4.6 Article

Molecular Size Matters: Ultrafast Dye Singlet Sensitization Pathways to Bright Nanoparticle Emission

期刊

ADVANCED OPTICAL MATERIALS
卷 9, 期 7, 页码 -

出版社

WILEY-V C H VERLAG GMBH
DOI: 10.1002/adom.202001678

关键词

dye-sensitized nanoparticles; energy transfer; lanthanide emission; photosensitization; transient absorption spectroscopy

资金

  1. National Natural Science Foundation of China (NSFC) [52002336]
  2. Fundamental Research Funds for the Central Universities [SWU019041]
  3. Science and Technology project of Chongqing Education Committee [KJCX2020005]
  4. Chongqing Engineering Research Center for Rapid Diagnosis of Dread Disease, Southwest University, China
  5. Chongqing Engineering Research Center for Micro-Nano Biomedical Materials and Devices, Southwest University, China
  6. FWO (Research Foundation Flanders)
  7. European Union's Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant [665501, 12U3417N LV]

向作者/读者索取更多资源

This study investigates the energy transfer pathways from dyes to lanthanide nanoparticles using a combination of photoluminescence and transient absorption spectroscopy. By selecting small-sized dye molecules with localized molecular orbitals close to the nanoparticle surface, exceptionally high efficiency in lanthanide nanoparticles sensitization can be achieved.
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.

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