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Understanding the Role of Yb3+ in the Nd/Yb Coupled 808-nm-Responsive Upconversion.

ABSTRACT: The realization of upconversion at 808 nm excitation has shown great advantages in advancing the broad bioapplications of lanthanide-doped nanomaterials. In an 808 nm responsive system, Nd3+ and Yb3+ are both needed where Nd3+ acts as a sensitizer through absorbing the excitation irradiation. However, few studies have been dedicated to the role of Yb3+. Here, we report a systemic investigation on the role of Yb3+ by designing a set of core-shell-based nanostructures. We find that energy migration over the ytterbium sublattice plays a key role in facilitating the energy transportation, and moreover, we show that the interfacial energy transfer occurring at the core-shell interface also has a contribution to the upconversion. By optimizing the dopant concentration and surface anchoring the infrared indocyanine green dye, the 808 nm responsive upconversion is markedly enhanced. These results present an in-depth understanding of the fundamental interactions among lanthanides, and more importantly, they offer new possibilities to tune and control the upconversion of lanthanide-based luminescent materials.

SUBMITTER: Song N

PROVIDER: S-EPMC6355672 | biostudies-literature | 2018

REPOSITORIES: biostudies-literature

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Understanding the Role of Yb3+ in the Nd/Yb Coupled 808-nm-Responsive Upconversion.

Song Nan N Zhou Bo B Yan Long L Huang Jinshu J Zhang Qinyuan Q

Frontiers in chemistry 20190125

The realization of upconversion at 808 nm excitation has shown great advantages in advancing the broad bioapplications of lanthanide-doped nanomaterials. In an 808 nm responsive system, Nd3+ and Yb3+ are both needed where Nd3+ acts as a sensitizer through absorbing the excitation irradiation. However, few studies have been dedicated to the role of Yb3+. Here, we report a systemic investigation on the role of Yb3+ by designing a set of core-s ...[more]

PMID: 30740392

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Project description:Lanthanide-doped upconversion nanoparticles (UCNPs) have a unique capability of upconverting near-infrared (NIR) excitation into ultraviolet, visible, and NIR emission. Conventional UCNPs composed of NaYF4:Yb3+/Er3+(Tm3+) are excited by NIR light at 980 nm, where undesirable absorption by water can cause overheating or damage of living tissues and reduce nanoparticle luminescence. Incorporation of Nd3+ ions into the UCNP lattice shifts the excitation wavelength to 808 nm, where absorption of water is minimal. Herein, core-shell NaYF4:Yb3+/Er3+@NaYF4:Nd3+ nanoparticles, which are doubly doped by sensitizers (Yb3+ and Nd3+) and an activator (Er3+) in the host NaYF4 matrix, were synthesized by high-temperature coprecipitation of lanthanide chlorides in the presence of oleic acid as a stabilizer. Uniform core (24 nm) and core-shell particles with tunable shell thickness (~0.5-4 nm) were thoroughly characterized by transmission electron microscopy (TEM), energy-dispersive analysis, selected area electron diffraction, and photoluminescence emission spectra at 808 and 980 nm excitation. To ensure dispersibility of the particles in biologically relevant media, they were coated by in-house synthesized poly(ethylene glycol) (PEG)-neridronate terminated with an alkyne (Alk). The stability of the NaYF4:Yb3+/Er3+@NaYF4:Nd3+-PEG-Alk nanoparticles in water or 0.01 M PBS and the presence of PEG on the surface were determined by dynamic light scattering, ζ-potential measurements, thermogravimetric analysis, and FTIR spectroscopy. Finally, the adhesive azidopentanoyl-modified GGGRGDSGGGY-NH2 (RGDS) peptide was immobilized on the NaYF4:Yb3+/Er3+@NaYF4:Nd3+-PEG-Alk particles via Cu(I)-catalyzed azide-alkyne cycloaddition. The toxicity of the unmodified core-shell NaYF4:Yb3+/Er3+@NaYF4:Nd3+, NaYF4:Yb3+/Er3+@NaYF4:Nd3+-PEG-Alk, and NaYF4:Yb3+/Er3+@NaYF4:Nd3+-PEG-RGDS nanoparticles on both Hep-G2 and HeLa cells was determined, confirming no adverse effect on their survival and proliferation. The interaction of the nanoparticles with Hep-G2 cells was monitored by confocal microscopy at both 808 and 980 nm excitation. The NaYF4:Yb3+/Er3+@NaYF4:Nd3+-PEG-RGDS nanoparticles were localized on the cell membranes due to specific binding of the RGDS peptide to integrins, in contrast to the NaYF4:Yb3+/Er3+@NaYF4:Nd3+-PEG-Alk particles, which were not engulfed by the cells. The NaYF4:Yb3+/Er3+@NaYF4:Nd3+-PEG-RGDS nanoparticles thus appear to be promising as a new non-invasive probe for specific bioimaging of cells and tissues. This development makes the nanoparticles useful for diagnostic and/or, after immobilization of a bioactive compound, even theranostic applications in the treatment of various fatal diseases.

Dataset Information

Understanding the Role of Yb3+ in the Nd/Yb Coupled 808-nm-Responsive Upconversion.

Publications

Understanding the Role of Yb<sup>3+</sup> in the Nd/Yb Coupled 808-nm-Responsive Upconversion.

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