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Molecular size matters : ultrafast dye singlet sensitization pathways to bright nanoparticle emission

Jing Liu, Pieter Geiregat (UGent) , Luca Pilia, Rik Van Deun (UGent) and Flavia Artizzu (UGent)
(2021) ADVANCED OPTICAL MATERIALS. 9(7).
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Abstract
Dye-sensitized luminescent lanthanide (Ln)-based nanoparticles enable broad applications spanning from fluorescent microscopy to biological therapy. However, the limited understanding of the dye -> Ln(3+) sensitization process still leaves ample room for the improvement of its efficiency. In this work, a unique combination of photoluminescence and transient absorption spectroscopy is employed to reveal the hereto hidden dye -> Ln(3+) or dye -> Ln(1)(3+)-> Ln(2)(3+) energy transfer pathways in the ultrafast time scale. Steady-state and time-resolved data, supported by density functional theory calculations, demonstrate that Ln(3+) sensitization is realized directly from the singlet excited state of dye molecules and is strictly regulated by a distance-dependent regime overcoming the role of the donor-acceptor spectral overlap for the size and geometry of dye molecules. It is shown that exceptionally high efficiency is achieved by judiciously selecting small-sized dye molecules with localized molecular orbitals sitting close (<0.5 nm) to the nanoparticle surface. This new understanding will enable a rational design of dye-sensitized Ln nanoparticles allowing for a dramatic improvement of the emission efficiency in a variety of nanomaterials for light conversion.
Keywords
dye-sensitized nanoparticles, energy transfer, lanthanide emission, photosensitization, transient absorption spectroscopy

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MLA
Liu, Jing, et al. “Molecular Size Matters : Ultrafast Dye Singlet Sensitization Pathways to Bright Nanoparticle Emission.” ADVANCED OPTICAL MATERIALS, vol. 9, no. 7, 2021, doi:10.1002/adom.202001678.
APA
Liu, J., Geiregat, P., Pilia, L., Van Deun, R., & Artizzu, F. (2021). Molecular size matters : ultrafast dye singlet sensitization pathways to bright nanoparticle emission. ADVANCED OPTICAL MATERIALS, 9(7). https://doi.org/10.1002/adom.202001678
Chicago author-date
Liu, Jing, Pieter Geiregat, Luca Pilia, Rik Van Deun, and Flavia Artizzu. 2021. “Molecular Size Matters : Ultrafast Dye Singlet Sensitization Pathways to Bright Nanoparticle Emission.” ADVANCED OPTICAL MATERIALS 9 (7). https://doi.org/10.1002/adom.202001678.
Chicago author-date (all authors)
Liu, Jing, Pieter Geiregat, Luca Pilia, Rik Van Deun, and Flavia Artizzu. 2021. “Molecular Size Matters : Ultrafast Dye Singlet Sensitization Pathways to Bright Nanoparticle Emission.” ADVANCED OPTICAL MATERIALS 9 (7). doi:10.1002/adom.202001678.
Vancouver
1.
Liu J, Geiregat P, Pilia L, Van Deun R, Artizzu F. Molecular size matters : ultrafast dye singlet sensitization pathways to bright nanoparticle emission. ADVANCED OPTICAL MATERIALS. 2021;9(7).
IEEE
[1]
J. Liu, P. Geiregat, L. Pilia, R. Van Deun, and F. Artizzu, “Molecular size matters : ultrafast dye singlet sensitization pathways to bright nanoparticle emission,” ADVANCED OPTICAL MATERIALS, vol. 9, no. 7, 2021.
@article{8689452,
  abstract     = {{Dye-sensitized luminescent lanthanide (Ln)-based nanoparticles enable broad applications spanning from fluorescent microscopy to biological therapy. However, the limited understanding of the dye -> Ln(3+) sensitization process still leaves ample room for the improvement of its efficiency. In this work, a unique combination of photoluminescence and transient absorption spectroscopy is employed to reveal the hereto hidden dye -> Ln(3+) or dye -> Ln(1)(3+)-> Ln(2)(3+) energy transfer pathways in the ultrafast time scale. Steady-state and time-resolved data, supported by density functional theory calculations, demonstrate that Ln(3+) sensitization is realized directly from the singlet excited state of dye molecules and is strictly regulated by a distance-dependent regime overcoming the role of the donor-acceptor spectral overlap for the size and geometry of dye molecules. It is shown that exceptionally high efficiency is achieved by judiciously selecting small-sized dye molecules with localized molecular orbitals sitting close (<0.5 nm) to the nanoparticle surface. This new understanding will enable a rational design of dye-sensitized Ln nanoparticles allowing for a dramatic improvement of the emission efficiency in a variety of nanomaterials for light conversion.}},
  articleno    = {{2001678}},
  author       = {{Liu, Jing and Geiregat, Pieter and Pilia, Luca and Van Deun, Rik and Artizzu, Flavia}},
  issn         = {{2195-1071}},
  journal      = {{ADVANCED OPTICAL MATERIALS}},
  keywords     = {{dye-sensitized nanoparticles,energy transfer,lanthanide emission,photosensitization,transient absorption spectroscopy}},
  language     = {{eng}},
  number       = {{7}},
  pages        = {{8}},
  title        = {{Molecular size matters : ultrafast dye singlet sensitization pathways to bright nanoparticle emission}},
  url          = {{http://dx.doi.org/10.1002/adom.202001678}},
  volume       = {{9}},
  year         = {{2021}},
}
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