Dramatic Enhancement of Quantum Cutting in Lanthanide-Doped Nanocrystals Photosensitized with an Aggregation-Induced Enhanced Emission Dye

Applications of multiphoton processes in lanthanide-doped nanophosphors (NPs) are often limited by relatively weak and narrow absorbance. Here, the concept of an ultimate photosensitization by aggregation-induced enhanced emission (AIEE) dyes to overcome this limitation is introduced. Because AIEE dyes do not suffer from concentration quenching, they can fully cover the NP surface at high density to maximize absorbance while passivating the surface. This concept is applied to multiphoton down-conversion by quantum cutting. Specifically, coating Yb³⁺/Tb³⁺-doped NPs with an AIEE dye designed for efficient energy transfer and attachment to the NPs produces a 2260-fold enhancement of multiphoton down-conversion by quantum cutting with remarkable photostability. In a prototypical application, the quantum cutting of UV photons to near-infrared photons that are matched to the band gap of a silicon solar cell produces an average 4% increase in efficiency under concentrated solar illumination. This provides a general strategy for NP photosensitization that can be applied to both multiphoton up- and down-conversion.