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@ARTICLE{Reichholf:639100,
      author       = {Reichholf, Nico and Horta, Sharona and Van der Heggen,
                      David and Seno, Carlotta and Pulparayil Mathew, Jikson and
                      Ibáñez, Maria and Smet, Philippe F. and De Roo, Jonathan},
      title        = {{I}dentification and {E}limination of {S}urface {E}mission
                      in {L}anthanide ({C}o)doped {Z}irconia {N}anocrystals},
      journal      = {ACS nano},
      volume       = {19},
      number       = {33},
      issn         = {1936-0851},
      address      = {Washington, DC},
      publisher    = {Soc.},
      reportid     = {PUBDB-2025-04303},
      pages        = {30371 - 30382},
      year         = {2025},
      abstract     = {Zirconia nanocrystals (ZrO2 NCs) are a stable host material
                      for lanthanides, but their performance lags behind that of
                      the leading NaYF4 nanomaterials. Here, we leverage surface
                      chemistry and core/shell architectures to uncover the
                      contribution of dopants at the nanocrystal surface and of
                      dopants in the nanocrystal bulk. We first assess the doping
                      efficiency by ICP and find that, while Eu is almost
                      quantitatively incorporated, the other lanthanides (La, Ce,
                      Tb, Tm, Er, Yb) have about $50\%$ incorporation efficiency
                      over the studied doping range of $1–10\%.$ We then
                      determine the nanocrystal surface chemistry using NMR
                      spectroscopy, despite the additional spectral line
                      broadening caused by the paramagnetic lanthanide dopants. By
                      varying the surface ligands and measuring the
                      photoluminescence, we resolve the spectroscopic signals that
                      are sensitive to a change in surface chemistry.
                      Time-resolved emission spectra further reinforce the notion
                      of a bulk component with a long luminescent lifetime and a
                      surface component with a fast lifetime. Upon shelling Eu- or
                      Tb-doped zirconia NCs with pure zirconia, the surface
                      component disappears, and the photoluminescence quantum
                      yield increases. We further functionalized the surface of
                      the core/shell particles with oleylphosphonic acid ligands
                      to obtain excellent dispersibility. These results show that
                      lanthanide-doped zirconia NCs can be engineered to eliminate
                      deactivation pathways.},
      cin          = {FS DOOR-User},
      ddc          = {540},
      cid          = {$I:(DE-H253)FS_DOOR-User-20241023$},
      pnm          = {6G3 - PETRA III (DESY) (POF4-6G3) / FS-Proposal: I-20231114
                      EC (I-20231114-EC)},
      pid          = {G:(DE-HGF)POF4-6G3 / G:(DE-H253)I-20231114-EC},
      experiment   = {EXP:(DE-H253)P-P21.1-20150101},
      typ          = {PUB:(DE-HGF)16},
      doi          = {10.1021/acsnano.5c09137},
      url          = {https://bib-pubdb1.desy.de/record/639100},
}