Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.021
Publication date: 16th December 2024
While fluoride nanocrystals (e.g., NaYF4) are popular host materials for lanthanide-based up-and downconversion, ceramic oxide hosts (e.g., ZrO2 and HfO2) have found less widespread use, due to the synthetic challenge of producing colloidally stable oxide nanocrystals with a complex (e.g., core/shell) architecture. The oxides are however, more chemically and thermally stable.
We first present the results of our mechanistic investigation in the synthesis of zirconium and hafnium oxide from metal chloride and metal alkoxide in trioctylphosphine oxide (TOPO). We study the metal speciation in solution, we determined the decomposition kinetics and its mechanism and we study the nucleation and growth. We find evidence for an E1 elimination mechanism and the occurrence of amorphous particles as intermediate on route the final highly crystalline particles. This is a consequence of the rate imbalance between a fast precursor decomposition and a slow crystallization process.
Second, we demonstrate the epitaxial growth of hafnia shells onto zir-conia cores, and pure zirconia shells onto europium doped zirconia cores. The core/shell structures are fully crystalline. Upon shelling, the optical properties of the europium dopant are dramatically improved (featuring a more uniform coordination and a longer photoluminescence lifetime), indicating the suppression of non-radiative pathways.
Third, we dive deeper in lanthanide doped zirconia nanocrystals. We determine the incorporation efficiency of multiple lanthanide in zirconia. We show the influence of the surface chemistry on the emission spectrum and lifetimes of Eu3+ of Tb3+. Time resolved emission spectra allow us to differentiate different europium sites (surface and bulk).
These results launch the stable zirconium and hafnium oxide hosts as alternatives for the established NaYF4 systems.
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