Fabrication and characterization of red-emitting electroluminescent devices based on thiol-stabilized semiconductor nanocrystals

Thiol-capped CdTe nanocrystals were used to fabricate light-emitting diodes, consisting of an emissive nanocrystal multilayer deposited via layer-by-layer, sandwiched between indium-tin-oxide and aluminum electrodes. The emissive and electrical properties of devices with different numbers of nanocrystal layers were studied. The improved structural homogeneity of the nanocrystal multilayer allowed for stable and repeatable current- and electroluminescence-voltage characteristics. These indicate that both current and electroluminescence are electric-field dependent. Devices were operated under ambient conditions and a clear red-light was detected. The best-performing device shows a peak external efficiency of 0.51% and was measured at 0.35mA/cm2 and 3.3V

Cathodic and Anodic Material Diffusion in Polymer/Semiconductor-Nanocrystal Composite Devices

In the present day, the information technologies and telecommunications sector continually increase their demand for low cost, low power consumption, high performance electroluminescent devices for display applications. Furthermore, general lighting applications, such as white light and large array colour displays, would also benefit from an increase in the overall efficiency. Several technologies are being investigated to fulfill these needs, such as organic light emitting diodes (OLED), polymeric light emitting diodes (PLED) and field effect emission devices. A new and promising technology is light emitting devices (LEDs) based on nanostructured materials. With organic LEDs (OLEDs) already making an impact on the market in an increasingly large number of applications, hybrid technologies based on organic/inorganic nano-composites are a potential the next step. The incorporation of highefficiency fluorescent semiconductor nanoparticles has been shown to have a beneficial effect on device performance, [1] modify the colour output from the device 2 and provide a simplified route to generation of LED type devices. [3

Excitonic improvement of colloidal nanocrystals in salt powder matrix for quality lighting and color enrichment

Here we report excitonic improvement in color-converting colloidal nanocrystal powders enabled by co-integrating nonpolar green-and red-emitting nanocrystal energy transfer pairs into a single LiCl salt matrix. This leads to nonradiative energy transfer (NRET) between the cointegrated nanocrystals in the host matrix. Here we systematically studied the resulting NRET process by varying donor and acceptor concentrations in the powders. We observed that NRET is a strong function of both of the nanocrystal concentrations and that NRET efficiency increases with increasing acceptor concentration. Nevertheless, with increasing donor concentration in the powders, NRET efficiency was found to first increase ( up to a maximum level of 53.9%) but then to decrease. As a device demonstrator, we employed these NRET-improved nanocrystal powders as color-converters on blue light-emitting diodes ( LEDs), with the resulting hybrid LED exhibiting a luminous efficiency > 70 lm/Welect. The proposed excitonic nanocrystal powders potentially hold great promise for quality lighting and color enrichment applications. (C) 2015 Optical Society of Americ

Stable and efficient colour enrichment powders of nonpolar nanocrystals in LiCl

In this work, we propose and develop the inorganic salt encapsulation of semiconductor nanocrystal (NC) dispersion in a nonpolar phase to make a highly stable and highly efficient colour converting powder for colour enrichment in light-emitting diode backlighting. Here the wrapping of the as-synthesized green-emitting CdSe/CdZnSeS/ZnS nanocrystals into a salt matrix without ligand exchange is uniquely enabled by using a LiCl ionic host dissolved in tetrahydrofuran (THF), which simultaneously disperses these nonpolar nanocrystals. We studied the emission stability of the solid films prepared using NCs with and without LiCl encapsulation on blue LEDs driven at high current levels. The encapsulated NC powder in epoxy preserved 95.5% of the initial emission intensity and stabilized at this level while the emission intensity of NCs without salt encapsulation continuously decreased to 34.7% of its initial value after 96 h of operation. In addition, we investigated the effect of ionic salt encapsulation on the quantum efficiency of nonpolar NCs and found the quantum efficiency of the NCs-inLiCl to be 75.1% while that of the NCs in dispersion was 73.0% and that in a film without LiCl encapsulation was 67.9%. We believe that such ionic salt encapsulated powders of nonpolar NCs presented here will find ubiquitous use for colour enrichment in display backlighting

Precise Engineering of Nanocrystal Shells via Colloidal Atomic Layer Deposition

We present a general strategy for a facile synthesis of complex multifunctional nanoscale materials via colloidal atomic layer deposition (c-ALD). The c-ALD technique is based on self-limiting half-reactions of ionic precursors on the surface of a nanocrystal (NC) occurring at room temperature. Using this technique, uniform layers of CdS and ZnS semiconductor shells were epitaxially grown on CdSe semiconductor cores with different shell combinations, leading to the precise control of the optical properties of these heterostructures. All core-shell multicomponent nanoparticles preserve narrow size distributions, phase crystallinity, and shape homogeneity of the initial NCs. Furthermore, we attempted to extend the toolbox of the c-ALD to combine materials with intrinsically different properties, such as Au/CdS core/shell structures with substantial lattice mismatch. The results presented in this work demonstrate great opportunities for creating functional materials with programmable properties for electronics and optoelectronics

Modification of emission of CdTe nanocrystals by the local field of Langmuir-Blodgett colloidal photonic crystals

A light source on the surface of a slab of 2+1-dimensional photonic crystal has been prepared by the Langmuir-Blodgett deposition of a colloidal crystal on top of a thin film containing CdTe nanocrystals. The directional enhancement of the light emission intensity in the spectral range of the photonic bandgap has been revealed through the comparative examination of the angle-resolved transmission, diffraction, and photoluminescence spectra of the prepared structures. Changes in the emission spectrum have been tentatively explained in terms of the acceleration of the radiative recombination due to the increase in the local field strength at photonic bandgap resonance and changes in the emission diagram-as arising from the wavelength dependence of the topology of the local field pattern

Self-Supported Three-Dimensional Quantum Dot Aerogels as a Promising Photocatalyst for CO2 Reduction

With the merits of quantum dots (QDs) (e.g., high molar extinction coefficient, strong visible light absorption, large specific surface area, and abundant functional surface active sites) and aerogels (e.g., self-supported architectures, porous network), semiconductor QD aerogels show great prospect in photocatalytic applications. However, typical gelation methods rely on oxidative treatments of QDs. Moreover, the remaining organic ligands (e.g., mercaptoacids) are still present on the surface of gels. Both these factors inhibit the activity of such photocatalysts, hampering their widespread use. Herein, we present a facile 3D assembly of II–VI semiconductor QDs capped with inorganic (NH4)2S ligands into aerogels using H2O as a dispersion solvent. Without any sacrificial agents, the resulting CdSe QD aerogels achieve a high CO generation rate of 15 μmol g–1 h–1, which is 12-fold higher than that of pristine-aggregated QD powders. Our work not only provides a facile strategy to fabricate QD aerogels but also offers a platform for designing advanced aerogel-based photocatalysts

A spray-coating process for highly conductive silver nanowire networks as the transparent top-electrode for small molecule organic photovoltaics

We present a novel top-electrode spray-coating process for the solution-based deposition of silver nanowires (AgNWs) onto vacuum-processed small molecule organic electronic solar cells. The process is compatible with organic light emitting diodes (OLEDs) and organic light emitting thin film transistors (OLETs) as well. By modifying commonly synthesized AgNWs with a perfluorinated methacrylate, we are able to disperse these wires in a highly fluorinated solvent. This solvent does not dissolve most organic materials, enabling a top spray-coating process for sensitive small molecule and polymer-based devices. The optimized preparation of the novel AgNW dispersion and spray-coating at only 30 °C leads to high performance electrodes directly after the deposition, exhibiting a sheet resistance of 10.0 Ω □−1 at 87.4% transparency (80.0% with substrate). By spraying our novel AgNW dispersion in air onto the vacuum-processed organic p-i-n type solar cells, we obtain working solar cells with a power conversion efficiency (PCE) of 1.23%, compared to the air exposed reference devices employing thermally evaporated thin metal layers as the top-electrode

Resonance energy transfer in self-organized organic/inorganic dendrite structures

Hybrid materials formed by semiconductor quantum dots and J-aggregates of cyanine dyes provide a unique combination of enhanced absorption in inorganic constituents with large oscillator strength and extremely narrow exciton bands of the organic component. The optical properties of dendrite structures with fractal dimension 1.7–1.8, formed from J-aggregates integrated with CdTe quantum dots (QDs), have been investigated by photoluminescence spectroscopy and fluorescence lifetime imaging microscopy. Our results demonstrate that (i)J-aggregates are coupled to QDs by F¨orster-type resonant energy transfer and (ii) there are energy fluxes from the periphery to the centre of the structure, where the QD density is higher than in the periphery of the dendrite. Such an anisotropic energy transport can be only observed when dendrites are formed from QDs integrated with J-aggregates. These QD/ J-aggregate hybrid systems can have applications in light harvesting systems and optical sensors with extended absorption spectra.Fundação para a Ciência e a Tecnologia (FCT

Absolute photoluminescence quantum yields of IR26 and IR-emissive Cd₁₋ₓHgₓTe and PbS quantum dots: method- and material-inherent challenges

Bright emitters with photoluminescence in the spectral region of 800–1600 nm are increasingly important as optical reporters for molecular imaging, sensing, and telecommunication and as active components in electrooptical and photovoltaic devices. Their rational design is directly linked to suitable methods for the characterization of their signal-relevant properties, especially their photoluminescence quantum yield (Φf ). Aiming at the development of bright semiconductor nanocrystals with emission >1000 nm, we designed a new NIR/IR integrating sphere setup for the wavelength region of 600–1600 nm. We assessed the performance of this setup by acquiring the corrected emission spectra and Φf of the organic dyes |trybe, IR140, and IR26 and several infrared (IR)-emissive Cd₁₋ₓHgₓTe and PbS semiconductor nanocrystals and comparing them to data obtained with two independently calibrated fluorescence instruments absolutely or relative to previously evaluated reference dyes. Our results highlight special challenges of photoluminescence studies in the IR ranging from solvent absorption to the lack of spectral and intensity standards together with quantum dot-specific challenges like photobrightening and photodarkening and the size-dependent air stability and photostability of differently sized oleate-capped PbS colloids. These effects can be representative of lead chalcogenides. Moreover, we redetermined the Φf of IR26, the most frequently used IR reference dye, to 1.1 × 10⁻³ in 1,2-dichloroethane DCE with a thorough sample reabsorption and solvent absorption correction. Our results indicate the need for a critical reevaluation of Φf values of IR-emissive nanomaterials and offer guidelines for improved Φf measurements