RESUMO
Fluorescent nanothermometers based on thermal-dependent lifetime have a significant advantage in biological imaging owing to their immunity toward scattering, absorption, and autofluorescence. In this study, we present the first example of a water-soluble europium complex ([L1Eu]-) that exhibits high sensitivity (1.2% K-1 at 298 K) based on a temperature-dependent lifetime in the millisecond time range. This complex and its analogues show considerable potential for organelle imaging. The mechanism behind this thermal-sensitive behavior has been extensively investigated using transient absorption spectroscopy and variable temperature time-resolved luminescence methods. A highly efficient ligand sensitization process and a thermally activated back energy transfer process have been demonstrated. This study bridges the gap in small molecule thermometers with lifetimes longer than 1 ms and provides guidance in ligand design for metal coordination complex thermometers.
RESUMO
Impurity doping has been widely applied in nanomaterial synthesis for modulating the crystallographic phase, morphology, and size of nanocrystalline materials, but mostly by altering thermodynamic equilibria of final products. Here, we report the use of lanthanide dopants to manipulate the growing kinetics of halide perovskite nanocrystals to enable the preparation of highly anisotropic two-dimensional (2D) CsPbBr3-based nanoplatelets with precisely controlled thickness. We demonstrate that the incorporation of trivalent lanthanides increases the energy barrier in growing three-monolayer (3 ML) CsPbBr3 from a 2 ML intermediate. It enables the growth of thermodynamically unfavorable 2 ML CsPbBr3 products through kinetic control. This finding provides a novel approach for dimensional control of perovskite nanocrystals with strong quantum confinement. It offers opportunities to generate deep-blue emitting (at 430 nm) CsPbBr3:Lu3+ nanoplatelets with good structural- and photo-stabilities potentially useful for many applications including light-emitting, lasers, and photocatalysis.