. Liu, K. Kathan, W. Saad, and R. K. Prud'homme, "Ostwald ripening of beta-carotene nanoparticles," Phys. Rev. Lett. 98 (2007).
[PubMed]

B. K. Johnson and R. K. Prud'homme, "Flash NanoPrecipitation of organic actives and block copolymers using a confined impinging jets mixer," Australian J. Chem. 56, 1021-1024 (2003).
[CrossRef]

Raap, T. A. K.

K. van de Rijke, H. Zijlmans, S. V. Li, T. A. K. Raap, R. S. Niedbala, and H. J. Tanke, "Up-converting phosphor reporters for nucleic acid microarrays," Nature Biotech. 19, 273-276 (2001).
[CrossRef]

Rantanen, T.

K. Kuningas, T. Rantanen, U. Karhunen, T. Lovgren, and T. Soukka, "Simultaneous use of time-resolved fluorescence and anti-stokes photoluminescence in a bioaffinity assay," Anal. Chem. 77, 2826-2834 (2005).
[CrossRef] [PubMed]

Reddy, R. G.

M. J. Moreno, E. Monson, R. G. Reddy, A. Rehemtulla, B. D. Ross, M. Philbert, R. J. Schneider, and R. Kopelman, "Production of singlet oxygen by Ru(dpp(SO3)(2))(3) incorporated in polyacrylamide PEBBLES," Sens. Actuat. B-Chem. 90, 82-89 (2003).
[CrossRef]

Rehemtulla, A.

M. J. Moreno, E. Monson, R. G. Reddy, A. Rehemtulla, B. D. Ross, M. Philbert, R. J. Schneider, and R. Kopelman, "Production of singlet oxygen by Ru(dpp(SO3)(2))(3) incorporated in polyacrylamide PEBBLES," Sens. Actuat. B-Chem. 90, 82-89 (2003).
[CrossRef]

Riehn, R.

S. F. Lim, R. Riehn, W. S. Ryu, N. Khanarian, C. K. Tung, D. Tank, and R. H. Austin, "In vivo and scanning electron microscopy imaging of upconverting nanophosphors in Caenorhabditis elegans," Nano Lett.6-2 (2006).

Rodgers, M. A. J.

B. A. Lindig, M. A. J. Rodgers, and A. P. Schaap, "Determination of the Lifetime of Singlet Oxygen in D2o Using 9,10-Anthracenedipropionic Acid, a Water-Soluble Probe," J. Am. Chem. Soc. 102, 5590-5593 (1980).
[CrossRef]

Ross, B. D.

M. J. Moreno, E. Monson, R. G. Reddy, A. Rehemtulla, B. D. Ross, M. Philbert, R. J. Schneider, and R. Kopelman, "Production of singlet oxygen by Ru(dpp(SO3)(2))(3) incorporated in polyacrylamide PEBBLES," Sens. Actuat. B-Chem. 90, 82-89 (2003).
[CrossRef]

Ryu, W. S.

S. F. Lim, R. Riehn, W. S. Ryu, N. Khanarian, C. K. Tung, D. Tank, and R. H. Austin, "In vivo and scanning electron microscopy imaging of upconverting nanophosphors in Caenorhabditis elegans," Nano Lett.6-2 (2006).

Saad, W.

S. M. Ansell, S. A. Johnstone, P. G. Tardi, L. Lo, S. W. Xie, Y. Shu, T. O. Harasym, N. L. Harasym, L. Williams, D. Bermudes, B. D. Liboiron, W. Saad, R. K. Prud'homme, and L. D. Mayer, "Modulating the therapeutic activity of nanoparticle delivered paclitaxel by manipulating the hydrophobicity of prodrug conjugates," J. Med. Chem. 51, 3288-3296 (2008).
[CrossRef] [PubMed]

Y. Liu, K. Kathan, W. Saad, and R. K. Prud'homme, "Ostwald ripening of beta-carotene nanoparticles," Phys. Rev. Lett. 98 (2007).
[PubMed]

Schaap, A. P.

B. A. Lindig, M. A. J. Rodgers, and A. P. Schaap, "Determination of the Lifetime of Singlet Oxygen in D2o Using 9,10-Anthracenedipropionic Acid, a Water-Soluble Probe," J. Am. Chem. Soc. 102, 5590-5593 (1980).
[CrossRef]

Schneider, R. J.

M. J. Moreno, E. Monson, R. G. Reddy, A. Rehemtulla, B. D. Ross, M. Philbert, R. J. Schneider, and R. Kopelman, "Production of singlet oxygen by Ru(dpp(SO3)(2))(3) incorporated in polyacrylamide PEBBLES," Sens. Actuat. B-Chem. 90, 82-89 (2003).
[CrossRef]

Scholfield, M.

P. Zhang, W. Steelant, M. Kumar, and M. Scholfield, "Versatile photosensitizers for photodynamic therapy at infrared excitation," J. Am. Chem. Soc. 129, 4526 (2007).
[CrossRef] [PubMed]

Shan, J.

J. Shan and Y. G. Ju, "Synthesis, characterization and SiO2 coating of NaF4Y:Er3+ upconversion nanophosphors using high temperature ligands," Adv. Mat.Submitted (2007).

Shu, Y.

S. M. Ansell, S. A. Johnstone, P. G. Tardi, L. Lo, S. W. Xie, Y. Shu, T. O. Harasym, N. L. Harasym, L. Williams, D. Bermudes, B. D. Liboiron, W. Saad, R. K. Prud'homme, and L. D. Mayer, "Modulating the therapeutic activity of nanoparticle delivered paclitaxel by manipulating the hydrophobicity of prodrug conjugates," J. Med. Chem. 51, 3288-3296 (2008).
[CrossRef] [PubMed]

Soukka, T.

K. Kuningas, T. Rantanen, U. Karhunen, T. Lovgren, and T. Soukka, "Simultaneous use of time-resolved fluorescence and anti-stokes photoluminescence in a bioaffinity assay," Anal. Chem. 77, 2826-2834 (2005).
[CrossRef] [PubMed]

Steelant, W.

P. Zhang, W. Steelant, M. Kumar, and M. Scholfield, "Versatile photosensitizers for photodynamic therapy at infrared excitation," J. Am. Chem. Soc. 129, 4526 (2007).
[CrossRef] [PubMed]

Tank, D.

S. F. Lim, R. Riehn, W. S. Ryu, N. Khanarian, C. K. Tung, D. Tank, and R. H. Austin, "In vivo and scanning electron microscopy imaging of upconverting nanophosphors in Caenorhabditis elegans," Nano Lett.6-2 (2006).

Tanke, H. J.

M. Zuiderwijk, H. J. Tanke, R. S. Niedbala, and P. Corstjens, "An amplification-free hybridization-based DNA assay to detect Streptococcus pneumoniae utilizing the up-conversion phosphor technology," Clin. Biochem. 36, 401-403 (2003).
[CrossRef] [PubMed]

K. van de Rijke, H. Zijlmans, S. V. Li, T. A. K. Raap, R. S. Niedbala, and H. J. Tanke, "Up-converting phosphor reporters for nucleic acid microarrays," Nature Biotech. 19, 273-276 (2001).
[CrossRef]

Tardi, P. G.

S. M. Ansell, S. A. Johnstone, P. G. Tardi, L. Lo, S. W. Xie, Y. Shu, T. O. Harasym, N. L. Harasym, L. Williams, D. Bermudes, B. D. Liboiron, W. Saad, R. K. Prud'homme, and L. D. Mayer, "Modulating the therapeutic activity of nanoparticle delivered paclitaxel by manipulating the hydrophobicity of prodrug conjugates," J. Med. Chem. 51, 3288-3296 (2008).
[CrossRef] [PubMed]

Torchilin, V. P.

V. P. Torchilin, and V. S. Trubetskoy, "Which Polymers Can Make Nanoparticulate Drug Carriers Long-Circulating," Adv. Drug Del. Rev. 16, 141-155 (1995).
[CrossRef]

Trubetskoy, V. S.

V. P. Torchilin, and V. S. Trubetskoy, "Which Polymers Can Make Nanoparticulate Drug Carriers Long-Circulating," Adv. Drug Del. Rev. 16, 141-155 (1995).
[CrossRef]

Tung, C. K.

S. F. Lim, R. Riehn, W. S. Ryu, N. Khanarian, C. K. Tung, D. Tank, and R. H. Austin, "In vivo and scanning electron microscopy imaging of upconverting nanophosphors in Caenorhabditis elegans," Nano Lett.6-2 (2006).

van de Rijke, K.

K. van de Rijke, H. Zijlmans, S. V. Li, T. A. K. Raap, R. S. Niedbala, and H. J. Tanke, "Up-converting phosphor reporters for nucleic acid microarrays," Nature Biotech. 19, 273-276 (2001).
[CrossRef]

Williams, L.

S. M. Ansell, S. A. Johnstone, P. G. Tardi, L. Lo, S. W. Xie, Y. Shu, T. O. Harasym, N. L. Harasym, L. Williams, D. Bermudes, B. D. Liboiron, W. Saad, R. K. Prud'homme, and L. D. Mayer, "Modulating the therapeutic activity of nanoparticle delivered paclitaxel by manipulating the hydrophobicity of prodrug conjugates," J. Med. Chem. 51, 3288-3296 (2008).
[CrossRef] [PubMed]

Xie, S. W.

S. M. Ansell, S. A. Johnstone, P. G. Tardi, L. Lo, S. W. Xie, Y. Shu, T. O. Harasym, N. L. Harasym, L. Williams, D. Bermudes, B. D. Liboiron, W. Saad, R. K. Prud'homme, and L. D. Mayer, "Modulating the therapeutic activity of nanoparticle delivered paclitaxel by manipulating the hydrophobicity of prodrug conjugates," J. Med. Chem. 51, 3288-3296 (2008).
[CrossRef] [PubMed]

Yong, Z.

D. K. Chatterjee and Z. Yong, "Upconverting nanoparticles as nanotransducers for photodynamic therapy in cancer cells," Nanomed. 3, 73-82 (2008).
[CrossRef]

Zhang, P.

P. Zhang, W. Steelant, M. Kumar, and M. Scholfield, "Versatile photosensitizers for photodynamic therapy at infrared excitation," J. Am. Chem. Soc. 129, 4526 (2007).
[CrossRef] [PubMed]

Zijlmans, H.

K. van de Rijke, H. Zijlmans, S. V. Li, T. A. K. Raap, R. S. Niedbala, and H. J. Tanke, "Up-converting phosphor reporters for nucleic acid microarrays," Nature Biotech. 19, 273-276 (2001).
[CrossRef]

Zuiderwijk, M.

M. Zuiderwijk, H. J. Tanke, R. S. Niedbala, and P. Corstjens, "An amplification-free hybridization-based DNA assay to detect Streptococcus pneumoniae utilizing the up-conversion phosphor technology," Clin. Biochem. 36, 401-403 (2003).
[CrossRef] [PubMed]

Adv. Drug Del. Rev.

V. P. Torchilin, and V. S. Trubetskoy, "Which Polymers Can Make Nanoparticulate Drug Carriers Long-Circulating," Adv. Drug Del. Rev. 16, 141-155 (1995).
[CrossRef]

Adv. Mat.

J. Shan and Y. G. Ju, "Synthesis, characterization and SiO2 coating of NaF4Y:Er3+ upconversion nanophosphors using high temperature ligands," Adv. Mat.Submitted (2007).

S. Heer, K. Kompe, H. U. Gudel, and M. Haase, "Highly efficient multicolour upconversion emission in transparent colloids of lanthanide-doped NaYF4 nanocrystals," Adv. Mat. 16, 2102-+ (2004).
[CrossRef]

Anal. Chem.

K. Kuningas, T. Rantanen, U. Karhunen, T. Lovgren, and T. Soukka, "Simultaneous use of time-resolved fluorescence and anti-stokes photoluminescence in a bioaffinity assay," Anal. Chem. 77, 2826-2834 (2005).
[CrossRef] [PubMed]

Australian J. Chem.

B. K. Johnson and R. K. Prud'homme, "Flash NanoPrecipitation of organic actives and block copolymers using a confined impinging jets mixer," Australian J. Chem. 56, 1021-1024 (2003).
[CrossRef]

Biomacromol.

M. E. Gindy, S. Ji, T. R. Hoye, A. Z. Panagiotopoulos, and R. K. Prud’homme, "Preparation of Poly(ethylene glycol) Protected Nanoparticles with Variable Bioconjugate Ligand Density," Biomacromol. 9, 2705-2711 (2008).
[CrossRef]

Chem. Rev.

F. Auzel, "Upconversion and anti-stokes processes with f and d ions in solids," Chem. Rev. 104, 139-173 (2004).
[CrossRef] [PubMed]

Clin. Biochem.

M. Zuiderwijk, H. J. Tanke, R. S. Niedbala, and P. Corstjens, "An amplification-free hybridization-based DNA assay to detect Streptococcus pneumoniae utilizing the up-conversion phosphor technology," Clin. Biochem. 36, 401-403 (2003).
[CrossRef] [PubMed]

Int. Immunopharm.

H. Maeda, J. Fang, T. Inutsuka, and Y. Kitamoto, "Vascular permeability enhancement in solid tumor: various factors, mechanisms involved and its implications," Int. Immunopharm. 3, 319-328 (2003).
[CrossRef]

J. Am. Chem. Soc.

B. A. Lindig, M. A. J. Rodgers, and A. P. Schaap, "Determination of the Lifetime of Singlet Oxygen in D2o Using 9,10-Anthracenedipropionic Acid, a Water-Soluble Probe," J. Am. Chem. Soc. 102, 5590-5593 (1980).
[CrossRef]

P. Zhang, W. Steelant, M. Kumar, and M. Scholfield, "Versatile photosensitizers for photodynamic therapy at infrared excitation," J. Am. Chem. Soc. 129, 4526 (2007).
[CrossRef] [PubMed]

J. Med. Chem.

S. M. Ansell, S. A. Johnstone, P. G. Tardi, L. Lo, S. W. Xie, Y. Shu, T. O. Harasym, N. L. Harasym, L. Williams, D. Bermudes, B. D. Liboiron, W. Saad, R. K. Prud'homme, and L. D. Mayer, "Modulating the therapeutic activity of nanoparticle delivered paclitaxel by manipulating the hydrophobicity of prodrug conjugates," J. Med. Chem. 51, 3288-3296 (2008).
[CrossRef] [PubMed]

Langmuir

M. E. Gindy, A. Z. Panagiotopoulos, and R. K. Prud'homme, "Composite block copolymer stabilized nanoparticles: Simultaneous encapsulation of organic actives and inorganic nanostructures," Langmuir 24, 83-90 (2008).
[CrossRef]

Nano Lett.

S. F. Lim, R. Riehn, W. S. Ryu, N. Khanarian, C. K. Tung, D. Tank, and R. H. Austin, "In vivo and scanning electron microscopy imaging of upconverting nanophosphors in Caenorhabditis elegans," Nano Lett.6-2 (2006).

Nanomed.

D. K. Chatterjee and Z. Yong, "Upconverting nanoparticles as nanotransducers for photodynamic therapy in cancer cells," Nanomed. 3, 73-82 (2008).
[CrossRef]

Nature Biotech.

K. van de Rijke, H. Zijlmans, S. V. Li, T. A. K. Raap, R. S. Niedbala, and H. J. Tanke, "Up-converting phosphor reporters for nucleic acid microarrays," Nature Biotech. 19, 273-276 (2001).
[CrossRef]

Phys. Rev. Lett.

Y. Liu, K. Kathan, W. Saad, and R. K. Prud'homme, "Ostwald ripening of beta-carotene nanoparticles," Phys. Rev. Lett. 98 (2007).
[PubMed]

Sens. Actuat. B-Chem.

M. J. Moreno, E. Monson, R. G. Reddy, A. Rehemtulla, B. D. Ross, M. Philbert, R. J. Schneider, and R. Kopelman, "Production of singlet oxygen by Ru(dpp(SO3)(2))(3) incorporated in polyacrylamide PEBBLES," Sens. Actuat. B-Chem. 90, 82-89 (2003).
[CrossRef]

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Figures (5)

Fig. 1.
Fig. 1.

Schematic representation of Flash NanoPrecipitation method for assembly of the composite nanoparticles incorporating the highly hydrophobic organic photosensitizer, tetraphenylporphyrin (red), 170-nm hexagonal NaYF4:Er3=,Yb3+ upconversion crystals (green) in a shell consisting of PEG(5k)-b-PCL(7k) amphiphilic block copolymer. All the constituents are initially dissolved or suspended in the organic phase, which is mixed at high speed against a large volume of water (10:1 water:THF), yielding the composite nanoparticle (CNP) structure shown right.

Fig. 2.
Fig. 2.

Particle size distributions (normalized to constant area) for varying ratios of BCP:UCP:TPP in the turbulent micromixer. The initial distribution of the bare UCPs in hexane is the solid green line.

Fig. 3.
Fig. 3.

Emission spectrum for upconversion crystals (lower spectrum) juxtaposed with absorption spectrum of tetraphenylporphine (TPP) photosensitizer (upper spectrum). Both spectra were collected from assembled nanoparticles rather than the components in an organic solvent, though the results were virtually identical for the latter case. Both spectra display strong, sharp peaks with overlap of the emission of the UCP and absorption by the TPP in the 550-nm region.

Fig. 4.
Fig. 4.

Microscopy setup for the singlet oxygen production test using a fluorescent dye assay. Samples containing composite nanoparticles and the fluorescent dye ADPA were loaded into 1-mm wells drilled into glass microscope slides. The dye was imaged epifluorescently, with excitation at 380nm and emission collected from 430–480nm. IR excitation was delivered from below the well, with a 2.5 Watt infrared laser beam focused to a 0.3mm spot. UV and IR excitation light, as well as the visible emissions from the particles were filtered out and only the blue fluorescence signal from the ADPA was recorded for each sample.

Fig. 5.
Fig. 5.

Time course of ADPA bleaching during NIR-exposure. The right panel shows images from the first 98 minutes of testing, with minimal bleaching in the first three frames (no NIR input), and significant bleaching in the subsequent frames. This is illustrated in the curve in the left panel: the UV needed to image the ADPA dye leads to some baseline bleaching, but the ADPA bleaching takes on a markedly different rate under infrared illumination. We use a log-log scale, showing the power-law behavior of the bleaching.

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