Epitaxial
growth of an inert shell around the optical active lanthanide
upconversion nanoparticles (UCNPs) is a general strategy to enhance
their brightness. Yet, its potential as a tool in multiplexing emission
tailoring has rarely been reported. Here, by developing the atomic
vacancies into color selectivity actuators, we present an efficient
strategy to achieve inert-shell-modulated multiplexing upconversion
in 1540 nm activated UCNPs. Artificially generated fluoride atomic
vacancies, owing to the decreased NaOH/NH4F dosage during
shell growth, reduce the coordination number of Y–F and lattice
densities in the inert shell, leading to the core–engineered
shell nanoparticles with distinctive emission profiles. The multicolor
tailoring is independent of shell thickness and can be readily applied
to Lu3+/Gd3+-based shells. The upconversion
emission can be exploited to visualize in security decoding and in vivo multiplexing bioimaging. This method of regulating
atomic vacancies based on the inert-shell engineering opens new insights
of upconversion modulation in core–shell lanthanide nanostructures.
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