Rare-earth-doped luminescent nanothermometers are not reliable as their emission spectra can be affected by numerous environmental and experimental factors.
We propose two effective approaches to enhance the Förster resonance energy transfer (FRET) efficiency from nearinfrared (NIR) excited upconverting nanoparticles (UCNPs, namely LiYF4:Yb 3+ ,Tm 3+ ) to CuInS2 quantum dots (QDs) upon engineering of the donor's architecture. The study of the particles' interaction highlighted a radiative nature of the energy transfer (ET) among the moieties under investigation when in solution. However, analyses performed on dry powders allowed to observe clear evidence of a FRET mechanism. In particular, photoluminescence lifetime measurements showed that FRET efficiency could be effectively increased by, both, reducing the size of the UCNPs and directly controlling the distribution of the active ions throughout the donor's volume, i.e. doping them only in the outer shell of a core/shell system. Both strategies resulted at least in a more than doubled FRET efficiency compared to larger core-only UCNPs. Obtained experimental values were compatible with those predicted from geometrical considerations on the active ions' distribution over the UCNP volume. These results provide a concrete proof of the potential of UCNP-QD FRET pair when the system is properly designed, hence setting a solid base for the development of robust and efficient all-inorganic probes for FRET-based assays.
An approach to unequivocally determine the three-dimensional orientation of optically manipulated studies. Based on the strong polarization dependent upconverted luminescence of UCNRs it is possible to unequivocally determine, in real time, their three-dimensional orientation when optically trapped. In single-beam traps, polarized single particle spectroscopy has concluded that UCNRs orientate parallel to the propagation axis of the trapping beam. On the other hand, when multiple-beam optical tweezers are used, single particle polarization spectroscopy demonstrated how full spatial control over UCNR orientation can be achieved by changing the trap-to-trap distance as well as the relative orientation between optical traps. All these results show the possibility of real time three-dimensional manipulation and tracking of anisotropic nanoparticles with wide potential application in modern nanobiophotonics.
Lanthanide-doped upconverting nanoparticles (UCNPs) have been studied for diverse biomedical applications due to their inherent ability to convert near-infrared (NIR) excitation light to higher energies (spanning the ultraviolet, visible, and NIR regions). To explore additional functionalities, rational combination with other optically active nanostructures may lead to the development of new multimodal nanoplatforms with theranostic (therapy and diagnostic) capabilities. Here, we develop a nanocomposite consisting of NaGdF:Er, Yb UCNPs, mesoporous silica (SiO), gold nanorods (GNRs) and a photosensitizer, with integrated functionalities including luminescence imaging, photothermal generation, nanothermometry and photodynamic effects. Under 980 nm irradiation, GNRs and UCNPs are simultaneously excited due to the overlap between the surface plasmon resonance of the GNRs and the absorption of the UCNPs leading to plasmonic enhancement of the upconverted luminescence, while concomitantly creating a temperature gradient. The temperature increase can be determined from the intensity ratio of the upconverted green emission of the UCNPs. Finally, a photosensitizer, zinc phthalocyanine, was loaded into the mesoporous SiO. Upon laser irradiation, the upconverted visible light subsequently activates the photosensitizer to release reactive oxygen species. The multifunctional GNR@SiO@UCNPs nanocomposites showed strong luminescence signal when incubated in HeLa cervical cancer cells, making them ideal bioprobes for future theranostic applications.
The current status of the use of core-shell rare-earth-doped nanoparticles in biomedical applications is reviewed in detail. The different core-shell rare-earth-doped nanoparticles developed so far are described and the most relevant examples of their application in imaging, sensing, and therapy are summarized. In addition, the advantages and disadvantages they present are discussed. Finally, a critical opinion of their potential application in real life biomedicine is given.
Optical trapping has been evidence as a very powerful tool for the manipulation and study of biological entities. This review explains the main concepts regarding the use of optical trapping for biosensing, focusing its attention to those applications involving the manipulation of particles which are used as handles, force transducers and sensors.
Nowadays a large variety of applications are based on solid nanoparticles dispersed in liquids-so called nanofluids. The interaction between the fluid and the nanoparticles plays a decisive role in the physical properties of the nanofluid. A novel approach based on the nonradiative energy transfer between two small luminescent nanocrystals (GdVO :Nd and GdVO :Yb ) dispersed in water is used in this work to investigate how temperature affects both the processes of interaction between nanoparticles and the effect of the fluid on the nanoparticles. From a systematic analysis of the effect of temperature on the GdVO :Nd → GdVO :Yb interparticle energy transfer, it can be concluded that a dramatic increase in the energy transfer efficiency occurs for temperatures above 45 °C. This change is properly explained by taking into account a crossover existing in diverse water properties that occurs at about this temperature. The obtained results allow elucidation on the molecular arrangement of water molecules below and above this crossover temperature. In addition, it is observed that an energy transfer process is produced as a result of interparticle collisions that induce irreversible ion exchange between the interacting nanoparticles.
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