Excitation energy mediated cross-relaxation for tunable upconversion luminescence from a single lanthanide ion

Precise control of energy migration between sensitizer ions and activator ions in lanthanide-doped upconversion nanoparticles (UCNPs) nowadays has been extensively investigated to achieve efficient photon upconversion. However, these UCNPs generally emit blue, green or red light only under fixed excitation conditions. In this work, regulation of the photon transition process between different energy levels of a single activator ion to obtain tunable upconversion fluorescence under different excitation conditions is achieved by introducing a modulator ion. The cross-relaxation process between modulator ion and activator ion can be controlled to generate tunable luminescence from the same lanthanide activator ion under excitation at different wavelengths or with different laser power density and pulse frequency. This strategy has been tested and proven effective in two different nanocrystal systems and its usefulness has been demonstrated for high-level optical encryption. Here, the authors report tunable luminescence from a single lanthanide ion upon changing excitation conditions through co-doping an energy-modulator ion, thus adjusting the photon transition process of the lanthanide activator ion. Optical encryption has also been demonstrated as an application of this universal strategy.