Cross Relaxation Enables Spatiotemporal Color-Switchable Upconversion in a Single Sandwich Nanoparticle for Information Security.

Smart control of ionic interaction dynamics offers new possibilities for tuning and editing luminescence properties of lanthanide-based materials. However, it remains a daunting challenge to achieve the dynamic control of cross relaxation mediated photon upconversion, and in particular the involved intrinsic photophysics is still unclear. Herein, this work reports a conceptual model to realize the color-switchable upconversion of Tm3+ through spatiotemporal control of cross relaxation in the design of NaYF4:Gd@NaYbF4:Tm@NaYF4 sandwich nanostructure. It shows that cross relaxation plays a key role in modulating upconversion dynamics and tuning emission colors of Tm3+. Interestingly, it is found that there is a short temporal delay for the occurrence of cross relaxation in contrast to the spontaneous emission as a result of the slight energy mismatch between relevant energy levels. This further enables a fine emission color tuning upon non-steady state excitation. Moreover, a characteristic quenching time is proposed to describe the temporal evolution of cross relaxation quantitatively. These findings present a deep insight into the physics of ionic interactions in heavy doping systems, and also show great promise in frontier applications including information security, anti-counterfeiting and nanophotonics.

Carbon Dots in Hydroxy Fluorides: Achieving Multicolor Long-Wavelength Room-Temperature Phosphorescence and Excellent Stability via Crystal Confinement.

Carbon dots (CDs) have aroused widespread interest in the construction of room-temperature phosphorescent (RTP) materials. However, it is a great challenge to obtain simultaneous multicolor long-wavelength RTP emission and excellent stability in CD-based RTP materials. Herein, a novel and universal "CDs-in-YOHF" strategy is proposed to generate multicolor and long-wavelength RTP by confining various CDs in the Y(OH)xF3-x (YOHF) matrix. The mechanism of the triplet emission of CDs is related to the space confinement, the formation of hydrogen bonds and C-F bonds, and the electron-withdrawing fluorine atoms. Remarkably, the RTP lifetime of orange-emissive CDs-o@YOHF is the longest among the reported single-CD-matrix composites for emission above 570 nm. Furthermore, CDs-o@YOHF exhibited higher RTP performance at long wavelength in comparison to CDs-o@matrix (matrix = PVA, PU, urea, silica). The resulting CDs@YOHF shows excellent photostability, thermostability, chemical stability, and temporal stability, which is rather favorable for information security, especially in a complex environment.

Near-Infrared-Excited Multicolor Afterglow in Carbon Dots-Based Room-Temperature Afterglow Materials.

Room-temperature afterglow (RTA) materials with long lifetime have shown tremendous application prospects in many fields. However, there is no general design strategy to construct near-infrared (NIR)-excited multicolor RTA materials. Herein, we report a universal approach based on the efficient radiative energy transfer that supports the reabsorption from upconversion materials (UMs) to carbon dots-based RTA materials (CDAMs). Thus, the afterglow emission (blue, cyan, green, and orange) of various CDAMs can be activated by UMs under the NIR continuous-wave laser excitation. The efficient radiative energy transfer ensured the persistent multicolor afterglow up to 7 s, 6 s, 5 s, and 0.5 s by naked eyes, respectively. Given the unusual afterglow properties, we demonstrated preliminary applications in fingerprint recognition and information security. This work provides a new avenue for the activation of NIR-excited afterglow in CDAMs and will greatly expand the applications of RTA materials.

Red, orange, yellow and green luminescence by carbon dots: hydrogen-bond-induced solvation effects.

The mechanism of the solvation-dependent multicolor luminescence of carbon dots (CDs) is not clear, despite the fact that multicolor luminescent CDs have important applications in many fields. In this article, we report solvated chromogenic CDs with productivity of up to 57%. The luminescence of the CD particles exhibits a regular redshift in N,N-dimethylformamide (DMF), ethanol, water, and acetic acid. The redshift of the CDs may be ascribed to the linking of the CD surfaces to the solvent through hydrogen bonds (HB). Different surface level states are formed by HB between the surfaces of the CDs and the solvent, and differences in dispersion states lead to different energy resonance transfer (ETR) efficiencies. The CDs/B2O3 composite exhibits excellent fluorescence thermal stability, and it has also been used to manufacture white-light-emitting devices with a high color rendering index of 87. Additionally, the excellent solvation effects of the CDs have application prospects in the detection of the water content in organic solvents. Finally, the CDs are used to realize cell imaging and positioning, which has significant application prospects in biological fields.