Near-Infrared Excited Orthogonal Emissive Upconversion Nanoparticles for Imaging-Guided On-Demand Therapy

Photodynamic therapy (PDT) has been considered as a promising and noninvasive strategy for clinical cancer treatment. Nonetheless, building a smart "off-on" theranostic PDT platform to spatiotemporally control the generation of reactive oxygen species in the PDT treatment still remains challenging. Here, we have rationally developed photoswitching upconversion nanoparticles (UCNPs) with orthogonal emissive properties in response to two distinct near-infrared (NIR) emissions at 808 and 980 nm, i.e., red emission with 980 nm excitation and green emission with 808 nm excitation. Unlike traditional photoswitching UCNPs, these specially designed core-shell-shell structured UCNPs do not require complicated multilayer doping as their red and green upconversion luminescence both originate from the same activator Er³⁺ ions in the core structure. As a proof of concept, we have demonstrated the capability of these orthogonal emissive UCNPs for imaging-guided PDT in a real-time manner, where the red emission excited by 980 nm light is used to trigger PDT and the green emission with 808 nm excitation is to diagnose and monitor the therapeutic treatment. Our study suggests that such specially designed UCNPs with orthogonal emissions hold great promise for NIR light-targeted and imaging-guided therapy under precisely spatiotemporal control.