Blue, green, and red full-color ultralong afterglow in nitrogen-doped carbon dots.

Carbon dots (CDs) with tunable emission colors and multiple emission modes are highly desirable in advanced optical anti-counterfeiting. Some pioneering efforts to trigger additional long-lived emission modes, nevertheless, did not perfectly solve the issue of printability and color-tunability in practical applications. Herein, we developed an encapsulating-dissolving-recrystallization route for the synthesis of CD-based anti-counterfeiting inks, and accordingly realized blue, green, and red full-color afterglow emissions from these CD-based inks when printed on paper. The printed inks simultaneously possessed triple emission modes including fluorescence (FL), delayed fluorescence (DF), and room-temperature phosphorescence (RTP), among which the long-lived emissions (DF and RTP) could be selectively activated by using different excitation wavelengths. We believe that the proposed synthetic route in this work may promote the development of multicolor-encoded and multiple-mode-integrated optical anti-counterfeiting systems, and will expand the application of CD-based materials to the fields of sensing, photodynamic therapy and bio-imaging.

Chromium-Doped Zinc Gallogermanate@Zeolitic Imidazolate Framework-8: A Multifunctional Nanoplatform for Rechargeable In Vivo Persistent Luminescence Imaging and pH-Responsive Drug Release.

Multifunctional theranostic nanoplatforms greatly improve the accuracy and effectiveness in tumor treatments. Much effort has been made in developing advanced optical imaging-based tumor theranostic nanoplatforms. However, autofluorescence and irradiation damage of the conventional fluorescence imaging technologies as well as unsatisfied curative effects of the nanoplatforms remain great challenges against their wide applications. Herein, we constructed a novel core-shell multifunctional nanoplatform, that is, chromium-doped zinc gallogermanate (ZGGO) near-infrared (NIR) persistent luminescent nanoparticles (PLNPs) as a core and zeolitic imidazolate framework-8 (ZIF-8) as a shell (namely ZGGO@ZIF-8). The ZGGO@ZIF-8 nanoplatform possessed dual functionalities of the autofluorescence-free NIR PersL imaging as well as the pH-responsive drug delivery, thus it has high potential in tumor theranostics. Notably, the loading content of doxorubicin (DOX) in ZGGO@ZIF-8 (LC = 93.2%) was quite high, and the drug release of DOX-loaded ZGGO@ZIF-8 was accelerated in an acidic microenvironment such as tumor cells. The ZGGO@ZIF-8 opens up a new material system in the combination of PLNPs with metal-organic frameworks and may offer new opportunities for the development of advanced multifunctional nanoplatforms for tumor theranostics, chemical sensing, and optical information storage.

Tailoring Trap Depth and Emission Wavelength in Y3Al5- xGa xO12:Ce3+,V3+ Phosphor-in-Glass Films for Optical Information Storage.

Deep-trap persistent luminescent materials, due to their exceptional ability of energy storage and controllable photon release under external stimulation, have attracted considerable attention in the field of optical information storage. Currently, the lack of suitable materials is still the bottleneck that restrains their practical applications. Herein, we successfully synthesized a series of deep-trap persistent luminescent materials Y3Al5- xGa xO12:Ce3+,V3+ ( x = 0-3) with a garnet structure and developed novel phosphor-in-glass (PiG) films containing these phosphors. The synthesized PiG films exhibited sufficiently deep traps, narrow trap depth distributions, high trap density, high quantum efficiency, and excellent chemical stability, which solved the problem of chemical stability at high temperatures in the reported phosphor-in-silicone films. Moreover, the trap depth in the phosphors and PiG films could be tailored from 1.2 to 1.6 eV, thanks to the bandgap engineering effect, and the emission color was simultaneously changed from green to yellow due to the variation of crystal field strength. Image information was recorded on the PiG films by using a 450 nm blue-light laser in a laser direct writing mode and the recorded information was retrieved under high-temperature thermal stimulation or photostimulation. The Y3Al5- xGa xO12:Ce3+,V3+ PiG films as presented in this work are very promising in the applications of multidimensional and rewritable optical information storage.

Color-Tunable and High-Efficiency Dye-Encapsulated Metal-Organic Framework Composites Used for Smart White-Light-Emitting Diodes.

Luminescent metal-organic frameworks (MOFs) (typically dye-encapsulated MOFs) are considered as one kind of interesting downconversion materials for white-light-emitting diodes (LEDs), but their quantum efficiency (QE) is not sufficient and thus needs to be significantly enhanced for practical applications. In this study, we successfully synthesized a series of Rh@bio-MOF-1 (Rh = rhodamine) with an internal QE as high as ∼79% via a solvothermal reaction followed by cation exchanges. The high efficiency of the Rh@bio-MOF-1 composites was attributable to the high intrinsic luminescent efficiency of the selected Rh dyes, the confinement effect in the bio-MOF-1 host, and the uniform particle morphology. The emission maximum could be continuously tuned from 550 to 610 nm by controlling the species and concentration of encapsulated dye molecules, showing great color tunability of the dye-encapsulated MOFs. The emission lifetime of ∼7 ns was 1 or 2 magnitude orders shorter than that of Ce3+- or Eu2+-doped inorganic phosphors, allowing for visible light communication (VLC). White LEDs, fabricated by using the synthesized Rh@bio-MOF-1 composite and inorganic phosphors of green (Ba,Sr)2SiO4:Eu2+ and red CaAlSiN3:Eu2+, exhibited a high color rendering index of 80-94, a luminous efficacy of 94-156 lm/W, and an excellent stability in color point against drive current. The Rh@bio-MOF-1 composites with tunable colors, short emission lifetime, and high QE are expected to be used for smart white LEDs with multifunctions of both lighting and VLC.

Unique Color Converter Architecture Enabling Phosphor-in-Glass (PiG) Films Suitable for High-Power and High-Luminance Laser-Driven White Lighting.

As a next-generation high-power lighting technology, laser lighting has attracted great attention in high-luminance applications. However, thermally robust and highly efficient color converters suitable for high-quality laser lighting are scarce. Despite its versatility, the phosphor-in-glass (PiG) has been seldom applied in laser lighting because of its low thermal conductivity. In this work, we develop a unique architecture in which a phosphor-in-glass (PiG) film was directly sintered on a high thermally conductive sapphire substrate coated by one-dimensional photonic crystals. The designed color converter with the composite architecture exhibits a high internal quantum efficiency close to that of the original phosphor powders and an excellent packaging efficiency up to 90%. Furthermore, the PiG film can even be survived under the 11.2 W mm-2 blue laser excitation. Combining blue laser diodes with the YAG-PiG-on-sapphire plate, a uniform white light with a high luminance of 845 Mcd m-2(luminous flux: 1839 lm), luminous efficacy of 210 lm W-1, and correlated color temperature of 6504 K was obtained. A high color rendering index of 74 was attained by adding a robust orange or red phosphor layer to the architecture. These outstanding properties meet the standards of vehicle regulations, enabling the PiG films with the composite architecture to be applied in automotive lighting or other high-power and high-luminance laser lighting.

Trap Depth Engineering of SrSi2O2N2:Ln2+,Ln3+ (Ln2+ = Yb, Eu; Ln3+ = Dy, Ho, Er) Persistent Luminescence Materials for Information Storage Applications.

Deep-trap persistent luminescence materials exhibit unique properties of energy storage and controllable photon release under additional stimulation, allowing for both wavelength and intensity multiplexing to realize high-capacity storage in the next-generation information storage system. However, the lack of suitable persistent luminescence materials with deep traps is the bottleneck of such storage technologies. In this study, we successfully developed a series of novel deep-trap persistent luminescence materials in the Ln2+/Ln3+-doped SrSi2O2N2 system (Ln2+ = Yb, Eu; Ln3+ = Dy, Ho, Er) by applying the strategy of trap depth engineering. Interestingly, the trap depth can be tailored by selecting different codopants, and it monotonically increases from 0.90 to 1.18 eV in the order of Er, Ho, and Dy. This is well explained by the energy levels indicated in the host-referred binding energy scheme. The orange-red-emitting SrSi2O2N2:Yb,Dy and green-emitting SrSi2O2N2:Eu,Dy phosphors are demonstrated to be good candidates of information storage materials, which are attributed to their deep traps, narrow thermoluminescence glow bands, high emission efficiency, and excellent chemical stability. This work not only validates the suitability of deep-trap persistent luminescence materials in the information storage applications, but also broadens the avenue to explore such kinds of new materials for applications in anticounterfeiting and advanced displays.

Significantly enhanced photoluminescence and thermal stability of La3Si8N11O4:Ce3+,Tb3+ via the Ce3+ → Tb3+ energy transfer: a blue-green phosphor for ultraviolet LEDs.

A series of Ce3+-, Tb3+- and Ce3+/Tb3+-doped La3Si8N11O4 phosphors were synthesized by gas-pressure sintering (GPS). The energy transfer between Ce3+ and Tb3+ occurred in the co-doped samples, leading to a tunable emission color from blue to green under the 360 nm excitation. The energy transfer mechanism was controlled by the dipole-dipole interaction. The Ce3+/Tb3+ co-doped sample had an external quantum efficiency of 46.7%, about 5.6 times higher than the Tb-doped La3Si8N11O4 phosphor (8.3%). The thermal quenching of the Tb3+ emission in La3Si8N11O4:Tb,Ce was greatly reduced from 74 to 30% at 250 °C, owing to the energy transfer from Ce3+ to Tb3+. The blue-green La3Si8N11O4:0.01Ce,0.05Tb phosphor was testified to fabricate a warm white LED that showed a high color rendering index of 90.2 and a correlated color temperature of 3570 K. The results suggested that the co-doped La3Si8N11O4:Ce,Tb phosphor could be a potential blue-green down-conversion luminescent material for use in UV-LED pumped wLEDs.

Enhanced Photovoltage Response of Hematite-X-Ferrite Interfaces (X = Cr, Mn, Co, or Ni).

High-fluorescent p-X-ferrites (XFe2O4; XFO; X = Fe, Cr, Mn, Co, or Ni) embedded in n-hematite (Fe2O3) surfaces were successfully fabricated via a facile bio-approach using Shewanella oneidensis MR-1. The results revealed that the X ions with high/low work functions modify the unpaired spin Fe2+-O2- orbitals in the XFe2O4 lattices to become localized paired spin orbitals at the bottom of conduction band, separating the photovoltage response signals (73.36~455.16/-72.63~-32.43 meV). These (Fe2O3)-O-O-(XFe2O4) interfacial coupling behaviors at two fluorescence emission peaks (785/795 nm) are explained via calculating electron-hole effective masses (Fe2O3-FeFe2O4 17.23 × 10-31 kg; Fe2O3-CoFe2O4 3.93 × 10-31 kg; Fe2O3-NiFe2O4 11.59 × 10-31 kg; Fe2O3-CrFe2O4 -4.2 × 10-31 kg; Fe2O3-MnFe2O4 -11.73 × 10-31 kg). Such a system could open up a new idea in the design of photovoltage response biosensors.

Mechanism of Fluorescence Enhancement of Biosynthesized XFe2O4-BiFeO3 (X = Cr, Mn, Co, or Ni) Membranes.

Ferrites-bismuth ferrite is an intriguing option for medical diagnostic imaging device due to its magnetoelectric and enhanced near-infrared fluorescent properties. However, the embedded XFO nanoparticles are randomly located on the BFO membranes, making implementation in devices difficult. To overcome this, we present a facile bio-approach to produce XFe2O4-BiFeO3 (XFO-BFO) (X = Cr, Mn, Co, or Ni) membranes using Shewanella oneidensis MR-1. The perovskite BFO enhances the fluorescence intensity (at 660 and 832 nm) and surface potential difference (-469 ~ 385 meV and -80 ~ 525 meV) of the embedded spinel XFO. This mechanism is attributed to the interfacial coupling of the X-Fe (e- or h+) and O-O (h+) interfaces. Such a system could open up new ideas in the design of environmentally friendly fluorescent membranes.