Suppression of Cation Intermixing Highly Boosts the Performance of Core–Shell Lanthanide Upconversion Nanoparticles

[Image: see text] Lanthanide upconversion nanoparticles (UCNPs) have been extensively explored as biomarkers, energy transducers, and information carriers in wide-ranging applications in areas from healthcare and energy to information technology. In promoting the brightness and enriching the functionalities of UCNPs, core–shell structural engineering has been well-established as an important approach. Despite its importance, a strong limiting issue has been identified, namely, cation intermixing in the interfacial region of the synthesized core–shell nanoparticles. Currently, there still exists confusion regarding this destructive phenomenon and there is a lack of facile means to reach a delicate control of it. By means of a new set of experiments, we identify and provide in this work a comprehensive picture for the major physical mechanism of cation intermixing occurring in synthesis of core–shell UCNPs, i.e., partial or substantial core nanoparticle dissolution followed by epitaxial growth of the outer layer and ripening of the entire particle. Based on this picture, we provide an easy but effective approach to tackle this issue that enables us to produce UCNPs with highly boosted optical properties.