Phase angle encoded upconversion luminescent nanocrystals for multiplexing applications

Lanthanide-doped upconversion nanoparticles (UCNPs) are increasingly used as luminescent candidates in multiplexed applications due to their excellent optical properties. Inthepast,several encodingidentities havebeen proposedforUCNPs,includingemissioncolour,intensity ratio between different emissionbands, colourspatial distribution, and luminescencelifetime.In this paper, a new optical encoding dimension for upconversion nanomaterials is developed by exploring their luminescence kinetics, i.e., the phase angle of upconversion luminescence in response to a harmonic-wave excitation. Our theoretical derivation shows that the phase angle is governed jointly by the rise and decay times, characterizing the upconversion luminescence kinetics. Experimentally, a full set of methods are developed to manage the upconversion luminescence kinetics, through which the rise and decay times can be manipulated dependently or independently. Furthermore,a large phase-angle space is achieved in which tens of unique codes can be potentially generated in the same colour channel. Our work greatly extends the multiplexing capacity of UCNPs,and offers newopportunities for their applicationsin a wide range such as microarray assays, bioimaging, anti-counterfeiting, deep tissue multiplexed labelling/detectionand high-density data storage.In addition, the development of thisluminescence kinetics-based optical encoding strategy is also instructive for developing multiplexing techniques using other cascade luminescent systems that inherently lack multi-spectral channels, such as triplet-triplet annihilation molecule pairs.QC 20170330