Distinctive upconversion or downshifting of lanthanide nanocrystals holds promise for biomedical and photonic applications. However, either process requires high-energy lasers at discrete wavelengths for excitation. Here we demonstrate that co-sensitization can break this limitation with ultrawide excitation bands. We achieve co-sensitization by employing Nd3+ and Ho3+ as the co-sensitizers with complementary absorptions from the ultraviolet to infrared region. Symmetric penta-layer core-shell nanostructure enables tunable fluorescence in the visible and the second near-infrared window when incorporating different activators (Er3+, Ho3+, Pr3+, and Tm3+). Transient spectra confirm the directional energy transfer from sensitizers to activators through the bridge of Yb3+. We validate the features of the nanocrystals for low-powered white light-emitting diode-mediated whole-body angiography of mice with a signal-to-noise ratio of 12.3 and excitation-regulated encryption. This co-sensitization strategy paves a new way in lanthanide nanocrystals for multidirectional photon conversion manipulation and excitation-bandwidth-regulated fluorescence applications.
© 2023. The Author(s).