Jiwoong Yang

Wearable red–green–blue quantum dot light-emitting diode array using high-resolution intaglio transfer printing

Deformable full-colour light-emitting diodes with ultrafine pixels are essential for wearable electronics, which requires the conformal integration on curvilinear surface as well as retina-like high-definition displays. However, there are remaining challenges in terms of polychromatic configuration, electroluminescence efficiency and/or multidirectional deformability. Here we present ultra-thin, wearable colloidal quantum dot light-emitting diode arrays utilizing the intaglio transfer printing technique, which allows the alignment of red–green–blue pixels with high resolutions up to 2,460 pixels per inch. This technique is readily scalable and adaptable for low-voltage-driven pixelated white quantum dot light-emitting diodes and electronic tattoos, showing the best electroluminescence performance (14,000 cd m−2 at 7 V) among the wearable light-emitting diodes reported up to date. The device performance is stable on flat, curved and convoluted surfaces under mechanical deformations such as bending, crumpling and wrinkling. These deformable device arrays highlight new possibilities for integrating high-definition full-colour displays in wearable electronics.

Designed Assembly and Integration of Colloidal Nanocrystals for Device Applications.

Colloidal nanocrystals have been intensively studied over the past three decades due to their unique properties that originate, in large part, from their nanometer-scale sizes. For applications in electronic and optoelectronic devices, colloidal nanoparticles are generally employed as assembled nanocrystal solids, rather than as individual particles. Consequently, tailoring 2D patterns as well as 3D architectures of assembled nanocrystals is critical for their various applications to micro- and nanoscale devices. Here, recent advances in the designed assembly, film fabrication, and printing/integration methods for colloidal nanocrystals are presented. The advantages and drawbacks of these methods are compared, and various device applications of assembled/integrated colloidal nanocrystal solids are discussed.

Highly Efficient Copper–Indium–Selenide Quantum Dot Solar Cells: Suppression of Carrier Recombination by Controlled ZnS Overlayers

Copper-indium-selenide (CISe) quantum dots (QDs) are a promising alternative to the toxic cadmium- and lead-chalcogenide QDs generally used in photovoltaics due to their low toxicity, narrow band gap, and high absorption coefficient. Here, we demonstrate that the photovoltaic performance of CISe QD-sensitized solar cells (QDSCs) can be greatly enhanced simply by optimizing the thickness of ZnS overlayers on the QD-sensitized TiO2 electrodes. By roughly doubling the thickness of the overlayers compared to the conventional one, conversion efficiency is enhanced by about 40%. Impedance studies reveal that the thick ZnS overlayers do not affect the energetic characteristics of the photoanode, yet enhance the kinetic characteristics, leading to more efficient photovoltaic performance. In particular, both interfacial electron recombination with the electrolyte and nonradiative recombination associated with QDs are significantly reduced. As a result, our best cell yields a conversion efficiency of 8.10% under standard solar illumination, a record high for heavy metal-free QD solar cells to date.

Dimension-Controlled Synthesis of CdS Nanocrystals: From 0D Quantum Dots to 2D Nanoplates

The dimension-controlled synthesis of CdS nanocrystals in the strong quantum confinement regime is reported. Zero-, one-, and two-dimensional CdS nanocrystals are selectively synthesized via low-temperature reactions using alkylamines as surface-capping ligands. The shape of the nanocrystals is controlled systematically by using different amines and reaction conditions. The 2D nanoplates have a uniform thickness as low as 1.2 nm. Furthermore, their optical absorption and emission spectra show very narrow peaks indicating extremely uniform thickness. It is demonstrated that 2D nanoplates are generated by 2D assembly of CdS magic-sized clusters formed at the nucleation stage, and subsequent attachment of the clusters. The stability of magic-sized clusters in amine solvent strongly influences the final shapes of the nanocrystals. The thickness of the nanoplates increases in a stepwise manner while retaining their uniformity, similar to the growth behavior of inorganic clusters. The 2D CdS nanoplates are a new type of quantum well with novel nanoscale properties in the strong quantum confinement regime.

Colloidal Synthesis of Uniform‐Sized Molybdenum Disulfide Nanosheets for Wafer‐Scale Flexible Nonvolatile Memory

Large-scale colloidal synthesis and integration of uniform-sized molybdenum disulfide (MoS2 ) nanosheets for a flexible resistive random access memory (RRAM) array are presented. RRAM using MoS2 nanosheets shows a ≈10 000 times higher on/off ratio than that based on exfoliated MoS2 . The good uniformity of the MoS2 nanosheets allows wafer-scale system integration of the RRAM array with pressure sensors and quantum-dot light-emitting diodes.

Route to the Smallest Doped Semiconductor: Mn2+-Doped (CdSe)13 Clusters

Doping semiconductor nanocrystals with magnetic transition-metal ions has attracted fundamental interest to obtain a nanoscale dilute magnetic semiconductor, which has unique spin exchange interaction between magnetic spin and exciton. So far, the study on the doped semiconductor NCs has usually been conducted with NCs with larger than 2 nm because of synthetic challenges. Herein, we report the synthesis and characterization of Mn(2+)-doped (CdSe)13 clusters, the smallest doped semiconductors. In this study, single-sized doped clusters are produced in large scale. Despite their small size, these clusters have semiconductor band structure instead of that of molecules. Surprisingly, the clusters show multiple excitonic transitions with different magneto-optical activities, which can be attributed to the fine structure splitting. Magneto-optically active states exhibit giant Zeeman splittings up to elevated temperatures (128 K) with large g-factors of 81(±8) at 4 K. Our results present a new synthetic method for doped clusters and facilitate the understanding of doped semiconductor at the boundary of molecules and quantum nanostructure.

Quantum Confinement-Controlled Exchange Coupling in Manganese(II)-Doped CdSe Two-Dimensional Quantum Well Nanoribbons

The impact of quantum confinement on the exchange interaction between charge carriers and magnetic dopants in semiconductor nanomaterials has been controversially discussed for more than a decade. We developed manganese-doped CdSe quantum well nanoribbons with a strong quantum confinement perpendicular to the c-axis, showing distinct heavy hole and light hole resonances up to 300 K. This allows a separate study of the s-d and the p-d exchange interactions all the way up to room temperature. Taking into account the optical selection rules and the statistical distribution of the nanoribbons orientation on the substrate, a remarkable change in particular of the s-d exchange constant with respect to bulk is indicated. Room-temperature studies revealed an unusually high effective g-factor up to ~13 encouraging the implementation of the DMS quantum well nanoribbons for (room temperature) spintronic applications.

Ultrathin Quantum Dot Display Integrated with Wearable Electronics

An ultrathin skin-attachable display is a critical component for an information output port in next-generation wearable electronics. In this regard, quantum dot (QD) light-emitting diodes (QLEDs) offer unique and attractive characteristics for future displays, including high color purity with narrow bandwidths, high electroluminescence (EL) brightness at low operating voltages, and easy processability. Here, ultrathin QLED displays that utilize a passive matrix to address individual pixels are reported. The ultrathin thickness (≈5.5 µm) of the QLED display enables its conformal contact with the wearers skin and prevents its failure under vigorous mechanical deformation. QDs with relatively thick shells are employed to improve EL characteristics (brightness up to 44 719 cd m-2 at 9 V, which is the record highest among wearable LEDs reported to date) by suppressing the nonradiative recombination. Various patterns, including letters, numbers, and symbols can be successfully visualized on the skin-mounted QLED display. Furthermore, the combination of the ultrathin QLED display with flexible driving circuits and wearable sensors results in a fully integrated QLED display that can directly show sensor data.

Digital Doping in Magic-Sized CdSe Clusters

Magic-sized semiconductor clusters represent an exciting class of materials located at the boundary between quantum dots and molecules. It is expected that replacing single atoms of the host crystal with individual dopants in a one-by-one fashion can lead to unique modifications of the material properties. Here, we demonstrate the dependence of the magneto-optical response of (CdSe)13 clusters on the discrete number of Mn(2+) ion dopants. Using time-of-flight mass spectrometry, we are able to distinguish undoped, monodoped, and bidoped cluster species, allowing for an extraction of the relative amount of each species for a specific average doping concentration. A giant magneto-optical response is observed up to room temperature with clear evidence that exclusively monodoped clusters are magneto-optically active, whereas the Mn(2+) ions in bidoped clusters couple antiferromagnetically and are magneto-optically passive. Mn(2+)-doped clusters therefore represent a system where magneto-optical functionality is caused by solitary dopants, which might be beneficial for future solotronic applications.

Sulfur‐Modified Graphitic Carbon Nitride Nanostructures as an Efficient Electrocatalyst for Water Oxidation

There is an urgent need to develop metal-free, low cost, durable, and highly efficient catalysts for industrially important oxygen evolution reactions. Inspired by natural geodes, unique melamine nanogeodes are successfully synthesized using hydrothermal process. Sulfur-modified graphitic carbon nitride (S-modified g-CN x ) electrocatalysts are obtained by annealing these melamine nanogeodes in situ with sulfur. The sulfur modification in the g-CN x structure leads to excellent oxygen evolution reaction activity by lowering the overpotential. Compared with the previously reported nonmetallic systems and well-established metallic catalysts, the S-modified g-CN x nanostructures show superior performance, requiring a lower overpotential (290 mV) to achieve a current density of 10 mA cm-2 and a Tafel slope of 120 mV dec-1 with long-term durability of 91.2% retention for 18 h. These inexpensive, environmentally friendly, and easy-to-synthesize catalysts with extraordinary performance will have a high impact in the field of oxygen evolution reaction electrocatalysis.