White light-emitting diodes (WLEDs) as new solid-state light sources have a greatly promising application in the field of lighting and display. So far much effort has been devoted to exploring novel luminescent materials for WLEDs. Currently the major challenges in WLEDs are to achieve high luminous efficacy, high chromatic stability, brilliant color-rending properties, and price competitiveness against fluorescent lamps, which rely critically on the phosphor properties. In recent years, numerous efforts have been made to develop single-phase white-light-emitting phosphors for near-ultraviolet or ultraviolet excitation to solve the above challenges with certain achievements. This review article highlights the current methods to realize the white light emission in a single-phase host, including: (1) doping a single rare earth ion (Eu(3+), Eu(2+) or Dy(3+)) into appropriate single-phase hosts; (2) co-doping various luminescent ions with different emissions into a single matrix simultaneously, such as Tm(3+)/Tb(3+)/Eu(3+), Tm(3+)/Dy(3+), Yb(3+)/Er(3+)/Tm(3+)etc.; (3) codoping different ions in one host to control emission color via energy transfer processes; and (4) controlling the concentration of the defect and reaction conditions of defect-related luminescent materials.
Red phosphor materials play a key role in improving the lighting and backlit display quality of phosphor-converted white light-emitting diodes (pc-WLEDs). However, the development of a red phosphor with simultaneous high efficiency, excellent thermal stability and high colour purity is still a challenge. In this work, unique non-concentration quenching in solid-solution Cs3Gd1 − xGe3O9:xEu3+ (CGGO:xEu3+) (x = 0.1–1.0) phosphors is successfully developed to achieve a highly efficient red-emitting Cs3EuGe3O9 (CEGO) phosphor. Under the optimal 464 nm blue light excitation, CEGO shows a strong red emission at 611 nm with a high colour purity of 95.07% and a high internal quantum efficiency of 94%. Impressively, this red-emitting CEGO phosphor exhibits a better thermal stability at higher temperatures (175–250 °C, >90%) than typical red K2SiF6:Mn4+ and Y2O3:Eu3+ phosphors, and has a remarkable volumetric negative thermal expansion (coefficient of thermal expansion, α = −5.06 × 10−5/°C, 25–250 °C). By employing this red CEGO phosphor, a fabricated pc-WLED emits warm white light with colour coordinates (0.364, 0.383), a high colour rendering index (CRI = 89.7), and a low colour coordinate temperature (CCT = 4508 K). These results indicate that this highly efficient red-emitting phosphor has great potential as a red component for pc-WLEDs, opening a new perspective for developing new phosphor materials.
Near‐infrared (NIR)‐emitting phosphor materials have been extensively developed for optoelectronic and biomedical applications. Although Cr3+‐activated phosphors have been widely reported, it is challenging to achieve ultra‐broad and tunable NIR emission. Here, a new ultra‐broadband NIR‐emitting LiIn2SbO6:Cr3+ phosphor with emission peak at 965 nm and a full‐width at half maximum of 217 nm is reported. Controllable emission tuning from 965 to 892 nm is achieved by chemical unit cosubstitution of [Zn2+–Zn2+] for [Li+–In3+], which can be ascribed to the upshift of 4T2g energy level due to the strengthened crystal field. Moreover, the emission is greatly enhanced, and the FWHM reaches 235 nm. The as‐prepared luminescent tunable NIR‐emitting phosphors have demonstrated the potential in night‐vision and NIR spectroscopy techniques. This work proves the feasibility of chemical unit cosubstitution strategy in emission tuning of Cr3+‐doped phosphors, which can stimulate further studies on the emission‐tunable NIR‐emitting phosphor materials.
A novel approach for the fabrication of multifunctional microspheres integrating several advantages of mesoporous, luminescence, and temperature responses into one single entity is reported. First, the hollow mesoporous silica capsules are fabricated via a sacrificial template route. Then, Gd2O3:Eu3+ luminescent nanoparticles are incorporated into the internal cavities to form rattle‐type mesoporous silica nanocapsules by an incipient‐wetness impregnation method. Finally, the rattle‐type capsules serve as a nanoreactor for successfully filling temperature‐responsive hydrogel via photoinduced polymerization to form the multifunctional composite microspheres. The organic–inorganic hybrid microspheres show a red emission under UV irradiation due to the luminescent Gd2O3:Eu3+ core. The in vitro cytotoxicity tests show that the samples have good biocompatibility, which indicates that the nanocomposite could be a promising candidate for drug delivery. In addition, flow cytometry and confocal laser scanning microscopy (CLSM) confirm that the sample can be effectively taken up by SKOV3 cells. For in vitro magnetic resonance imaging (MRI), the sample shows the promising spin‐lattice relaxation time (T1) weighted effect and could potentially apply as a T1‐positive contrast agent. This composite drug delivery system (DDS) provides a positive temperature controlled “on‐off”drug release pattern and the drug, indomethacin (IMC), is released fast at 45 °C (on phase) and completely shut off at 20 °C (off phase). Meanwhile Gd2O3:Eu3+ plays an important role as the luminescent tag for tracking the drug loading and release process by the reversible luminescence quenching and recovery phenomenon. These results indicate that the obtained multifunctional composite has the potential to be used as a smart DDS for biomedical applications.
A series of Ca(4)Y(6)(SiO(4))(6)O (CYS): Ce(3+)/Mn(2+)/Tb(3+) oxyapatite phosphors were prepared via high-temperature solid-state reaction. Under UV excitation, there exist dual energy transfers (ET), i.e., Ce(3+)→Mn(2+) and Ce(3+)→Tb(3+) in the CYS: Ce(3+), Mn(2+), Tb(3+) system and their emitting colors can be adjusted from blue to orange-red via ET of Ce(3+)→Mn(2+) and from blue to green via ET of Ce(3+)→Tb(3+), respectively. Moreover, a wide-range-tunable white light emission with high quantum yields (13%-30%) were obtained by precisely controlling the contents of Ce(3+), Mn(2+) and Tb(3+) ions. On the other hand, the CL properties of CYS: Ce(3+), Mn(2+), Tb(3+) phosphors have been investigated in detail. The studied results indicate that the as-prepared CYS: Ce(3+), Mn(2+), Tb(3+) phosphors have good CL intensity and CIE color coordinate stability with a color-tunable emission crossing the whole white light region under low-voltage electron beam excitation. In general, the white light with varied hues has been obtained in Ce(3+), Mn(2+), and Tb(3+)-triactivated CYS phosphors by utilizing the principle of energy transfer and properly designed activator contents under UV (284, 358 nm) and low-voltage (1-5 kV) electron beam excitation, which make them as a potential single-composition trichromatic white-emitting phosphor.
CoreÀshell structured up-conversion luminescent and mesoporous NaYF 4 :Yb 3+ /Er 3+ @nSiO 2 @mSiO 2 nanospheres were prepared by coating mesoporous SiO 2 layers with different thicknesses on NaYF 4 :Yb 3+ / Er 3+ nanoparticles via a simple two-step solÀgel process. The obtained sample shows a typical mesoporous structure and well-dispersed spherical morphology with a narrow size distribution. The nanospheres exhibit little cytotoxicity (via MTT assay), and ibuprofen (IBU) was used as a model drug to access the release properties of the system in detail. The amount of IBU adsorbed in mesoporous channels increases with the thickness of the ordered mesoporous silica shell coated on the NaYF 4 :Yb 3+ /Er 3+ nanoparticles. The in vitro release study of IBU reveals a release profile in two steps: an initial diffusion-controlled release, followed by a slower release rate. Furthermore, upon excitation by a 980 nm near-infrared laser, the nanospheres emit green ( 2 H 11/2 and 4 S 3/2 f 4 I 15/2 ) and red ( 4 F 9/2 f 4 I 15/2 ) fluorescence of Er 3+ even after the loading of IBU. Interestingly, the emission intensity of Er 3+ in the bifunctional (mesoporous and luminescence) drug carrier increases with an increase of the cumulative released amount of the model drug (IBU). Thus, the extent of drug release can be easily identified, tracked, and monitored based on the change of the up-conversion luminescence. These results suggest that the coreÀshell structured NaYF 4 :Yb 3+ /Er 3+ @nSiO 2 @m-SiO 2 nanospheres are a promising material for controlled drug release.
LaCO(3)OH nano/microcrystals with a variety of morphologies/sizes including nanoflakes, microflowers, nano/microrhombuses, two-double microhexagrams sandwichlike microspindles, and peach-nucleus-shaped microcrystals have been synthesized via a facile homogeneous precipitation route under mild conditions. A series of controlled experiments indicate that the pH values in the initial reaction systems, carbon sources, and simple ions (NH(4)(+) and Na(+)) were responsible for the shape determination of the LaCO(3)OH products. A possible formation mechanism for these products with diverse architectures has been presented. After annealing at suitable temperatures, LaCO(3)OH was easily converted to La(2)O(2)CO(3) and La(2)O(3) with the initial morphologies. A systematic study on the photoluminescence and cathodoluminescence properties of Eu(3+)- or Tb(3+)-doped La(2)O(2)CO(3)/La(2)O(3) samples has been performed in detail. The excitation and site-selective emission spectra were recorded to investigate the microstructure, site symmetry, and difference in the (5)D(0) → (7)F(2) transition of Eu(3+) ions in La(2)O(2)CO(3) and La(2)O(3) host lattices. In addition, the dependence of the luminescent intensity on the morphology for the as-prepared La(2)O(2)CO(3)/La(2)O(3):Ln(3+) (Ln = Eu, Tb) samples has been investigated. The ability of generating diverse morphologies and multiemitting colors for different rare-earth activator ion (Ln = Eu, Tb) doped La(2)O(2)CO(3)/La(2)O(3) nano/microstructures provides a great opportunity for the systematic evaluation of morphology-dependent luminescence properties, as well as the full exploration of their application in many types of color display fields.
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