Abstract

Understanding the skin penetration of nanoparticles (NPs) is an important concern due to the increasing presence of NPs in consumer products, including cosmetics. Technical challenges have slowed progress in evaluating skin barrier and NP factors that contribute to skin penetration risk. To limit sampling error and other problems associated with histological processing, many researchers are implementing whole tissue confocal or multiphoton microscopies. This work introduces a fluorescence and reflectance confocal microscopy system that utilizes near-IR excitation and emission to detect near-IR lead sulfide quantum dots (QDs) through ex vivo human epidermis. We provide a detailed prediction and experimental analysis of QD detection sensitivity and demonstrate detection of QD skin penetration in a barrier disrupted model. The unique properties of near-IR lead-based QDs will enable future studies that examine the impact of further barrier-disrupting agents on skin penetration of QDs and elucidate mechanistic insight into QD tissue interactions at the cellular level.

© 2011 OSA

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  1. R. Alvarez-Román, A. Naik, Y. N. Kalia, H. Fessi, and R. H. Guy, “Visualization of skin penetration using confocal laser scanning microscopy,” Eur. J. Pharm. Biopharm. 58(2), 301–316 (2004).
    [CrossRef] [PubMed]
  2. R. Alvarez-Román, A. Naik, Y. N. Kalia, R. H. Guy, and H. Fessi, “Skin penetration and distribution of polymeric nanoparticles,” J. Control. Release 99(1), 53–62 (2004).
    [CrossRef] [PubMed]
  3. X. Wu, P. Griffin, G. J. Price, and R. H. Guy, “Preparation and in vitro evaluation of topical formulations based on polystyrene-poly-2-hydroxyl methacrylate nanoparticles,” Mol. Pharmacol. 6(5), 1449–1456 (2009).
    [CrossRef]
  4. A. V. Zvyagin, X. Zhao, A. Gierden, W. Sanchez, J. A. Ross, and M. S. Roberts, “Imaging of zinc oxide nanoparticle penetration in human skin in vitro and in vivo,” J. Biomed. Opt. 13(6), 064031 (2008).
    [CrossRef]
  5. J. Moger, B. D. Johnston, and C. R. Tyler, “Imaging metal oxide nanoparticles in biological structures with CARS microscopy,” Opt. Express 16(5), 3408–3419 (2008).
    [CrossRef] [PubMed]
  6. L. J. Mortensen, G. Oberdorster, A. P. Pentland, and L. A. DeLouise, “In vivo skin penetration of quantum dot nanoparticles in the murine model: the effect of UVR,” Nano Lett. 8(9), 2779–2787 (2008).
    [CrossRef] [PubMed]
  7. L. W. Zhang and N. A. Monteiro-Riviere, “Assessment of quantum dot penetration into intact, tape-stripped, abraded and flexed rat skin,” Skin Pharmacol. Appl. 21, 166–180 (2008).
    [CrossRef]
  8. N. V. Gopee, D. W. Roberts, P. Webb, C. R. Cozart, P. H. Siitonen, J. R. Latendresse, A. R. Warbitton, W. W. Yu, V. L. Colvin, N. J. Walker, and P. C. Howard, “Quantitative determination of skin penetration of PEG-coated CdSe quantum dots in dermabraded but not intact SKH-1 hairless mouse skin,” Toxicol. Sci. 111(1), 37–48 (2009).
    [CrossRef] [PubMed]
  9. S. Paliwal, G. K. Menon, and S. Mitragotri, “Low-frequency sonophoresis: ultrastructural basis for stratum corneum permeability assessed using quantum dots,” J. Invest. Dermatol. 126(5), 1095–1101 (2006).
    [CrossRef] [PubMed]
  10. L. J. Mortensen, H. Zheng, R. Faulknor, A. De Benedetto, L. Beck, and L. A. DeLouise, “Increased in vivo skin penetration of quantum dots with UVR and in vitro quantum dot cytotoxicity,” Proc. SPIE 7189, 718919 (2009).
  11. J. Seto, B. Polat, R. Lopez, D. Blankschtein, and R. Langer, “Effects of ultrasound and sodium lauryl sulfate on the transdermal delivery of hydrophilic permeants: comparative in vitro studies with full-thickness and split-thickness pig and human skin,” J. Control. Release 145(1), 26–32 (2010).
    [CrossRef] [PubMed]
  12. H. S. Choi, W. Liu, P. Misra, E. Tanaka, J. P. Zimmer, B. Itty Ipe, M. G. Bawendi, and J. V. Frangioni, “Renal clearance of quantum dots,” Nat. Biotechnol. 25(10), 1165–1170 (2007).
    [CrossRef] [PubMed]
  13. J. A. Fitzpatrick, S. K. Andreko, L. A. Ernst, A. S. Waggoner, B. Ballou, and M. P. Bruchez, “Long-term persistence and spectral blue shifting of quantum dots in vivo,” Nano Lett. 9(7), 2736–2741 (2009).
    [CrossRef] [PubMed]
  14. B. J. Marquis, S. A. Love, K. L. Braun, and C. L. Haynes, “Analytical methods to assess nanoparticle toxicity,” Analyst 134(3), 425–439 (2009).
    [CrossRef] [PubMed]
  15. N. A. Lewinski, V. L. Colvin, and R. A. Drezek, “Cytotoxicity of nanoparticles,” Small 4(1), 26–49 (2008).
    [CrossRef] [PubMed]
  16. P. Rivera Gil, G. Oberdörster, A. Elder, V. Puntes, and W. J. Parak, “Correlating physico-chemical with toxicological properties of nanoparticles: the present and the future,” ACS Nano 4(10), 5527–5531 (2010).
    [CrossRef] [PubMed]
  17. M. J. Bartek, J. A. LaBudde, and H. I. Maibach, “Skin permeability in vivo: comparison in rat, rabbit, pig and man,” J. Invest. Dermatol. 58(3), 114–123 (1972).
    [CrossRef] [PubMed]
  18. T. J. Franz, “Percutaneous absorption on the relevance of in vitro data,” J. Invest. Dermatol. 64(3), 190–195 (1975).
    [CrossRef] [PubMed]
  19. R. L. Bronaugh and R. F. Stewart, “Methods for in vitro percutaneous absorption studies IV: The flow-through diffusion cell,” J. Pharm. Sci. 74(1), 64–67 (1985).
    [CrossRef] [PubMed]
  20. X. Wu, G. J. Price, and R. H. Guy, “Disposition of nanoparticles and an associated lipophilic permeant following topical application to the skin,” Mol. Pharmaceutics 6(5), 1441–1448 (2009).
    [CrossRef]
  21. R. F. Lopez, J. E. Seto, D. Blankschtein, and R. Langer, “Enhancing the transdermal delivery of rigid nanoparticles using the simultaneous application of ultrasound and sodium lauryl sulfate,” Biomaterials 32(3), 933–941 (2011).
    [CrossRef]
  22. M. S. Roberts, M. J. Roberts, T. A. Robertson, W. Sanchez, C. Thörling, Y. Zou, X. Zhao, W. Becker, and A. V. Zvyagin, “In vitro and in vivo imaging of xenobiotic transport in human skin and in the rat liver,” J. Biophotonics 1(6), 478–493 (2008).
    [CrossRef]
  23. D. K. Bird, A. L. Schneider, A. C. Watkinson, B. Finnin, and T. A. Smith, “Navigating transdermal diffusion with multiphoton fluorescence lifetime imaging,” J. Microsc. 230, 61–69 (2008).
    [CrossRef] [PubMed]
  24. T.-R. Kuo, C.-L. Wu, C.-T. Hsu, W. Lo, S.-J. Chiang, S.-J. Lin, C.-Y. Dong, and C.-C. Chen, “Chemical enhancer induced changes in the mechanisms of transdermal delivery of zinc oxide nanoparticles,” Biomaterials 30(16), 3002–3008 (2009).
    [CrossRef] [PubMed]
  25. M. Kirillin, M. Shirmanova, M. Sirotkina, M. Bugrova, B. Khlebtsov, and E. Zagaynova, “Contrasting properties of gold nanoshells and titanium dioxide nanoparticles for optical coherence tomography imaging of skin: Monte Carlo simulations and in vivo study,” J. Biomed. Opt. 14(2), 021017 (2009).
    [CrossRef] [PubMed]
  26. M. Sirotkina, M. Shirmanova, M. Bugrova, V. Elagin, P. Agrba, M. Kirillin, V. Kamensky, and E. Zagaynova, “Continuous optical coherence tomography monitoring of nanoparticles accumulation in biological tissues,” J. Nanopart. Res. 13(1), 283–291 (2010).
    [CrossRef]
  27. X. He, K. Wang, and Z. Cheng, “In vivo near-infrared fluorescence imaging of cancer with nanoparticle-based probes,” WIREs Nanomed. Nanobiotechnol. 2(4), 349–366 (2010).
    [CrossRef]
  28. H. S. Choi, B. Itty Ipe, P. Misra, J. H. Lee, M. G. Bawendi, and J. V. Frangioni, “Tissue- and organ-selective biodistribution of NIR fluorescent quantum dots,” Nano Lett. 9(6), 2354–2359 (2009).
    [CrossRef] [PubMed]
  29. H. S. Choi, W. Liu, F. Liu, K. Nasr, P. Misra, M. G. Bawendi, and J. V. Frangioni, “Design considerations for tumour-targeted nanoparticles,” Nat. Nanotechnol. 5(1), 42–47 (2010).
    [CrossRef]
  30. M. Rajadhyaksha, S. Gonzalez, J. Zavislan, R. R. Anderson, and R. Webb, “In vivo confocal scanning laser microscopy of human skin II: advances in instrumentation and comparison with histology,” J. Invest. Dermatol. 113, 293–303 (1999).
    [CrossRef] [PubMed]
  31. Z. Wang, C. E. Glazowski, and J. M. Zavislan, “Modulation transfer function measurement of scanning reflectance microscopes,” J. Biomed. Opt. 12(5), 051802 (2007).
    [CrossRef] [PubMed]
  32. S. Empedocles, R. Neuhauser, and M. Bawendi, “Three-dimensional orientation measurements of symmetric single chromophores using polarization microscopy,” Nature 399(6732), 126–130 (1999).
    [CrossRef]
  33. M. J. van Gemert, S. L. Jacques, H. J. Sterenborg, and W. M. Star, “Skin optics,” IEEE Trans. Biomed. Eng. 36(12), 1146–1154 (1989).
    [CrossRef] [PubMed]
  34. S. Nickell, M. Hermann, M. Essenpreis, T. J. Farrell, U. Krämer, and M. S. Patterson, “Anisotropy of light propagation in human skin,” Phys. Med. Biol. 45(10), 2873–2886 (2000).
    [CrossRef] [PubMed]
  35. S. H. Tseng, A. Grant, and A. J. Durkin, “In vivo determination of skin near-infrared optical properties using diffuse optical spectroscopy,” J. Biomed. Opt. 13(1), 014016 (2008).
    [CrossRef] [PubMed]
  36. S. H. Tseng, P. Bargo, A. Durkin, and N. Kollias, “Chromophore concentrations, absorption and scattering properties of human skin in-vivo,” Opt. Express 17, 14599–14617 (2009).
    [CrossRef] [PubMed]
  37. C. K. Hayakawa, E. O. Potma, and V. Venugopalan, “Electric field Monte Carlo simulations of focal field distributions produced by tightly focused laser beams in tissues,” Biomed. Opt. Express 2, 278–290 (2011).
    [CrossRef] [PubMed]
  38. R. R. Anderson and J. A. Parrish, “The optics of human skin,” J. Invest. Dermatol. 77(1), 13–19 (1981).
    [CrossRef] [PubMed]
  39. C. R. Simpson, M. Kohl, M. Essenpreis, and M. Cope, “Near-infrared optical properties of ex vivo human skin and subcutaneous tissues measured using the Monte Carlo inversion technique,” Phys. Med. Biol. 43(9), 2465–2478 (1998).
    [CrossRef] [PubMed]
  40. C. A. Leatherdale, W.-K. Woo, F. V. Mikulec, and M. G. Bawendi, “On the absorption cross section of cdse nanocrystal quantum dots,” J. Phys. Chem. B 106(31), 7619–7622 (2002).
    [CrossRef]
  41. L. Cademartiri, E. Montanari, G. Calestani, A. Migliori, A. Guagliardi, and G. A. Ozin, “Size-dependent extinction coefficients of PbS quantum dots,” J. Am. Chem. Soc. 128(31), 10337–10346 (2006).
    [CrossRef] [PubMed]
  42. B.-R. Hyun, H. Chen, D. A. Rey, F. W. Wise, and C. A. Batt, “Near-infrared fluorescence imaging with water-soluble lead salt quantum dots,” J. Phys. Chem. B 111(20), 5726–5730 (2007).
    [CrossRef] [PubMed]
  43. S. Ravichandran, L. J. Mortensen, and L. A. DeLouise, “Quantification of human skin barrier function and susceptibility to quantum dot skin penetration,” Nanotoxicology Early Online, 1–12 (2010).
    [CrossRef]
  44. T. Dutkiewicz and H. Tyras, “Skin absorption of toluene, styrene, and xylene by man,” Br. J. Ind. Med. 25(3), 243 (1968).
  45. H. Tsuruta, “Percutaneous absorption of organic solvents. III. On the penetration rates of hydrophobic solvents through the excised rat skin,” Ind. Health 20(4), 335–345 (1982).
    [CrossRef] [PubMed]
  46. N. V. Gopee, D. W. Roberts, P. Webb, C. R. Cozart, P. H. Siitonen, A. R. Warbritton, W. W. Yu, V. L. Colvin, N. J. Walker, and P. C. Howard, “Migration of intradermally injected quantum dots to sentinel organs in mice,” Toxicol. Sci. 98(1), 249–257 (2007).
    [CrossRef] [PubMed]
  47. F. F. Larese, F. D’Agostin, M. Crosera, G. Adami, N. Renzi, M. Bovenzi, and G. Maina, “Human skin penetration of silver nanoparticles through intact and damaged skin,” Toxicology 255, 33–37 (2009).
    [CrossRef]
  48. B. Gulson, M. McCall, M. Korsch, L. Gomez, P. Casey, Y. Oytam, A. Taylor, M. McCulloch, J. Trotter, L. Kinsley, and G. Greenoak, “Small amounts of zinc from zinc oxide particles in sunscreens applied outdoors are absorbed through human skin,” Toxicol. Sci. 118(1), 140–149 (2010).
    [CrossRef] [PubMed]

2011 (2)

R. F. Lopez, J. E. Seto, D. Blankschtein, and R. Langer, “Enhancing the transdermal delivery of rigid nanoparticles using the simultaneous application of ultrasound and sodium lauryl sulfate,” Biomaterials 32(3), 933–941 (2011).
[CrossRef]

C. K. Hayakawa, E. O. Potma, and V. Venugopalan, “Electric field Monte Carlo simulations of focal field distributions produced by tightly focused laser beams in tissues,” Biomed. Opt. Express 2, 278–290 (2011).
[CrossRef] [PubMed]

2010 (7)

H. S. Choi, W. Liu, F. Liu, K. Nasr, P. Misra, M. G. Bawendi, and J. V. Frangioni, “Design considerations for tumour-targeted nanoparticles,” Nat. Nanotechnol. 5(1), 42–47 (2010).
[CrossRef]

M. Sirotkina, M. Shirmanova, M. Bugrova, V. Elagin, P. Agrba, M. Kirillin, V. Kamensky, and E. Zagaynova, “Continuous optical coherence tomography monitoring of nanoparticles accumulation in biological tissues,” J. Nanopart. Res. 13(1), 283–291 (2010).
[CrossRef]

X. He, K. Wang, and Z. Cheng, “In vivo near-infrared fluorescence imaging of cancer with nanoparticle-based probes,” WIREs Nanomed. Nanobiotechnol. 2(4), 349–366 (2010).
[CrossRef]

J. Seto, B. Polat, R. Lopez, D. Blankschtein, and R. Langer, “Effects of ultrasound and sodium lauryl sulfate on the transdermal delivery of hydrophilic permeants: comparative in vitro studies with full-thickness and split-thickness pig and human skin,” J. Control. Release 145(1), 26–32 (2010).
[CrossRef] [PubMed]

P. Rivera Gil, G. Oberdörster, A. Elder, V. Puntes, and W. J. Parak, “Correlating physico-chemical with toxicological properties of nanoparticles: the present and the future,” ACS Nano 4(10), 5527–5531 (2010).
[CrossRef] [PubMed]

S. Ravichandran, L. J. Mortensen, and L. A. DeLouise, “Quantification of human skin barrier function and susceptibility to quantum dot skin penetration,” Nanotoxicology Early Online, 1–12 (2010).
[CrossRef]

B. Gulson, M. McCall, M. Korsch, L. Gomez, P. Casey, Y. Oytam, A. Taylor, M. McCulloch, J. Trotter, L. Kinsley, and G. Greenoak, “Small amounts of zinc from zinc oxide particles in sunscreens applied outdoors are absorbed through human skin,” Toxicol. Sci. 118(1), 140–149 (2010).
[CrossRef] [PubMed]

2009 (11)

F. F. Larese, F. D’Agostin, M. Crosera, G. Adami, N. Renzi, M. Bovenzi, and G. Maina, “Human skin penetration of silver nanoparticles through intact and damaged skin,” Toxicology 255, 33–37 (2009).
[CrossRef]

S. H. Tseng, P. Bargo, A. Durkin, and N. Kollias, “Chromophore concentrations, absorption and scattering properties of human skin in-vivo,” Opt. Express 17, 14599–14617 (2009).
[CrossRef] [PubMed]

L. J. Mortensen, H. Zheng, R. Faulknor, A. De Benedetto, L. Beck, and L. A. DeLouise, “Increased in vivo skin penetration of quantum dots with UVR and in vitro quantum dot cytotoxicity,” Proc. SPIE 7189, 718919 (2009).

J. A. Fitzpatrick, S. K. Andreko, L. A. Ernst, A. S. Waggoner, B. Ballou, and M. P. Bruchez, “Long-term persistence and spectral blue shifting of quantum dots in vivo,” Nano Lett. 9(7), 2736–2741 (2009).
[CrossRef] [PubMed]

B. J. Marquis, S. A. Love, K. L. Braun, and C. L. Haynes, “Analytical methods to assess nanoparticle toxicity,” Analyst 134(3), 425–439 (2009).
[CrossRef] [PubMed]

X. Wu, P. Griffin, G. J. Price, and R. H. Guy, “Preparation and in vitro evaluation of topical formulations based on polystyrene-poly-2-hydroxyl methacrylate nanoparticles,” Mol. Pharmacol. 6(5), 1449–1456 (2009).
[CrossRef]

N. V. Gopee, D. W. Roberts, P. Webb, C. R. Cozart, P. H. Siitonen, J. R. Latendresse, A. R. Warbitton, W. W. Yu, V. L. Colvin, N. J. Walker, and P. C. Howard, “Quantitative determination of skin penetration of PEG-coated CdSe quantum dots in dermabraded but not intact SKH-1 hairless mouse skin,” Toxicol. Sci. 111(1), 37–48 (2009).
[CrossRef] [PubMed]

H. S. Choi, B. Itty Ipe, P. Misra, J. H. Lee, M. G. Bawendi, and J. V. Frangioni, “Tissue- and organ-selective biodistribution of NIR fluorescent quantum dots,” Nano Lett. 9(6), 2354–2359 (2009).
[CrossRef] [PubMed]

T.-R. Kuo, C.-L. Wu, C.-T. Hsu, W. Lo, S.-J. Chiang, S.-J. Lin, C.-Y. Dong, and C.-C. Chen, “Chemical enhancer induced changes in the mechanisms of transdermal delivery of zinc oxide nanoparticles,” Biomaterials 30(16), 3002–3008 (2009).
[CrossRef] [PubMed]

M. Kirillin, M. Shirmanova, M. Sirotkina, M. Bugrova, B. Khlebtsov, and E. Zagaynova, “Contrasting properties of gold nanoshells and titanium dioxide nanoparticles for optical coherence tomography imaging of skin: Monte Carlo simulations and in vivo study,” J. Biomed. Opt. 14(2), 021017 (2009).
[CrossRef] [PubMed]

X. Wu, G. J. Price, and R. H. Guy, “Disposition of nanoparticles and an associated lipophilic permeant following topical application to the skin,” Mol. Pharmaceutics 6(5), 1441–1448 (2009).
[CrossRef]

2008 (8)

M. S. Roberts, M. J. Roberts, T. A. Robertson, W. Sanchez, C. Thörling, Y. Zou, X. Zhao, W. Becker, and A. V. Zvyagin, “In vitro and in vivo imaging of xenobiotic transport in human skin and in the rat liver,” J. Biophotonics 1(6), 478–493 (2008).
[CrossRef]

D. K. Bird, A. L. Schneider, A. C. Watkinson, B. Finnin, and T. A. Smith, “Navigating transdermal diffusion with multiphoton fluorescence lifetime imaging,” J. Microsc. 230, 61–69 (2008).
[CrossRef] [PubMed]

S. H. Tseng, A. Grant, and A. J. Durkin, “In vivo determination of skin near-infrared optical properties using diffuse optical spectroscopy,” J. Biomed. Opt. 13(1), 014016 (2008).
[CrossRef] [PubMed]

A. V. Zvyagin, X. Zhao, A. Gierden, W. Sanchez, J. A. Ross, and M. S. Roberts, “Imaging of zinc oxide nanoparticle penetration in human skin in vitro and in vivo,” J. Biomed. Opt. 13(6), 064031 (2008).
[CrossRef]

J. Moger, B. D. Johnston, and C. R. Tyler, “Imaging metal oxide nanoparticles in biological structures with CARS microscopy,” Opt. Express 16(5), 3408–3419 (2008).
[CrossRef] [PubMed]

L. J. Mortensen, G. Oberdorster, A. P. Pentland, and L. A. DeLouise, “In vivo skin penetration of quantum dot nanoparticles in the murine model: the effect of UVR,” Nano Lett. 8(9), 2779–2787 (2008).
[CrossRef] [PubMed]

L. W. Zhang and N. A. Monteiro-Riviere, “Assessment of quantum dot penetration into intact, tape-stripped, abraded and flexed rat skin,” Skin Pharmacol. Appl. 21, 166–180 (2008).
[CrossRef]

N. A. Lewinski, V. L. Colvin, and R. A. Drezek, “Cytotoxicity of nanoparticles,” Small 4(1), 26–49 (2008).
[CrossRef] [PubMed]

2007 (4)

H. S. Choi, W. Liu, P. Misra, E. Tanaka, J. P. Zimmer, B. Itty Ipe, M. G. Bawendi, and J. V. Frangioni, “Renal clearance of quantum dots,” Nat. Biotechnol. 25(10), 1165–1170 (2007).
[CrossRef] [PubMed]

Z. Wang, C. E. Glazowski, and J. M. Zavislan, “Modulation transfer function measurement of scanning reflectance microscopes,” J. Biomed. Opt. 12(5), 051802 (2007).
[CrossRef] [PubMed]

B.-R. Hyun, H. Chen, D. A. Rey, F. W. Wise, and C. A. Batt, “Near-infrared fluorescence imaging with water-soluble lead salt quantum dots,” J. Phys. Chem. B 111(20), 5726–5730 (2007).
[CrossRef] [PubMed]

N. V. Gopee, D. W. Roberts, P. Webb, C. R. Cozart, P. H. Siitonen, A. R. Warbritton, W. W. Yu, V. L. Colvin, N. J. Walker, and P. C. Howard, “Migration of intradermally injected quantum dots to sentinel organs in mice,” Toxicol. Sci. 98(1), 249–257 (2007).
[CrossRef] [PubMed]

2006 (2)

L. Cademartiri, E. Montanari, G. Calestani, A. Migliori, A. Guagliardi, and G. A. Ozin, “Size-dependent extinction coefficients of PbS quantum dots,” J. Am. Chem. Soc. 128(31), 10337–10346 (2006).
[CrossRef] [PubMed]

S. Paliwal, G. K. Menon, and S. Mitragotri, “Low-frequency sonophoresis: ultrastructural basis for stratum corneum permeability assessed using quantum dots,” J. Invest. Dermatol. 126(5), 1095–1101 (2006).
[CrossRef] [PubMed]

2004 (2)

R. Alvarez-Román, A. Naik, Y. N. Kalia, H. Fessi, and R. H. Guy, “Visualization of skin penetration using confocal laser scanning microscopy,” Eur. J. Pharm. Biopharm. 58(2), 301–316 (2004).
[CrossRef] [PubMed]

R. Alvarez-Román, A. Naik, Y. N. Kalia, R. H. Guy, and H. Fessi, “Skin penetration and distribution of polymeric nanoparticles,” J. Control. Release 99(1), 53–62 (2004).
[CrossRef] [PubMed]

2002 (1)

C. A. Leatherdale, W.-K. Woo, F. V. Mikulec, and M. G. Bawendi, “On the absorption cross section of cdse nanocrystal quantum dots,” J. Phys. Chem. B 106(31), 7619–7622 (2002).
[CrossRef]

2000 (1)

S. Nickell, M. Hermann, M. Essenpreis, T. J. Farrell, U. Krämer, and M. S. Patterson, “Anisotropy of light propagation in human skin,” Phys. Med. Biol. 45(10), 2873–2886 (2000).
[CrossRef] [PubMed]

1999 (2)

S. Empedocles, R. Neuhauser, and M. Bawendi, “Three-dimensional orientation measurements of symmetric single chromophores using polarization microscopy,” Nature 399(6732), 126–130 (1999).
[CrossRef]

M. Rajadhyaksha, S. Gonzalez, J. Zavislan, R. R. Anderson, and R. Webb, “In vivo confocal scanning laser microscopy of human skin II: advances in instrumentation and comparison with histology,” J. Invest. Dermatol. 113, 293–303 (1999).
[CrossRef] [PubMed]

1998 (1)

C. R. Simpson, M. Kohl, M. Essenpreis, and M. Cope, “Near-infrared optical properties of ex vivo human skin and subcutaneous tissues measured using the Monte Carlo inversion technique,” Phys. Med. Biol. 43(9), 2465–2478 (1998).
[CrossRef] [PubMed]

1989 (1)

M. J. van Gemert, S. L. Jacques, H. J. Sterenborg, and W. M. Star, “Skin optics,” IEEE Trans. Biomed. Eng. 36(12), 1146–1154 (1989).
[CrossRef] [PubMed]

1985 (1)

R. L. Bronaugh and R. F. Stewart, “Methods for in vitro percutaneous absorption studies IV: The flow-through diffusion cell,” J. Pharm. Sci. 74(1), 64–67 (1985).
[CrossRef] [PubMed]

1982 (1)

H. Tsuruta, “Percutaneous absorption of organic solvents. III. On the penetration rates of hydrophobic solvents through the excised rat skin,” Ind. Health 20(4), 335–345 (1982).
[CrossRef] [PubMed]

1981 (1)

R. R. Anderson and J. A. Parrish, “The optics of human skin,” J. Invest. Dermatol. 77(1), 13–19 (1981).
[CrossRef] [PubMed]

1975 (1)

T. J. Franz, “Percutaneous absorption on the relevance of in vitro data,” J. Invest. Dermatol. 64(3), 190–195 (1975).
[CrossRef] [PubMed]

1972 (1)

M. J. Bartek, J. A. LaBudde, and H. I. Maibach, “Skin permeability in vivo: comparison in rat, rabbit, pig and man,” J. Invest. Dermatol. 58(3), 114–123 (1972).
[CrossRef] [PubMed]

1968 (1)

T. Dutkiewicz and H. Tyras, “Skin absorption of toluene, styrene, and xylene by man,” Br. J. Ind. Med. 25(3), 243 (1968).

Adami, G.

F. F. Larese, F. D’Agostin, M. Crosera, G. Adami, N. Renzi, M. Bovenzi, and G. Maina, “Human skin penetration of silver nanoparticles through intact and damaged skin,” Toxicology 255, 33–37 (2009).
[CrossRef]

Agrba, P.

M. Sirotkina, M. Shirmanova, M. Bugrova, V. Elagin, P. Agrba, M. Kirillin, V. Kamensky, and E. Zagaynova, “Continuous optical coherence tomography monitoring of nanoparticles accumulation in biological tissues,” J. Nanopart. Res. 13(1), 283–291 (2010).
[CrossRef]

Alvarez-Román, R.

R. Alvarez-Román, A. Naik, Y. N. Kalia, H. Fessi, and R. H. Guy, “Visualization of skin penetration using confocal laser scanning microscopy,” Eur. J. Pharm. Biopharm. 58(2), 301–316 (2004).
[CrossRef] [PubMed]

R. Alvarez-Román, A. Naik, Y. N. Kalia, R. H. Guy, and H. Fessi, “Skin penetration and distribution of polymeric nanoparticles,” J. Control. Release 99(1), 53–62 (2004).
[CrossRef] [PubMed]

Anderson, R. R.

M. Rajadhyaksha, S. Gonzalez, J. Zavislan, R. R. Anderson, and R. Webb, “In vivo confocal scanning laser microscopy of human skin II: advances in instrumentation and comparison with histology,” J. Invest. Dermatol. 113, 293–303 (1999).
[CrossRef] [PubMed]

R. R. Anderson and J. A. Parrish, “The optics of human skin,” J. Invest. Dermatol. 77(1), 13–19 (1981).
[CrossRef] [PubMed]

Andreko, S. K.

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S. H. Tseng, P. Bargo, A. Durkin, and N. Kollias, “Chromophore concentrations, absorption and scattering properties of human skin in-vivo,” Opt. Express 17, 14599–14617 (2009).
[CrossRef] [PubMed]

S. H. Tseng, A. Grant, and A. J. Durkin, “In vivo determination of skin near-infrared optical properties using diffuse optical spectroscopy,” J. Biomed. Opt. 13(1), 014016 (2008).
[CrossRef] [PubMed]

Tsuruta, H.

H. Tsuruta, “Percutaneous absorption of organic solvents. III. On the penetration rates of hydrophobic solvents through the excised rat skin,” Ind. Health 20(4), 335–345 (1982).
[CrossRef] [PubMed]

Tyler, C. R.

Tyras, H.

T. Dutkiewicz and H. Tyras, “Skin absorption of toluene, styrene, and xylene by man,” Br. J. Ind. Med. 25(3), 243 (1968).

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M. J. van Gemert, S. L. Jacques, H. J. Sterenborg, and W. M. Star, “Skin optics,” IEEE Trans. Biomed. Eng. 36(12), 1146–1154 (1989).
[CrossRef] [PubMed]

Venugopalan, V.

Waggoner, A. S.

J. A. Fitzpatrick, S. K. Andreko, L. A. Ernst, A. S. Waggoner, B. Ballou, and M. P. Bruchez, “Long-term persistence and spectral blue shifting of quantum dots in vivo,” Nano Lett. 9(7), 2736–2741 (2009).
[CrossRef] [PubMed]

Walker, N. J.

N. V. Gopee, D. W. Roberts, P. Webb, C. R. Cozart, P. H. Siitonen, J. R. Latendresse, A. R. Warbitton, W. W. Yu, V. L. Colvin, N. J. Walker, and P. C. Howard, “Quantitative determination of skin penetration of PEG-coated CdSe quantum dots in dermabraded but not intact SKH-1 hairless mouse skin,” Toxicol. Sci. 111(1), 37–48 (2009).
[CrossRef] [PubMed]

N. V. Gopee, D. W. Roberts, P. Webb, C. R. Cozart, P. H. Siitonen, A. R. Warbritton, W. W. Yu, V. L. Colvin, N. J. Walker, and P. C. Howard, “Migration of intradermally injected quantum dots to sentinel organs in mice,” Toxicol. Sci. 98(1), 249–257 (2007).
[CrossRef] [PubMed]

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X. He, K. Wang, and Z. Cheng, “In vivo near-infrared fluorescence imaging of cancer with nanoparticle-based probes,” WIREs Nanomed. Nanobiotechnol. 2(4), 349–366 (2010).
[CrossRef]

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Z. Wang, C. E. Glazowski, and J. M. Zavislan, “Modulation transfer function measurement of scanning reflectance microscopes,” J. Biomed. Opt. 12(5), 051802 (2007).
[CrossRef] [PubMed]

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N. V. Gopee, D. W. Roberts, P. Webb, C. R. Cozart, P. H. Siitonen, J. R. Latendresse, A. R. Warbitton, W. W. Yu, V. L. Colvin, N. J. Walker, and P. C. Howard, “Quantitative determination of skin penetration of PEG-coated CdSe quantum dots in dermabraded but not intact SKH-1 hairless mouse skin,” Toxicol. Sci. 111(1), 37–48 (2009).
[CrossRef] [PubMed]

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N. V. Gopee, D. W. Roberts, P. Webb, C. R. Cozart, P. H. Siitonen, A. R. Warbritton, W. W. Yu, V. L. Colvin, N. J. Walker, and P. C. Howard, “Migration of intradermally injected quantum dots to sentinel organs in mice,” Toxicol. Sci. 98(1), 249–257 (2007).
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M. Rajadhyaksha, S. Gonzalez, J. Zavislan, R. R. Anderson, and R. Webb, “In vivo confocal scanning laser microscopy of human skin II: advances in instrumentation and comparison with histology,” J. Invest. Dermatol. 113, 293–303 (1999).
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[CrossRef] [PubMed]

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M. Rajadhyaksha, S. Gonzalez, J. Zavislan, R. R. Anderson, and R. Webb, “In vivo confocal scanning laser microscopy of human skin II: advances in instrumentation and comparison with histology,” J. Invest. Dermatol. 113, 293–303 (1999).
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Zhao, X.

A. V. Zvyagin, X. Zhao, A. Gierden, W. Sanchez, J. A. Ross, and M. S. Roberts, “Imaging of zinc oxide nanoparticle penetration in human skin in vitro and in vivo,” J. Biomed. Opt. 13(6), 064031 (2008).
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M. S. Roberts, M. J. Roberts, T. A. Robertson, W. Sanchez, C. Thörling, Y. Zou, X. Zhao, W. Becker, and A. V. Zvyagin, “In vitro and in vivo imaging of xenobiotic transport in human skin and in the rat liver,” J. Biophotonics 1(6), 478–493 (2008).
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H. S. Choi, W. Liu, P. Misra, E. Tanaka, J. P. Zimmer, B. Itty Ipe, M. G. Bawendi, and J. V. Frangioni, “Renal clearance of quantum dots,” Nat. Biotechnol. 25(10), 1165–1170 (2007).
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Zou, Y.

M. S. Roberts, M. J. Roberts, T. A. Robertson, W. Sanchez, C. Thörling, Y. Zou, X. Zhao, W. Becker, and A. V. Zvyagin, “In vitro and in vivo imaging of xenobiotic transport in human skin and in the rat liver,” J. Biophotonics 1(6), 478–493 (2008).
[CrossRef]

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M. S. Roberts, M. J. Roberts, T. A. Robertson, W. Sanchez, C. Thörling, Y. Zou, X. Zhao, W. Becker, and A. V. Zvyagin, “In vitro and in vivo imaging of xenobiotic transport in human skin and in the rat liver,” J. Biophotonics 1(6), 478–493 (2008).
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A. V. Zvyagin, X. Zhao, A. Gierden, W. Sanchez, J. A. Ross, and M. S. Roberts, “Imaging of zinc oxide nanoparticle penetration in human skin in vitro and in vivo,” J. Biomed. Opt. 13(6), 064031 (2008).
[CrossRef]

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M. Kirillin, M. Shirmanova, M. Sirotkina, M. Bugrova, B. Khlebtsov, and E. Zagaynova, “Contrasting properties of gold nanoshells and titanium dioxide nanoparticles for optical coherence tomography imaging of skin: Monte Carlo simulations and in vivo study,” J. Biomed. Opt. 14(2), 021017 (2009).
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L. W. Zhang and N. A. Monteiro-Riviere, “Assessment of quantum dot penetration into intact, tape-stripped, abraded and flexed rat skin,” Skin Pharmacol. Appl. 21, 166–180 (2008).
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[CrossRef] [PubMed]

N. V. Gopee, D. W. Roberts, P. Webb, C. R. Cozart, P. H. Siitonen, A. R. Warbritton, W. W. Yu, V. L. Colvin, N. J. Walker, and P. C. Howard, “Migration of intradermally injected quantum dots to sentinel organs in mice,” Toxicol. Sci. 98(1), 249–257 (2007).
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X. He, K. Wang, and Z. Cheng, “In vivo near-infrared fluorescence imaging of cancer with nanoparticle-based probes,” WIREs Nanomed. Nanobiotechnol. 2(4), 349–366 (2010).
[CrossRef]

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Figures (6)

Fig. 1
Fig. 1

The basic optical design for the system used in these experiments. Reflectance (785 nm) and fluorescence (660 nm excitation) sources are pumped into a laser scanning confocal microscopy system.

Fig. 2
Fig. 2

Pictorial representation of an example normalized emission and absorbance curves (A) for the QDs used in these experiments. To enable imaging in the upright position, the PDMS microwells (B) of 100 μm diameter and 10 μm depth are filled with QDs and clamped as shown (C). Clamping the QD filled PDMS microwells (ii) between coverglass (iii) and a microscope slide (i) allows the imaging of a filled well. The QD signal (λmax =900 nm) can quite clearly be separated from the PDMS well.

Fig. 3
Fig. 3

Estimation of the power needed to be generated by QDs in the focal plane (A). The noise equivalent power (NEP) for the detector is scaled by the peak width of the QDs, the collection angle, and the system components. A clear minimum is observable in the ∼900 nm wavelength emission peak range. Using the measured absorbance to estimate the absorption cross section then allows the minimum laser power needed to achieve NEP on a single QD (note: in practice this is limited by blinking) at a range of laser wavelengths, and it is observed that there is a power minimum at the 600–700 nm wavelength range (B), for which a 660 nm laser line was chosen. When the power limitations of our excitation source is included, the system response to a range of QD concentrations is able to be estimated (C).

Fig. 4
Fig. 4

Signal response of system to QDs across a range of concentrations in the microwell and through ∼100 μm separated human epidermis with a laser power of 3.9 mW at the focal plane. Background noise is also plotted, and is calculated from the same frames as the signal.

Fig. 5
Fig. 5

The behavior of the experimental data follows the model. The improved theoretical sensitivity is expected, as we use idealized versions of the laser beams, QDs, and other components as well as scattering and absorption coefficients from the literature.

Fig. 6
Fig. 6

Skin penetration of 900 nm peak emission PbS QDs in toluene. The reflectance signal close to the surface of the skin is degraded by the highly scattering QDs and toluene barrier disruption (A). However, some cell borders can still be resolved (arrows). The QDs provide a strong fluorescence signal at the same plane (B). When these profiles are plotted, a clear permeation of QDs into the epidermis is observable relative to the collected reflectance signal (C). The ratio of these values at each dose provides a steady-state flux curve determination, whose shape suggests that there is some partitioning of the toluene solvated QDs at the stratum corneum/epidermal junction with a steady release through the epidermis thereafter (C). The average of 6 measurement locations yields a curve exhibiting the average permeation of PbS QDs into the epidermis (D).

Equations (10)

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

T SFP λ i = ( T L λ i ) 8 ( R M λ i ) 4 ( R D λ i ) ( R G λ i ) ( R P λ i ) ( T PB ) 2 ( R PB ) ( A P A B ) ( T Ob )
NEP FPD λ i = ( NEP Detector λ i ) [ ( t dwell ) ( T Ob ) ( T L λ i ) 10 ( R M λ i ) 3 ( R G λ i ) ( R P λ i ) ( T PB ) 2 ( 1 2 R PB ) ] 1
Ω = 2 π ( 1 cos ( arcsin ( NA RI ) ) )
NEP QD = 4 π Ω λ i = 200 λ i = 1600 ( I QD λ i ) ( NEP FPD λ i ) d λ i
NEP QD epi = 4 π Ω λ i = 200 λ i = 1600 ( I QD λ i ) ( NEP FPD λ i ) ( e z ( μ s λ i + μ a λ i ) ) d λ i
C abs = 2303 ɛ λ N A
NEP LFP = ( NEP QD ) ( π ( 0.61 λ L NA ) 2 ) [ ( QY ) ( I DT ) ( C abs ) ] 1
NEP Laser = ( NEP LFP ) ( T SFP λ i ) 1
NEP LFP epi = ( NEP QD - epi ) ( π ( 0.61 λ L NA ) 2 ) [ ( QY ) ( I DT ) ( C abs ) ] - 1
NEP Laser - epi = ( NEP LFP - epi ) ( T SFP λ i ) - 1 ( e z ( μ s λ i + μ a λ i ) )

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