Core-Shell Interface Engineering Strategies for Modulating Energy Transfer in Rare Earth-Doped Nanoparticles.

Rare earth-doped nanoparticles (RENPs) are promising biomaterials with substantial potential in biomedical applications. Their multilayered core-shell structure design allows for more diverse uses, such as orthogonal excitation. However, the typical synthesis strategies-one-pot successive layer-by-layer (LBL) method and seed-assisted (SA) method-for creating multilayered RENPs show notable differences in spectral performance. To clarify this issue, a thorough comparative analysis of the elemental distribution and spectral characteristics of RENPs synthesized by these two strategies was conducted. The SA strategy, which avoids the partial mixing stage of shell and core precursors inherent in the LBL strategy, produces RENPs with a distinct interface in elemental distribution. This unique elemental distribution reduces unnecessary energy loss via energy transfer between heterogeneous elements in different shell layers. Consequently, the synthesis method choice can effectively modulate the spectral properties of RENPs. This discovery has been applied to the design of orthogonal RENP biomedical probes with appropriate dimensions, where the SA strategy introduces a refined inert interface to prevent unnecessary energy loss. Notably, this strategy has exhibited a 4.3-fold enhancement in NIR-II in vivo imaging and a 2.1-fold increase in reactive oxygen species (ROS)-related photodynamic therapy (PDT) orthogonal applications.