Patterning nanoroads and quantum dots on fluorinated graphene

Using ab initio methods we have investigated the fluorination of graphene and find that different stoichiometric phases can be formed without a nucleation barrier, with the complete “2D-Teflon” CF phase being thermodynamically most stable. The fluorinated graphene is an insulator and turns out to be a perfect matrix-host for patterning nanoroads and quantum dots of pristine graphene. The electronic and magnetic properties of the nanoroads can be tuned by varying the edge orientation and width. The energy gaps between the highest occupied and lowest unoccupied molecular orbitals (HOMO-LUMO) of quantum dots are size-dependent and show a confinement typical of Dirac fermions. Furthermore, we study the effect of different basic coverage of F on graphene (with stoichiometries CF and C₄F) on the band gaps, and show the suitability of these materials to host quantum dots of graphene with unique electronic properties.     

量子点材料应用于发光二极管的研究进展

量子点材料因具有独特的光学特性而被广泛应用于发光领域,用其作发光层可制成量子点发光二极管。与有机电致发光二极管相比,量子点发光二极管具有发光光谱窄、色域广、稳定性好、寿命长、制作成本低等优势。本文介绍了量子点发光器件在国内外的热点研究方向及取得的成果,并对其发展前景进行展望。     

InGaAs quantum dots grown by molecular beam epitaxy for light emission on Si substrates

The aim of this study is to achieve homogeneous, high density and dislocation free InGaAs quantum dots grown by molecular beam epitaxy for light emission on silicon substrates. This work is part of a project which aims at overcoming the severe limitation suffered by silicon regarding its optoelectronic applications, especially efficient light emission device. For this study, one of the key points is to overcome the expected type II InGaAs/Si interface by inserting the InGaAs quantum dots inside a thin silicon quantum well in SiO2 fabricated on a SOI substrate. Confinement effects of the Si/SiO2 quantum well are expected to heighten the indirect silicon bandgap and then give rise to a type I interface with the InGaAs quantum dots. Band structure and optical properties are modeled within the tight binding approximation: direct energy bandgap is demonstrated in SiO2/Si/InAs/Si/SiO2 heterostructures for very thin Si layers and absorption coefficient is calculated. Thinned SOI substrates are successfully prepared using successive etching process resulting in a 2 nm-thick Si layer on top of silica. Another key point to get light emission from InGaAs quantum dots is to avoid any dislocations or defects in the quantum dots. We investigate the quantum dot size distribution, density and structural quality at different V/III beam equivalent pressure ratios, different growth temperatures and as a function of the amount of deposited material. This study was performed for InGaAs quantum dots grown on Si(001) substrates. The capping of InGaAs quantum dots by a silicon epilayer is performed in order to get efficient photoluminescence emission from quantum dots. Scanning transmission electronic microscopy images are used to study the structural quality of the quantum dots. Dislocation free In50Ga50As QDs are successfully obtained on a (001) silicon substrate. The analysis of QDs capped with silicon by Rutherford Backscattering Spectrometry in a channeling geometry is also presented.     

Solution-Processable Pure Green Thermally Activated Delayed Fluorescence Emitter Based on the Multiple Resonance Effect

Thermally activated delayed fluorescence (TADF) materials based on the multiple resonance (MR) effect are applied in organic light-emitting diodes (OLEDs), combining high color purity and efficiency. However, they are not fabricated via solution-processing, which is an economical approach toward the mass production of OLED displays. Here, a solution-processable MR-TADF material (OAB-ABP-1), with an extended π-skeleton and bulky substituents, is designed. OAB-ABP-1 is synthesized from commercially available starting materials via a four-step process involving one-shot double borylation. OAB-ABP-1 presents attractive photophysical properties, a narrow emission band, a high photoluminescence quantum yield, a small energy gap between S₁ and T₁, and low activation energy for reverse intersystem crossing. These properties are attributed to the alternating localization of the highest occupied and lowest unoccupied molecular orbitals induced by the boron, nitrogen, and oxygen atoms. Furthermore, to facilitate charge recombination, two novel semiconducting polymers with similar ionization potentials to that of OAB-ABP-1 are synthesized for use as interlayer and emissive layer materials. A solution-processed OLED device is fabricated using OAB-ABP-1 and the aforementioned polymers; it exhibits pure green electroluminescence with a small full-width at half-maximum and a high external quantum efficiency with minimum efficiency roll-off.     

Indium Phosphide‐Based Quantum Dots with Shell‐Enhanced Absorption for Luminescent Down‐Conversion

It is shown that admixing small amounts of cadmium into the shell of InP/ZnSe core/shell quantum dots results in an increased absorption of blue light and a limited redshift of the band‐edge emission. These effects reflect the reduced bandgap of (Zn,Cd)Se alloys and their smaller conduction‐band offset with InP. Nevertheless, adjusting the InP core size enables InP/ZnSe and InP/(Zn,Cd)Se quantum dots with identical emission characteristics to be made. Processing both materials into remote phosphor disks, it is demonstrated that the shell‐enhanced absorbance of InP/(Zn,Cd)Se has the double benefit of suppressing self‐absorption and reducing the amount of quantum dots by weight needed to attain a given blue‐to‐red color conversion.     

Synthesis and modulation of the optical properties of carbon quantum dots using microwave radiation

Abstract

Carbon quantum dots have exhibited highly fluorescent characteristics as nanomaterials. Soluble in water and easily synthesized by multiple simple techniques, there are immense fabrication possibilities by permuting their properties via changing precursors, synthesis route, reaction parameters, etc. As economic and environment-friendly seed material, they are being viewed as an alternative to conventional fluorescent materials in myriad of applications including displays, cancer detection, drug delivery carriers in biomedicine, absorbing material in photovoltaics, etc. In this work, the hydrophilic carbon quantum dots were synthesized from the aqueous solution of citric acid and urea through microwave radiation for varying heat durations. The method is facile, faster and friendly to the environment without any need for high temperature and complicated chemical techniques. It was observed that the bandgap of the fabricated carbon quantum dots and its optical properties namely absorbance, photoluminescence enhanced with an increase in exposure of samples to heat up to an optimum limit, owing to the increase in density of states. However, further exposure to heat for longer duration degraded the absorbance and bandgap while photoluminescence gets saturated. Stokes’ shift revealed that all the synthesized carbon quantum dots possess stable emission. This was reconfirmed from consistent emission peak positions under varying excitation in the samples. The absorbance and PL spectrum exhibited by the synthesized dots makes it a suitable material for boosting the performance of organic solar cell.     

Dual-mode emission of single-layered graphene quantum dots in confined nanospace: Anti-counterfeiting and sensor applications

Nano Research - Engineering of the luminescent properties for graphene quantum dots (GQDs) presents two enormous challenges: 1) The bandgap of GQDs is mainly determined by structural defects (size,...     

Exciplex kinetics in nanocrystal organic light-emitting diodes

We studied the exciplex kinetics in nanocrystal organic light-emitting diodes (NC-OLEDs) where the emissive layer of inorganic nanocrystal quantum dots is sandwiched between the electron and hole transport layers of organic semiconductors at the organic–organic interface. We modeled exciplex generation, diffusion, recombination, and capture by nanocrystals via the F?rster mechanism in NC-OLEDs. The exciplex kinetics determines the NC-OLED operation characterized by the quantum yield efficiency and emission intensity and it can be optimized by controlling the nanocrystal separation in the NC-OLED.     

Bandgap engineered graphene and hexagonal boron nitride for resonant tunnelling diode

In this article a double-barrier resonant tunnelling diode (DBRTD) has been modelled by taking advantage of single-layer hexagonal lattice of graphene and hexagonal boron nitride (h-BN). The DBRTD performance and operation are explored by means of a self-consistent solution inside the non-equilibrium Green’s function formalism on an effective mass-Hamiltonian. Both p- and n-type DBRTDs exhibit a negative differential resistance effect, which entails the resonant tunnelling through the hole and electron bound states in the graphene quantum well, respectively. The peak-to-valley ratio of approximately 8 (3) for p-type (n-type) DBRTD with quantum well of 5.1 nm (4.3 nm) at a barrier width of 1.3 nm was achieved for zero bandgap graphene at room temperature.     

53% Efficient Red Emissive Carbon Quantum Dots for High Color Rendering and Stable Warm White‐Light‐Emitting Diodes

Red emissive carbon quantum dots (R‐CQDs) with quantum yield of 53% is successfully prepared. An ultraviolet (UV)‐pumped CQD phosphors‐based warm white light‐emitting diode (WLED) is realized for the first time and achieves a color rendering index of 97. This work provides a new avenue for the exploration of low cost, environment‐friendly, and high‐performance CQD phosphors‐based warm WLEDs.     

AgInS2和Ag—Zn—In—S量子点的制备及表征

采用热注入法成功制备出三元AgInS2和四元Ag—Zn—In—S量子点,物性测试得到AgInS2量子点的发射峰为701nm,Ag—Zn—In—S量子点的发射峰593nm,即Ag-Zn-In—S量子点的发射峰相对于AgInS2量子点发生了蓝移,AgInS2和Ag—Zn—In—S量子点都表现出了较长的荧光寿命,分别为169ns和162ns,结合生物组织光学窗口范围限制,相对Ag—Z—In—S,AgInS2量子点更适用于生物标记。     

Bright infrared quantum-dot light-emitting diodes through inter-dot spacing control

Infrared light-emitting diodes are currently fabricated from direct-gap semiconductors using epitaxy, which makes them expensive and difficult to integrate with other materials. Light-emitting diodes based on colloidal semiconductor quantum dots, on the other hand, can be solution-processed at low cost, and can be directly integrated with silicon. However, so far, exciton dissociation and recombination have not been well controlled in these devices, and this has limited their performance. Here, by tuning the distance between adjacent PbS quantum dots, we fabricate thin-film quantum-dot light-emitting diodes that operate at infrared wavelengths with radiances (6.4?W?sr(-1)?m(-2)) eight times higher and external quantum efficiencies (2.0%) two times higher than the highest values previously reported. The distance between adjacent dots is tuned over a range of 1.3?nm by varying the lengths of the linker molecules from three to eight CH(2) groups, which allows us to achieve the optimum balance between charge injection and radiative exciton recombination. The electroluminescent powers of the best devices are comparable to those produced by commercial InGaAsP light-emitting diodes. By varying the size of the quantum dots, we can tune the emission wavelengths between 800 and 1,850?nm.     

Activated Electron‐Transport Layers for Infrared Quantum Dot Optoelectronics

Photovoltaic (PV) materials such as perovskites and silicon are generally unabsorptive at wavelengths longer than 1100 nm, leaving a significant portion of the IR solar spectrum unharvested. Small‐bandgap colloidal quantum dots (CQDs) are a promising platform to offer tandem complementary IR PV solutions. Today, the best performing CQD PVs use zinc oxide (ZnO) as an electron‐transport layer. However, these electrodes require ultraviolet (UV)‐light activation to overcome the low carrier density of ZnO, precluding the realization of CQD tandem photovoltaics. Here, a new sol–gel UV‐free electrode based on Al/Cl hybrid doping of ZnO (CAZO) is developed. Al heterovalent doping provides a strong n‐type character while Cl surface passivation leads to a more favorable band alignment for electron extraction. CAZO CQD IR solar cell devices exhibit, at wavelengths beyond the Si bandgap, an external quantum efficiency of 73%, leading to an additional 0.92% IR power conversion efficiency without UV activation. Conventional ZnO devices, on the other hand, add fewer than 0.01 power points at these operating conditions.     

Solid‐State Carbon Dots with Red Fluorescence and Efficient Construction of Dual‐Fluorescence Morphologies

Stable solid‐state red fluorescence from organosilane‐functionalized carbon dots (CDs) with sizes around 3 nm is reported for the first time. Meanwhile, a novel method is also first reported for the efficient construction of dual‐fluorescence morphologies. The quantum yield of these solid‐state CDs and their aqueous solution is 9.60 and 50.7%, respectively. The fluorescence lifetime is 4.82 ns for solid‐state CDs, and 15.57 ns for their aqueous solution. These CDs are detailedly studied how they can exhibit obvious photoluminescence overcoming the self‐quenching in solid state. Luminescent materials are constructed with dual fluorescence based on as‐prepared single emissive CDs (red emission) and nonfluorescence media (starch, Al₂O₃, and RnOCH₃COONa), with the characteristic peaks located at nearly 440 and 600 nm. Tunable photoluminescence can be successfully achieved by tuning the mass ratio of CDs to solid matrix (such as starch). These constructed dual‐fluorescence CDs/starch composites can also be applied in white light‐emitting diodes with UV chips (395 nm), and oxygen sensing.     

Red, green and blue lasing enabled by single-exciton gain in colloidal quantum dot films

Colloidal quantum dots exhibit efficient photoluminescence with widely tunable bandgaps as a result of quantum confinement effects. Such quantum dots are emerging as an appealing complement to epitaxial semiconductor laser materials, which are ubiquitous and technologically mature, but unable to cover the full visible spectrum (red, green and blue; RGB). However, the requirement for high colloidal-quantum-dot packing density, and losses due to non-radiative multiexcitonic Auger recombination, have hindered the development of lasers based on colloidal quantum dots. Here, we engineer CdSe/ZnCdS core/shell colloidal quantum dots with aromatic ligands, which form densely packed films exhibiting optical gain across the visible spectrum with less than one exciton per colloidal quantum dot on average. This single-exciton gain allows the films to reach the threshold of amplified spontaneous emission at very low optical pump energy densities of 90?μJ?cm(-2), more than one order of magnitude better than previously reported values. We leverage the low-threshold gain of these nanocomposite films to produce the first colloidal-quantum-dot vertical-cavity surface-emitting lasers (CQD-VCSEL). Our results represent a significant step towards full-colour single-material lasers.     

Layer-by-layer assembly of multicolored semiconductor quantum dots towards efficient blue, green, red and full color optical films

Multicolored semiconductor quantum dots have shown great promise for construction of miniaturized light-emitting diodes with compact size, low weight and cost, and high luminescent efficiency. The unique size-dependent luminescent property of quantum dots offers the feasibility of constructing single-color or full-color output light-emitting diodes with one type of material. In this paper, we have demonstrated the facile fabrication of blue-, green-, red-?and full-color-emitting semiconductor quantum dot optical films via a layer-by-layer assembly technique. The optical films were constructed by alternative deposition of different colored quantum dots with a series of oppositely charged species, in particular, the new use of cationic starch on glass substrates. Semiconductor ZnSe quantum dots exhibiting blue emission were deposited for fabrication of blue-emitting optical films, while semiconductor CdTe quantum dots with green and red emission were utilized for construction of green-?and red-emitting optical films. The assembly of integrated blue, green and red semiconductor quantum dots resulted in full-color-emitting optical films. The luminescent optical films showed very bright emitting colors under UV irradiation, and displayed dense, smooth and efficient luminous features, showing brighter luminescence in comparison with their corresponding quantum dot aqueous colloid solutions. The assembled optical films provide the prospect of miniaturized light-emitting-diode applications.     

Continuous distribution of emission states from single CdSe/ZnS quantum dots

The photoluminescence dynamics of colloidal CdSe/ZnS/streptavidin quantum dots were studied using time-resolved single-molecule spectroscopy. Statistical tests of the photon-counting data suggested that the simple "on/off" discrete state model is inconsistent with experimental results. Instead, a continuous emission state distribution model was found to be more appropriate. Autocorrelation analysis of lifetime and intensity fluctuations showed a nonlinear correlation between them. These results were consistent with the model that charged quantum dots were also emissive, and that time-dependent charge migration gave rise to the observed photoluminescence dynamics.     

Detection of bioconjugated quantum dots passivated with different ligands for bio-applications

Bioconjugation of quantum dots has resulted in a significant increase in resolution of biological fluorescent labeling. This intrinsic property of quantum dots can be utilized for sensitive detection of target analytes with high sensitivity; including pathogenic bacteria and cancer monitoring. The quantum dots and quantum dot doped silica nanoparticles exhibit prominent emission peaks when excited at 400 nm but on conjugation to model rabbit antigoat antibodies exhibit diminished intensity of emission peak at 600 nm. It shows that photoluminescence intensity of conjugated quantum dots and quantum dot doped silica nanoparticles could permit the detection of bioconjugation. Samples of conjugated and unconjugated quantum dots and quantum dot doped silica nanoparticles were subjected to enzyme linked immunosorbent assay for further confirmation of bioconjugation. In the present study ligand exchange, bioconjugation, fluorescence detection of bioconjugated quantum dots and quantum dot doped silica nanoparticles and further confirmation of bioconjugation by enzyme linked immunosorbent assay has been described.     

Electronic excited states in bilayer graphene double quantum dots

We report tunneling spectroscopy experiments on a bilayer graphene double quantum dot device that can be tuned by all-graphene lateral gates. The diameter of the two quantum dots are around 50 nm and the constrictions acting as tunneling barriers are 30 nm in width. The double quantum dot features additional energies on the order of 20 meV. Charge stability diagrams allow us to study the tunable interdot coupling energy as well as the spectrum of the electronic excited states on a number of individual triple points over a large energy range. The obtained constant level spacing of 1.75 meV over a wide energy range is in good agreement with the expected single-particle energy spacing in bilayer graphene quantum dots. Finally, we investigate the evolution of the electronic excited states in a parallel magnetic field.     

Effect of solvent-induced structural modifications on optical properties of CdS nanoparticles

We have investigated the effects of solvent used during synthesis on structural and optical properties of CdS quantum dots. Different methods of synthesis for the production of CdS quantum dots are presented. These are: (a) wet chemical co-precipitation in non-aqueous medium (i.e. methanol); (b) wet chemical co-precipitation in aqueous medium (deionized water) and (c) solid state reaction. It is demonstrated that the use of methanol as solvent leads to a strong enhancement of PL intensity of CdS quantum dots for use in optoelectronic devices. These products were characterized by X-ray powder diffraction (XRD), high resolution transmission electron microscopy (HRTEM) and scanning electron microscopy (SEM). The change in bandgap with size-quantization was investigated by UV-VIS absorption spectroscopy. CdS nanocrystals prepared in non-aqueous medium have narrow size distribution than those prepared in aqueous medium and solid state reaction. Phase transformation of CdS nanocrystals from a cubic to hexagonal structure was observed in methanol solution. The formation of CdS/Cd(OH)₂ nanostructure was also confirmed using X-ray diffraction pattern. This suggests that the strong enhancement of the PL intensity may have originated from the remarkable reduction of non-radiative recombination process, due to surface defects of quantum dots. The red shift of the Raman peaks compared to that for bulk CdS may be attributed to optical phonon confinement.