High Color-Purity Green, Orange, and Red Light-Emitting Didoes Based on Chemically Functionalized Graphene Quantum Dots.
ABSTRACT: Chemically derived graphene quantum dots (GQDs) to date have showed very broad emission linewidth due to many kinds of chemical bondings with different energy levels, which significantly degrades the color purity and color tunability. Here, we show that use of aniline derivatives to chemically functionalize GQDs generates new extrinsic energy levels that lead to photoluminescence of very narrow linewidths. We use transient absorption and time-resolved photoluminescence spectroscopies to study the electronic structures and related electronic transitions of our GQDs, which reveals that their underlying carrier dynamics is strongly related to the chemical properties of aniline derivatives. Using these functionalized GQDs as lumophores, we fabricate light-emitting didoes (LEDs) that exhibit green, orange, and red electroluminescence that has high color purity. The maximum current efficiency of 3.47?cd A(-1) and external quantum efficiency of 1.28% are recorded with our LEDs; these are the highest values ever reported for LEDs based on carbon-nanoparticle phosphors. This functionalization of GQDs with aniline derivatives represents a new method to fabricate LEDs that produce natural color.
Project description:Cesium lead halide perovskite nanocrystals (NCs) have unique optical properties such as high color purity and high photoluminescence (PL) efficiency. However, the external quantum efficiency (EQE) of the corresponding light-emitting diodes (LEDs) is low, primarily as a result of the NC surface defects. Here, we report a method to reduce the surface defects by capping CsPbI<sub>3</sub> NCs with PbS. This passivation significantly enhanced the PL efficiency, reduced the Stokes shift, narrowed the PL bandwidth, and increased the stability of CsPbI<sub>3</sub> NCs. At the same time, CsPbI<sub>3</sub> NC films switched from <i>n</i>-type behavior to nearly ambipolar by PbS capping, which allowed us to fabricate electroluminescence LEDs using <i>p</i>-<i>i</i>-<i>n</i> structures. The thus-fabricated LEDs exhibited dramatically improved storage and operation stability, and an EQE of 11.8%. These results suggest that, with a suitable surface passivation strategy, the perovskite NCs are promising for next-generation LED and display applications.
Project description:Monolithic phosphor-free two-color gallium nitride (GaN)-based white light emitting diodes (LED) have the potential to replace current phosphor-based GaN white LEDs due to their low cost and long life cycle. Unfortunately, the growth of high indium content indium gallium nitride (InGaN)/GaN quantum dot and reported LED's color rendering index (CRI) are still problematic. Here, we use flip-chip technology to fabricate an upside down monolithic two-color phosphor-free LED with four grown layers of high indium quantum dots on top of the three grown layers of lower indium quantum wells separated by a GaN tunneling barrier layer. The photoluminescence (PL) and electroluminescence (EL) spectra of this white LED reveal a broad spectrum ranging from 475 to 675 nm which is close to an ideal white-light source. The corresponding color temperature and color rendering index (CRI) of the fabricated white LED, operated at 350, 500, and 750 mA, are comparable to that of the conventional phosphor-based LEDs. Insights of the epitaxial structure and the transport mechanism were revealed through the TEM and temperature dependent PL and EL measurements. Our results show true potential in the Epi-ready GaN white LEDs for future solid state lighting applications.
Project description:Inorganic perovskite quantum dots bear many unique properties that make them potential candidates for optoelectronic applications, including color display and lighting. However, the white emission with inorganic perovskite quantum dots has rarely been realized due to the anion-exchange reaction. Here, we proposed a one-pot preparation to fabricate inorganic perovskite quantum dot-based white light-emitting composites by introducing anthracene as a blue emission component. The as-prepared white light-emitting composite exhibited a photoluminescence quantum yield of 41.9%. By combining CsPb(Br/I)3@anthracene composites with UV light-emitting device (LED) chips, white light-emitting devices with a color rendering index of 90 were realized with tunable color temperature from warm white to cool white. These results can promote the application of inorganic perovskite quantum dots in the field of white LEDs.
Project description:Achieving perovskite-based high-color purity blue-emitting light-emitting diodes (LEDs) is still challenging. Here, we report successful synthesis of a series of blue-emissive two-dimensional Ruddlesden-Popper phase single crystals and their high-color purity blue-emitting LED demonstrations. Although this approach successfully achieves a series of bandgap emissions based on the different layer thicknesses, it still suffers from a conventional temperature-induced device degradation mechanism during high-voltage operations. To understand the underlying mechanism, we further elucidate temperature-induced device degradation by investigating the crystal structural and spectral evolution dynamics via in situ temperature-dependent single-crystal x-ray diffraction, photoluminescence (PL) characterization, and density functional theory calculation. The PL peak becomes asymmetrically broadened with a marked intensity decay, as temperature increases owing to [PbBr6]4- octahedra tilting and the organic chain disordering, which results in bandgap decrease. This study indicates that careful heat management under LED operation is a key factor to maintain the sharp and intense emission.
Project description:Metal halide perovskite quantum dots (QDs) have attracted significant research interest in the next-generation display and solid illumination fields due to their excellent optical properties of high photoluminescence quantum efficiency, high color purity, obvious quantum confinement effect, and large exciton binding energy. A large amount of surface defects and nonradiative recombination induced by these defects are considered as major problems to be resolved urgently for practical applications of perovskite QDs in high-efficiency light-emitting diodes (LEDs). Herein, we report an efficient passivation of green perovskite QD CH3NH3PbBr3 with trioctylphosphine oxide (TOPO). By simply adding the appropriate amount of TOPO into the nonpolar toluene solvent to synthesize CH3NH3PbBr3 QDs, the surface defects of these as-synthesized perovskite QDs are obviously reduced, along with an increased photoluminescence lifetime and suppressed nonradiative recombination. Further investigation indicates that electronegative oxygen from TOPO (Lewis base) bonds with uncoordinated Pb2+ ions and labile lead atoms in perovskite. With TOPO passivation, the green perovskite QD LEDs based on CH3NH3PbBr3 show significant performance improvement factors of 93.5, 161.1, and 168.9% for luminance, current efficiency, and external quantum efficiency, respectively, reaching values of 1635 cd m-2, 5.51 cd A-1, and 1.64% in the eventual optimized devices. Furthermore, the presence of TOPO dramatically improves stabilities of CH3NH3PbBr3 QDs and related devices. Our work provides a robust platform for the fabrication of low-defect-density perovskite QDs and efficient, stable perovskite QD LEDs.
Project description:Perovskite quantum dots (PQDs) are a competitive candidate for next-generation display technologies as a result of their superior photoluminescence, narrow emission, high quantum yield, and color tunability. However, due to poor thermal resistance and instability under high energy radiation, most PQD-based white light-emitting diodes (LEDs) show only modest luminous efficiency of ?50 lm W-1 and a short lifetime of <100 h. In this study, by incorporating cellulose nanocrystals, a new type of QD film is fabricated: CH3NH3PbBr3 PQD paper that features 91% optical absorption, intense green light emission (518 nm), and excellent stability attributed to the complexation effect between the nanocellulose and PQDs. The PQD paper is combined with red K2SiF6:Mn4+ phosphor and blue GaN LED chips to fabricate a high-performance white LED demonstrating ultrahigh luminous efficiency (124 lm W-1), wide color gamut (123% of National Television System Committee), and long operation lifetime (240 h), which paves the way for advanced lighting technology.
Project description:Graphene quantum dots (GQDs) with an average diameter of 3.5 nm were prepared via pulsed laser ablation. The synthesized GQDs can improve the optical and electrical properties of InGaN/InAlGaN UV light emitting diodes (LEDs) remarkably. An enhancement of electroluminescence and a decrease of series resistance of LEDs were observed after incorporation of GQDs on the LED surface. As the GQD concentration is increased, the emitted light (series resistance) in the LED increases (decreases) accordingly. The light output power achieved a maximum increase as high as 71% after introducing GQDs with the concentration of 0.9 mg/ml. The improved performance of LEDs after the introduction of GQDs is explained by the photon recycling through the light extraction from the waveguide mode and the carrier transfer from GQDs to the active layer.
Project description:Large-scale applications of conventional rare-earth phosphors in white light-emitting diodes (W-LEDs) are restricted by the non-renewable raw material sources and high energy consumption during the production process. Recently, carbon dots (CDs) have been proposed as promising alternatives to rare-earth phosphors and present bright prospects in white lighting. However, the use of CDs in W-LEDs still has two major obstacles, i.e., solid-state quenching and lack of single-component white emissive products. In this work, a facile, rapid, and scalable method for the preparation of solid-state white emissive CDs (W-CDs) is reported via microwave-irradiation heating of L-aspartic acid (AA) in the presence of ammonia. The W-CDs exhibit blue photoluminescence (PL) in dilute aqueous dispersion and their emission spectra gradually broaden (emerging new emissions at orange-yellow regions) with concentration increases. Interestingly, the W-CDs powder displays a very broad PL spectrum covering nearly the whole visible-light region under ultraviolet (UV) excitation, which is responsible for the observed white emission. Further studies revealed that the self-quenching-resistance feature of the W-CDs is probably due to a covering of polymer-like structures on their surface, thus avoiding the close contact of nanoparticles with each other. PL emission of the W-CDs is reasonably ascribed to a cross-linked enhanced effect (CEE) of the sub-fluorophores contained in the material (e.g., -NH2 and C=O). Finally, applications of the W-CDs in fabricating single-component-based W-LEDs using commercially available UV chips were attempted and shown to exhibit satisfactory performances including high white light-emitting purity, high color rendering index (CRI), and tunable correlated color temperature (CCT), thus rendering great promise for W-CDs in the field of white lighting.
Project description:A search for new phosphor materials that exhibit high light-emission, spectral purity, long-time stability and processability capture particular attention to modern solid-state lighting. Here, polymerizable silane pre-functionalized carbon dot (SiCD) fluids were dripped and co-polymerized or completely bulk polymerized to build color conversion and encapsulation coatings of commercially available GaN blue LEDs. Most parameters of SiCD-based white LEDs were similar to or even better than those of phosphor-based white LEDs, particularly the insensitivity to excitation wavelength and working current. Thus, SiCDs were superior to those phosphors in terms of broadband properties, high transparency (no light blocking and leaking), as well as arbitrary doping of its content as color conversion and encapsulation layers simultaneously, unique solubility, flexible chemical, optical and mechanical processability. Thus, designing new CD-based white LEDs, instead of inorganic rare earth phosphor-based LEDs, is possible for better performance solid state lighting devices.
Project description:Although number of stimuli-responsive drug delivery systems based on mesoporous silica nanoparticles (MSNs) have been developed, the simultaneous real-time monitoring of carrier in order to guarantee proper drug targeting still remains as a challenge. GQDs-MSNs nanocomposite nanoparticles composed of graphene quantum dots (GQDs) and MSNs are proposed as efficient doxorubicin delivery and fluorescent imaging agent, allowing to monitor intracellular localization of a carrier and drug diffusion route from the carrier. Graphene quantum dots (average diameter 3.65?±?0.81 nm) as a fluorescent agent were chemically immobilized onto mesoporous silica nanoparticles (average diameter 44.08?±?7.18 nm) and loaded with doxorubicin. The structure, morphology, chemical composition, and optical properties as well as drug release behavior of doxorubicin (DOX)-loaded GQDs-MSNs were investigated. Then, the in vitro cytotoxicity, cellular uptake, and intracellular localization studies were carried out. Prepared GQDs-MSNs form stable suspensions exhibiting excitation-dependent photoluminescence (PL) behavior. These nanocomposite nanoparticles can be easily DOX-loaded and show pH- and temperature-dependent release behavior. Cytotoxicity studies proved that GQDs-MSNs nanocomposite nanoparticles are nontoxic; however, when loaded with drug, they enable the therapeutic activity of DOX via its active delivery and release. GQDs-MSNs owing to their fluorescent properties and efficient in vitro cellular internalization via caveolae/lipid raft-dependent endocytosis show a high potential for the optical imaging, including the simultaneous real-time optical tracking of the loaded drug during its delivery and release. Graphical abstract?.