Upconversion Perovskite Nanocrystal Heterostructures with Enhanced Luminescence and Stability by Lattice Matching

Lead halide perovskite quantum dots (PQDs) exhibit excellent photoelectric and optical properties, but their poor stability and low multiphoton absorption efficiency greatly limit their biological applications. Efforts have been made to combine upconversion nanoparticles (UCNPs) with PQDs to produce a composite material that is NIR-excitable, upconverting, and emission-tunable due to the unique optical properties of UCNPs, which converts tissue-penetrating near-infrared light into visible light based on an upconversion multiphoton excitation process. However, it is challenging to make such a nanocrystal heterostructure and maintain good optical properties and stability of both UCNPs and PQDs because they have different crystal structures. Here, we report the synthesis of heterostructured UCNP–PQD nanocrystals to bring hexagonal-phase NaYF₄ UCNPs and cubic-phase CsPbBr₁X₂ PQDs in close proximity in a single nanocrystal, leading to efficient Förster resonance energy transfer (FRET) from the UCNP to the PQD under NIR excitation, as compared to their counterparts in solution. Moreover, by further improving the lattice matching between the UCNP and PQD using Gd to replace Y, heterostructured CsPbBr₃-NaGdF₄:Yb,Tm nanocrystals are successfully synthesized, with much enhanced luminescence and stability at high temperatures or in polar solvents or under continuous ultraviolet light excitation as compared to those of the CsPbBr₃-NaYF₄:Yb,Tm nanocrystals and pure PQDs.