Advance in wet chemistry enables the sophisticated design of nanocrystal quantum dots (QDs) and allows unprecedented color purity and brightness, promising their useful applications in a variety of light-emitting applications. A representative example is core/shell heterostructures, in which charge carriers are effectively decoupled from structural artifacts to generate photons efficiently. Despite the development of widely accepted synthetic protocols for Cd- or Pb-based QDs, the progress in heterostructuring environmentally benign QDs has been lagging behind, and so is the practical use of these QDs. Herein, we present a design principle for InP/ZnSe x S1–x heterostructured QDs. A principal design approach is the growth of uniformly thick inorganic shell consisting of a ZnSe x S1–x inner shell and a ZnS outermost shell that effectively confines electrons from spreading inward of QDs. Comprehensive studies across synthesis, spectroscopic analysis, and calculation uncover that the presence of Se near the InP emissive core enables a uniform shell growth to an extended thickness and the S-rich exterior shell ensures the decoupling of the electron wave function from the surface trap states. Engineering composition profile across multiple shells enables us to realize InP/thick-shell QDs meeting the requirements of light-emitting applications such as high photoluminescence quantum yield, narrow spectral bandwidth, and enhanced photochemical robustness. We capitalize on bright, robust, and color-pure InP/ZnSe x S1–x /ZnS QDs with a range of emission wavelength covering from cyan to red regions by exemplifying their use in the primary-color light-emitting diodes (peak external quantum efficiency of 3.78 and 3.92% for green- and red-emitting ones, respectively).
Establishing multi-colour patterning technology for colloidal quantum dots is critical for realising high-resolution displays based on the material. Here, we report a solution-based processing method to form patterns of quantum dots using a light-driven ligand crosslinker, ethane-1,2-diyl bis(4-azido-2,3,5,6-tetrafluorobenzoate). The crosslinker with two azide end groups can interlock the ligands of neighbouring quantum dots upon exposure to UV, yielding chemically robust quantum dot films. Exploiting the light-driven crosslinking process, different colour CdSe-based core-shell quantum dots can be photo-patterned; quantum dot patterns of red, green and blue primary colours with a sub-pixel size of 4 μm × 16 μm, corresponding to a resolution of >1400 pixels per inch, are demonstrated. The process is non-destructive, such that photoluminescence and electroluminescence characteristics of quantum dot films are preserved after crosslinking. We demonstrate that red crosslinked quantum dot light-emitting diodes exhibiting an external quantum efficiency as high as 14.6% can be obtained.
The potential profile and the energy level offset of core/shell heterostructured nanocrystals (h-NCs) determine the photophysical properties and the charge transport characteristics of h-NC solids. However, limited material choices for heavy metal-free III-V/II-VI h-NCs pose challenges in comprehensive control of the potential profile. Herein, we present an unprecedented approach to such control by steering dipole moments at the interface of III-V/II-VI h-NCs. The controllable heterovalency at the interface is responsible for interfacial dipole moments that result in the vacuum-level shift, providing an additional knob for the control of optical and electrical characteristics of h-NCs. We capitalize on the atomic precision with which to synthesize h-NCs by correlating interfacial dipole moments to photochemical stability and optoelectronic performance of resulting h-NCs.
Busulfan, a bifunctional alkylating agent, has been used as a conditioning regimen prior to allogeneic hematopoietic stem cell transplantation (HSCT). The aim of this study was to derive a novel once-daily intravenous (IV) busulfan dosing nomogram for pediatric patients undergoing HSCT using a population pharmacokinetic (PK) model. A population PK analysis was performed using 2183 busulfan concentrations in 137 pediatric patients (age: 0.6-22.2 years), who received IV busulfan once-daily for 4 days before undergoing HSCT. Based on the final population PK model, an optimal once-daily IV busulfan dosing nomogram was derived. The percentage of simulated patients achieving the daily target area under the concentration-time curve (AUC) by the new nomogram was compared with that by other busulfan dosing regimens including the FDA regimen, the EMA regimen, and the empirical once-daily regimen without therapeutic drug monitoring (TDM). A one-compartment open linear PK model incorporating patient's body surface area, age, dosing day, and aspartate aminotransferase as a significant covariate adequately described the concentration-time profiles of busulfan. An optimal dosing nomogram based on the PK model performed significantly better than the other dosing regimens, resulting in >60% of patients achieving the target AUC while the percentage of patients exceeding the toxic AUC level was kept <25% during the entire treatment period. A novel once-daily busulfan dosing nomogram for pediatric patients undergoing HSCT is useful for clinicians, particularly in a setting where TDM service is not readily available or to optimize the dose on day 1.
The charge injection imbalance into the quantum dot (QD) emissive layer of QD-based light-emitting diodes (QD-LEDs) is an unresolved issue that is detrimental to the efficiency and operation stability of devices. Herein, an integrated approach to harmonize the charge injection rates for bright and stable QD-LEDs is proposed. Specifically, the electronic characteristics of the hole transport layer (HTL) is delicately designed in order to facilitate the hole injection from the HTL into QDs and confine the electron overflow toward the HTL. The well-defined exciton recombination zone by the engineered QDs and HTL results in high performance with a peak luminance exceeding 410 000 cd/m 2 , suppressed efficiency roll-off characteristics (ΔEQE < 5% between 200 and 200 000 cd/m 2 ), and prolonged operational stability. The electric and optoelectronic analyses reveal the charge carrier injection mechanism at the interface between the HTL and QDs and provides the design principle of QD heterostructures and charge transport layers for high-performance QD-LEDs.
Colloidal quantum dots (QDs) stand at the forefront of a variety of photonic applications given their narrow spectral bandwidth and near-unity luminescence e ciency. Integrating desired forms of QD lms into photonic systems without compromising their optical or transport characteristics is the key to bridging the gap between expectations and outcomes. Here, we devise a dual-ligand passivation system comprising photocrosslinkable ligands and dispersing ligands to enable QDs to be universally compatible with solution-based patterning techniques. The successful control on the structure of both ligands allows multiscale, direct patterning of the dual-ligand QDs on various substrates via commercialized photolithography (i-line) or inkjet printing systems without compromising the optical properties of QDs or the optoelectronic performances of the devices implementing them. Our approach offers a versatile way of creating various structures of luminescent QDs in a cost-effective and non-destructive manner, and thus enables the implementation of QDs in a range of photonic applications. MainColloidal quantum dots (QDs) are promising materials for use in next-generation light sources due to their wide-ranging bandgap tunability, narrow spectral bandwidths, and near-unity luminescence quantum yields (QY) [1][2][3][4][5] . Together with the capability of cost-effective solution processing, QDs have become the key light-emissive materials for information displays 3,5−7 . The patterned QD down-conversion layer on blue light-emitting diodes (LEDs) renders high-color reproduction and ultra-high image quality in full-color displays 8,9 . Likewise, a laterally patterned array consisting of red, green, and blue (RGB) QD-LEDs, in which QDs convert electrically pumped charge carriers into photons, allows for excellent color gamut and brightness as well as light-weight, thin, and exible form factors [10][11][12][13] , which are suited for wearable neareye displays for virtual reality (VR) and augmented reality (AR) devices. For these "mixed-reality" applications, the QD deposition process should enable the patterning of RGB QDs (or RG QDs along with the bank) into a few micrometer sub-pixels over a large area with high-precision and high-delity 14,15 . At the same time, the process should not disrupt the optical and transport characteristics of QDs and adjacent functional layers. Moreover, from a practical standpoint, it poses great bene t if one can use equipment that are already deployed in display device manufacturing steps for the patterning process.
Quasi-type II heterostructured nanocrystals (NCs) have been of particular interest due to their great potential for controlling the interplay of charge carriers. However, the lack of material choices for quasi-type II NCs restricts the accessible emission wavelength from red to near-infrared (NIR), which hinders their use in light-emitting applications that demand a wide range of visible colors. Herein, we demonstrate a new class of quasi-type II nanoemitters formulated in ZnSe/ZnSe1-XTeX/ZnSe seed/spherical quantum well/shell heterostructures (SQWs) whose emission wavelength ranges from blue to orange. In a given geometry, ZnSe1-XTeX emissive layers grown between the ZnSe seed and the shell layer are strained to fit into the surrounding media, and thus, the lattice mismatch between ZnSe1-XTeX and ZnSe is effectively alleviated. In addition, composition of the ZnSe1-XTeX emissive layer and the dimension of the ZnSe shell layer are engineered to tailor the distribution and energy of electron and hole wave functions. Benefitting from the capabilities to tune the charge carriers on demand and to form defect-free heterojunctions, ZnSe/ZnSe1-XTeX/ZnSe/ZnS NCs show near-unity photoluminescence quantum yield (PL QY>90%) in a broad range of emission wavelengths (peak PL from 450 nm to 600 nm). Finally, we exemplify dichromatic white NC-based light-emitting diodes (NC-LEDs) employing the mixed layer of blue- and yellow-emitting ZnSe/ZnSe1-XTeX/ZnSe/ZnS SQW NCs.
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