Bright upconversion over extended temperatures enabled by an organic surface layer

Abstract

Lanthanide-doped nanocrystals are promising for photon frequency upconversion with substantial spectrum tunability. However, the utilization of the upconversion process has been constrained by low luminescence efficiency, which may further attenuate at elevated temperatures due to thermal quenching. Herein, we report a versatile strategy to boost upconversion luminescence across a wide temperature range by surface coordination of small organic molecules. Mechanistic investigations affirm that the organic surface layer passivates defects and isolates high-energy surface oscillators, thereby preventing the dissipation of excitation energy. The energy preserving effect becomes more prominent with increasing temperatures, especially in a humid environment. Accordingly, the upconversion emission of NaGdF4:Yb3+/Tm3+ nanocrystals is substantially enhanced in the ambient environment after ligand coordination, accompanied by an additional emission augmentation with increasing temperature to 443 K. By leveraging this anomalous optical response to thermal stimuli, we further establish full-color thermochromic upconversion switching for advanced anti-counterfeiting and logic encryption technologies.