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Optics Express

Optics Express

  • Editor: Andrew M. Weiner
  • Vol. 22, Iss. 15 — Jul. 28, 2014
  • pp: 17782–17790

Potential of multi-photon upconversion emissions for fluorescence diffuse optical imaging

Haichun Liu, Can T. Xu, and Stefan Andersson-Engels  »View Author Affiliations

Optics Express, Vol. 22, Issue 15, pp. 17782-17790 (2014)

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The spatial resolution of fluorescence molecular imaging is a critical issue for the success of the technique in biomedical applications. One important method for increasing the imaging resolution is to utilize multi-photon emissions. In this study, we thoroughly investigate the potential of the multi-photon upconversion emissions from rare-earth-doped upconverting nanoparticles for the improvement in spatial resolution of diffuse optical imaging. It is found that the imaging resolution is increased by a factor of 1.45 through employing two-photon upconversion emission compared with using the linear emission, and can be further elevated by a factor of 1.23 by using three-photon upconversion emission. In addition, we demonstrate that the pulsed excitation approach holds the promise of overcoming the low quantum yield associated with the high-order upconversion emissions.

© 2014 Optical Society of America

OCIS Codes
(160.4670) Materials : Optical materials
(160.5690) Materials : Rare-earth-doped materials
(170.7050) Medical optics and biotechnology : Turbid media
(160.4236) Materials : Nanomaterials

ToC Category:
Imaging Systems

Original Manuscript: April 3, 2014
Revised Manuscript: May 9, 2014
Manuscript Accepted: May 14, 2014
Published: July 15, 2014

Virtual Issues
Vol. 9, Iss. 9 Virtual Journal for Biomedical Optics

Haichun Liu, Can T. Xu, and Stefan Andersson-Engels, "Potential of multi-photon upconversion emissions for fluorescence diffuse optical imaging," Opt. Express 22, 17782-17790 (2014)

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  1. R. Weissleder and U. Mahmood, “Molecular imaging,” Radiology 219, 316–333 (2001). [CrossRef] [PubMed]
  2. C. Xu, W. Zipfel, J. B. Shear, R. M. Williams, and W. W. Webb, “Multiphoton fluorescence excitation: new spectral windows for biological nonlinear microscopy,” Proc. Natl. Acad. Sci. USA 93, 10763–10768 (1996). [CrossRef] [PubMed]
  3. Z. Li and Y. Zhang, “An efficient and user-friendly method for the synthesis of hexagonal-phase NaYF4:Yb, Er/Tm nanocrystals with controllable shape and upconversion fluorescence,” Nanotechnology 19, 345606 (2008). [CrossRef]
  4. F. Auzel, “Upconversion and anti-stokes processes with f and d ions in solids,” Chem. Rev. 104, 139–173 (2004). [CrossRef] [PubMed]
  5. M. Yu, F. Li, Z. Chen, H. Hu, C. Zhan, H. Yang, and C. Huang, “Laser scanning up-conversion luminescence microscopy for imaging cells labeled with rare-earth nanophosphors,” Anal. Chem. 81, 930–935 (2009). [CrossRef] [PubMed]
  6. J. Pichaandi, J.-C. Boyer, K. R. Delaney, and F. C. J. M. van Veggel, “Two-photon upconversion laser (scanning and wide-field) microscopy using Ln3+-doped NaYF4 upconverting nanocrystals: A critical evaluation of their performance and potential in bioimaging,” J. Phys. Chem. C 115, 19054–19064 (2011). [CrossRef]
  7. G. Chen, J. Shen, T. Y. Ohulchanskyy, N. J. Patel, A. Kutikov, Z. Li, J. Song, R. K. Pandey, H. Ågren, P. N. Prasad, and G. Han, “(α-NaYbF4:Tm3+)/CaF2 core/shell nanoparticles with efficient near-infrared to near-infrared up-conversion for high-contrast deep tissue bioimaging,” ACS Nano 6, 8280–8287 (2012). [CrossRef] [PubMed]
  8. Q. Liu, Y. Sun, T. Yang, W. Feng, C. Li, and F. Li, “Sub-10 nm hexagonal lanthanide-doped NaLuF4 upconversion nanocrystals for sensitive bioimaging in vivo,” J. Am. Chem. Soc. 133, 17122–17125 (2011). [CrossRef] [PubMed]
  9. J. Zhou, Z. Liu, and F. Li, “Upconversion nanophosphors for small-animal imaging,” Chem. Soc. Rev. 41, 1323–1349 (2012). [CrossRef]
  10. G. Chen, H. Qiu, P. N. Prasad, and X. Chen, “Upconversion nanoparticles: Design, nanochemistry, and applications in theranostics,” Chem. Rev. DOI: (2014). [CrossRef]
  11. H. Päkkilä, M. Ylihärsilä, S. Lahtinen, L. Hattara, N. Salminen, R. Arppe, M. Lastusaari, P. Saviranta, and T. Soukka, “Quantitative multianalyte microarray immunoassay utilizing upconverting phosphor technology,” Anal. Chem. 84, 8628–8634 (2012). [CrossRef] [PubMed]
  12. F. Wang, D. Banerjee, Y. Liu, X. Chen, and X. Liu, “Upconversion nanoparticles in biological labeling, imaging, and therapy,” Analyst 135, 1839–1854 (2010). [CrossRef] [PubMed]
  13. C. T. Xu, N. Svensson, J. Axelsson, P. Svenmarker, G. Somesfalean, G. Chen, H. Liang, H. Liu, Z. Zhang, and S. Andersson-Engels, “Autofluorescence insensitive imaging using upconverting nanocrystals in scattering media,” Appl. Phys. Lett. 93, 171103 (2008). [CrossRef]
  14. M. Nyk, R. Kumar, T. Y. Ohulchanskyy, E. J. Bergey, and P. N. Prasad, “High contrast in vitro and in vivo photoluminescence bioimaging using near infrared to near infrared up-conversion in Tm3+ and Yb3+ doped fluoride nanophosphors,” Nano Lett. 8, 3834–3838 (2008). [CrossRef] [PubMed]
  15. C. T. Xu, J. Axelsson, and S. Andersson-Engels, “Fluorescence diffuse optical tomography using upconverting nanoparticles,” Appl. Phys. Lett. 94, 251107 (2009). [CrossRef]
  16. H. Liu, C. T. Xu, D. Lindgren, H. Xie, D. Thomas, C. Gundlach, and S. Andersson-Engels, “Balancing power density based quantum yield characterization of upconverting nanoparticles for arbitrary excitation intensities,” Nanoscale 5, 4770–4775 (2013). [CrossRef] [PubMed]
  17. P. Svenmarker, C. T. Xu, and S. Andersson-Engels, “Use of nonlinear upconverting nanoparticles provides increased spatial resolution in fluorescence diffuse imaging,” Opt. Lett. 35, 2789–2791 (2010). [CrossRef] [PubMed]
  18. C. T. Xu, P. Svenmarker, H. Liu, X. Wu, M. E. Messing, L. R. Wallenberg, and S. Andersson-Engels, “High-resolution fluorescence diffuse optical tomography developed with nonlinear upconverting nanoparticles,” ACS Nano 6, 4788–4795 (2012). [CrossRef] [PubMed]
  19. H. Qiu, C. Yang, W. Shao, J. Damasco, X. Wang, H. Ågren, P. N. Prasad, and G. Chen, “Enhanced upconversion luminescence in Yb3+/Tm3+-codoped fluoride active core/active shell/inert shell nanoparticles through directed energy migration,” Nanomaterials 4, 55–68 (2014). [CrossRef]
  20. L. Caillat, B. Hajj, V. Shynkar, L. Michely, D. Chauvat, J. Zyss, and F. Pellé, “Multiphoton upconversion in rare earth doped nanocrystals for sub-diffractive microscopy,” Appl. Phys. Lett. 102, 143114 (2013). [CrossRef]
  21. H.-S. Qian and Y. Zhang, “Synthesis of hexagonal-phase core-shell NaYF4 nanocrystals with tunable upconversion fluorescence,” Langmuir 24, 12123–12125 (2008). [CrossRef] [PubMed]
  22. M. K. G. Jayakumar, N. M. Idris, and Y. Zhang, “Remote activation of biomolecules in deep tissues using near-infrared-to-uv upconversion nanotransducers,” Proc. Natl. Acad. Sci. USA 109, 8483–8488 (2012). [CrossRef] [PubMed]
  23. G. Chen, C. Yang, and P. N. Prasad, “Nanophotonics and nanochemistry: Controlling the excitation dynamics for frequency up- and down-conversion in lanthanide-doped nanoparticles,” Acc. Chem. Res. 46, 1474–1486 (2013). [CrossRef] [PubMed]
  24. W. Zou, C. Visser, J. A. Maduro, M. S. Pshenichnikov, and J. C. Hummelen, “Broadband dye-sensitized upconversion of near-infrared light,” Nat. Photonics 6, 560–564 (2012). [CrossRef]
  25. A. Priyam, N. M. Idris, and Y. Zhang, “Gold nanoshell coated NaYF4 nanoparticles for simultaneously enhanced upconversion fluorescence and darkfield imaging,” J. Mater. Chem. 22, 960–965 (2012). [CrossRef]
  26. J. Shen, G. Chen, T. Y. Ohulchanskyy, S. J. Kesseli, S. Buchholz, Z. Li, P. N. Prasad, and G. Han, “Tunable near infrared to ultraviolet upconversion luminescence enhancement in (α-NaYbF4:Tm3+)/CaF2 core/shell nanoparticles for in situ real-time recorded biocompatible photoactivation,” Small 9, 3213–3217 (2013). [PubMed]
  27. G. Chen, T. Y. Ohulchanskyy, R. Kumar, H. Ågren, and P. N. Prasad, “Ultrasmall monodisperse NaYF4:Yb3+/Tm3+ nanocrystals with enhanced near-infrared to near-infrared upconversion photoluminescence,” ACS Nano 4, 3163–3168 (2010). [CrossRef] [PubMed]
  28. H. Liu, C. T. Xu, G. Dumlupinar, O. B. Jensen, P. E. Andersen, and S. Andersson-Engels, “Deep tissue optical imaging of upconverting nanoparticles enabled by exploiting higher intrinsic quantum yield through using millisecond single pulse excitation with high peak power,” Nanoscale 5, 10034–10040 (2013). [CrossRef] [PubMed]
  29. C. T. Xu, Q. Zhan, H. Liu, G. Somesfalean, J. Qian, S. He, and S. Andersson-Engels, “Upconverting nanoparticles for pre-clinical diffuse optical imaging, microscopy and sensing: Current trends and future challenges,” Laser Photonics Rev. 7, 663–697 (2013). [CrossRef]

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