Liang, L.; Qin, X.; Zheng, K.; Liu, X. Acc. Chem. Res. 2019, 52 (1), 228–236. Lanthanide-doped upconversion nanoparticles (UCNPs) exhibit unique optical characteristics, including a large anti-Stokes shift, a long luminescence lifetime, sharp emission bands, and high photostability. These virtues make UCNPs highly useful in many emerging applications such as biolabeling, security, multicolor displays, and optogenetics. Despite the enticing prospects of UCNPs, their practical utility is greatly hindered by the low efficiency of the conversion from near-infrared (NIR) excitation to visible emission. In a typical nanosystem codoped with sensitizers and activators, upconversion processes occur through NIR light sensitization, energy transfer from sensitizers to activators, sequential energy population at the excited states of the activators, and eventually the release of higher-energy photons. In fact, in the upconversion nanosystem, each step in the energy flux, including NIR energy injection, energy transfer and migration, and energy dissipation, has a decisive effect on the resulting luminescence intensity. Important in-depth studies have been conducted in pursuit of brighter UCNPs. Specifically, lanthanide ions possessing larger absorption cross sections (Nd3+) or organic dye molecules have been chosen as NIR light sensitizers to improve the light harvesting ability of upconversion nanostructures. The doping concentration and spatial distribution of lanthanide ions are strictly managed to mitigate detrimental energy cross-talk processes. The surfaces of UCNPs are passivated with epitaxially grown layers to block surface quenching. Therefore, rational design of energy flux manipulation, through control of excitation energy collection, transmission, and release in a three-dimensional nanospace of UCNPs, is crucial in constructing nanosystems with high upconversion efficiencies. ... |
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