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Trivalent europium (Eu 3+ ) doped inorganic nanoparticles (NPs), emerging as a new class of red luminescent nanoprobes, have shown great promise in bioapplications as diverse as luminescent bioassays and disease theranostics owing to their superior optical properties such as long-lived downshifting luminescence (DSL) and upconverting luminescence (UCL). However, the exploration of Eu 3+ -doped NPs as red luminescent bioprobes particularly combined with DSL and UCL of Eu 3+ hitherto remains untouched. Herein, we report a rational core-shell-shell (CSS) design strategy to construct Eu 3+ -activated NaGdF 4 :Yb/Tm@NaGdF 4 :Eu@NaEuF 4 CSS NPs functionalized with efficient UCL and dissolution-enhanced DSL of Eu 3+ for in vitro tumor marker detection and tumor-targeted imaging. By utilizing the CSS NPs as red luminescent nanoprobes, we demonstrate the successful UCL and DSL bioassays of a typical hepatic carcinoma biomarker, alpha-fetoprotein (AFP), in human serum samples. The UCL bioassay shows a limit of detection (LOD) of AFP down to 20 pg mL -1 (290 fM), which is the lowest among luminescent bioassays of AFP ever reported, and a 30-fold improvement relative to that of the commercial dissociation-enhanced lanthanide fluoroimmunoassay kit. Meanwhile the DSL bioassay, by employing the identical CSS NPs, can serve as a self-referential validation for the reliability and accuracy of the UCL bioassay for AFP detection. Furthermore, these CSS NPs can also function well in tumor-targeted UCL bioimaging, thereby revealing the great promise of the designed CSS NPs as red luminescent bioprobes in ultrasensitive in vitro detection of tumor markers in clinical diagnosis.

In vitro upconverting/downshifting luminescent detection of tumor markers based on Eu3+-activated core–shell–shell lanthanide nanoprobes

In vitro upconverting/downshifting luminescent detection of tumor markers based on Eu³⁺-activated core–shell–shell lanthanide nanoprobes