Structure-Property Relationships in Lanthanide-Doped Upconverting Nanocrystals: Recent Advances in Understanding Core-Shell Structures.

The production of upconverting nanostructures with tailored optical properties is of major technological interest, and rapid progress toward the realization of such production has been made in recent years. Ultimately, accurate understanding of nanostructure organization will lead to design rules for accurately tailoring optical properties. Here, the context of open questions still of general importance to the upconversion and nanocrystal communities is presented, with a particular emphasis on the structure-property relationships of core-shell upconverting nanocrystals. Although the optical properties of the latter have been thoroughly investigated, little is known regarding their atomic-scale organization. Indeed, solving the atomic-scale structure of such nanomaterials is challenging because of their intrinsic nonperiodic nature. Familiar concepts of crystallography are no longer appropriate; chemical and structural modulation waves must be introduced. To reveal the exact core-shell structures, innovative characterization techniques need to be applied and developed, as discussed herein. The continued development and application of structural characterization techniques will be vital to consolidate the currently incomplete link between atomic-scale structure and upconversion properties. This will ultimately provide a valuable contribution to the emerging detailed guidelines on how to better design upconverting nanostructures to achieve given optical properties in terms of efficiency, absorption, spectral emission, and dynamics.