Monodispersed CsPb₂Br₅@SiO₂ Core-Shell Nanoparticles as Luminescent Labels for Biosensing

Despite the rising advances in the field of metal halide perovskite nanocrystals (NCs), the exploitation of such nanoparticles as luminescent labels for ex vivo imaging and biosensing is still unclear and in the early stages of investigation. One of the major challenges toward the implementation of metal halide perovskite NCs in biosensing applications is to produce monodispersed nanoparticles with desired surface characteristics and compatible with aqueous environments. Here, we report the synthesis of monodispersed spherical CsPb₂Br₅@SiO₂ core-shell nanoparticles by post-synthetic chemical transformation of 3D CsPbBr₃ NCs in the presence of tetraethyl orthosilicate and a critical water/ammonia ratio. This method involves an ammonia-mediated and ammonia-induced "top-down" transformation of as-synthesized 3D CsPbBr₃ NCs to smaller CsPb2Br5 nanoclusters (ca. 2-3 nm), which trigger a seed-mediated silica growth, yielding monodispersed spherical blue luminescent (λ_emission = 432 nm) CsPb₂Br₅@SiO₂ perovskite nanoparticles. By adjusting the reaction conditions, core-shell nanoparticles of a 36.1 ± 4.5 nm diameter, which preserve their optical properties in water, were obtained. Besides that, the viability of the developed nanoparticles as a luminescent label for biosensing has been proven by specific biorecognition of the IgG protein in a direct immunoassay. Our work sheds light on the chemical processes and transformations involved in the silica nucleation mechanism in the presence of perovskite nanoparticles and opens the way for the future rational design of the next generation of semiconductor NC luminescent biological labels.