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Correction for 'NIR laser scanning microscopy for photophysical characterization of upconversion nanoparticles and nanohybrids' by Juan Ferrera-González et al., Nanoscale, 2021, 13, 10067-10080, DOI: .
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Photophysical characterization of upconversion nanoparticles (UCNPs) and nanohybrids (UCNHs) is more challenging than that of down-conversion nanomaterials. Moreover, it is still difficult to gain knowledge about the homogeneity of the sample and colocalization of emissive chromophores and nanoparticles in nanohybrids. Near infrared laser scanning microscopy (NIR-LSM) is a well-known and useful imaging technique, which enables excitation in the NIR region and has been extensively applied to optical fluorescence imaging of organic fluorophores and nanomaterials, such as quantum dots, which exhibit a short-lived emission. NIR-LSM has recently been used to determine the empirical emission lifetime of UCNPs, thus extending its application range to nanomaterials with a long lifetime emission. Here, we review our previous findings and include new measurements and samples to fully address the potential of this technique. NIR-LSM has proved to be extraordinarily useful not only for photophysical characterization of UCNHs consisting of UCNPs capped with a fluorophore to easily visualize the occurrence of the resonance energy transfer process between the UCNH constituents and their homogeneity, but also to assess the colocalization of the fluorophore and the UCNP in the UCNH; all this information can be acquired on the micro-/nano-meter scale by just taking one image.
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The stability of organic cappings on hexagonal NaYF4:Ln3+ upconversion nanoparticles (UCNPs) is crucial for their luminescence efficiency in aqueous solutions. The capping removal quickens as the acidity of the medium increases. We demonstrate here that polysulfonates, namely poly(2-acrylamido-2-methyl-1-propanesulfonate) (PAMPS) and poly(sodium 4-styrene sulfonate) (PSS), remain anchored to the surface of NaYF4:Yb3+,Er3+/Tm3 UCNPs even at a pH as low as 2 due to strong acidity of the sulfonate anchoring groups (pK a of ca. -3). Bare UCNPs progressively disintegrate into their compositional F-, Na+, Y3+, and Ln3+ ions. Their disintegration is particularly worrying in highly diluted dispersions of nanoparticles because both the lanthanide ions and/or the bare UCNPs can cause undesirable interference in a chemical or biological environment. Remarkably, the UC@PSS nanohybrid is particularly chemically stable, exhibiting an amazingly low release of Y3+ and Ln3+ ions for up to 96 h in highly diluted water dispersions (10 µg/mL). Additional advantages of the use of PSS as capping layer are its biocompatibility and its high dispersibility in water, together with easy further functionalization of the UCNP@PSS nanohybrids.
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Up to now, most strategies to build efficient 800 nm-light responsive upconversion nanoparticles (UCNPs) have included onion-layered structures, in which Nd3+ is confined within the inorganic crystal structure of at least one layer. We report here an easy room-temperature modular preparation of core-shell UCNPs consisting of NaYF4:Yb,Er(Tm)/NaYF4 (UCCS) with Nd3+ anchored at the organic capping by using cucurbituril[7] (CB[7]) as an adhesive. Strikingly, excitation at 800 nm effectively triggers the upconversion emission of UCCS@CB[7]@Nd nanohybrids.
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Water-dispersible upconversion nanoparticles (ß-NaYF4:Yb(3+),Er(3+), UCNP) coated with a thin shell of a biocompatible copolymer comprising 2-hydroxyethylmethacrylate (HEMA) and 2-acrylamido-2-methyl-1-propanesulphonsulphonic acid (AMPS), which we will term COP, have been prepared by multidentate grafting. This capping is remarkably resistant to strong acidic conditions as low as pH 2. The additional functionality of the smart UCNP@COP nanosystem has been proved by its association to a well-known photosensitizer (namely, methylene blue, MB). The green-to-red emission ratio of the UC@COP@MB nanohybrid exhibits excellent linear dependence in the 7 to 2 pH range as a consequence of the release of the dye as the pH decreases.