resumo
We propose two effective approaches to enhance the Forster resonance energy transfer (FRET) efficiency from near-infrared excited upconverting nanoparticles (UCNPs, namely, LiYF4:Yb3+,Tm3+) 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 among the moieties under investigation when in solution. However, analyses performed on dry powders allowed observing 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 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 a 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.
palavras-chave
UP-CONVERSION NANOPARTICLES; CORE-SHELL NANOPARTICLES; TRANSFER FRET; ORGANIC-DYES; NANOCRYSTALS; EMISSION; PLATFORM; ASSAY; PHOTOLUMINESCENCE; NANOPHOSPHOR
categoria
Science & Technology - Other Topics; Materials Science; Optics; Physics
autores
Marin, R; Labrador-Paez, L; Skripka, A; Haro-Gonzalez, P; Benayas, A; Canton, P; Jaque, D; Vetrone, F
nossos autores
Grupos
agradecimentos
This work was supported by the Spanish Ministerio de Educacion y Ciencia (MAT2016-75362-C3-1-R) and by COST Action CM1403. L.L.-P. thanks the Universidad Autonoma de Madrid for the "Formacion de Personal Investigador (FPI-UAM)" program. P.H.-G. thanks the Spanish Ministerio de Economia y Competitividad for the Juan de la Cierva program (IJCI-2015-24551). A.B. thanks the Canadian Institutes of Health Research Breast Cancer Society of Canada (CIHR-BCSC), for the support given to him through the Eileen Iwanicki Postdoctoral Fellowship on Breast Cancer Imaging. A.B. also thanks the European Commission, as his participation in this project at its later stage has received funding from the European Union's Horizon 2020 research and innovation program under the Marie Sklodowska Curie grant agreement no. 709270 "TEMPTATION". F.V. is grateful to the Natural Sciences and Engineering Research Council (NSERC) of Canada for supporting his research.