All-inorganic CsPbX3 (X = Cl, Br, and I) perovskite quantum dots (PeQDs) have shown great promise in optoelectronics and photovoltaics owing to their outstanding linear optical properties; however, nonlinear upconversion is limited by the small cross-section of multiphoton absorption, necessitating high power density excitation. Herein, we report a convenient and versatile strategy to fine tuning the upconversion luminescence in CsPbX3 PeQDs through sensitization by lanthanide-doped nanoparticles. Full-color emission with wavelengths beyond the availability of lanthanides is achieved through tailoring of the PeQDs bandgap, in parallel with the inherent high conversion efficiency of energy transfer upconversion under low power density excitation. Importantly, the luminescent lifetimes of the excitons can be enormously lengthened from the intrinsic nanosecond scale to milliseconds depending on the lifetimes of lanthanide ions. These findings provide a general approach to stimulate photon upconversion in PeQDs, thereby opening up a new avenue for exploring novel and versatile applications of PeQDs.

Amine-functionalized lanthanide-doped KGdF(4) nanocrystals, synthesized via a facile one-step solvothermal route by employing polyethylenimine as the surfactant and capping ligand, have been demonstrated to be sensitive time-resolved FRET bioprobes to detect a trace amount of biomolecules such as avidin at a concentration of 5.5 nM and to be potential T(1)-MRI contrast agents due to a large longitudinal relaxivity of Gd(3+) (5.86 S(-1)·mM(-1) per Gd ion and 3.99 × 10(5) S(-1)·mM(-1) per nanocrystal).

Impurity doping is an effective approach to tuning the optoelectronic performance of host materials by imparting extrinsic electronic channels. Herein, a family of lanthanide (Ln3+) ions was successfully incorporated into a Bi:Cs2AgInCl6 lead-free double-perovskite (DP) semiconductor, expanding the spectral range from visible (Vis) to near-infrared (NIR) and improving the photoluminescence quantum yield (PLQY). After multidoping with Nd, Yb, Er and Tm, Bi/Ln:Cs2AgInCl6 yielded an ultrabroadband continuous emission spectrum with a full width at half-maximum of ~365 nm originating from intrinsic self-trapped exciton recombination and abundant 4f–4f transitions of the Ln3+ dopants. Steady-state and transient-state spectra were used to ascertain the energy transfer and emissive processes. To avoid adverse energy interactions between the various Ln3+ ions in a single DP host, a heterogeneous architecture was designed to spatially confine different Ln3+ dopants via a “DP-in-glass composite” (DiG) structure. This bottom-up strategy endowed the prepared Ln3+-doped DIG with a high PLQY of 40% (nearly three times as high as that of the multidoped DP) and superior long-term stability. Finally, a compact Vis–NIR ultrabroadband (400~2000 nm) light source was easily fabricated by coupling the DiG with a commercial UV LED chip, and this light source has promising applications in nondestructive spectroscopic analyses and multifunctional lighting.