Adjusting Microscale to Atomic-Scale Structural Order in PbS Nanocrystal Superlattice for Enhanced Photodetector Performance.

An investigation is presented into the effect of the long-range order on the optoelectronic properties of PbS quantum dot (QD) superlattices, which form mesocrystals, for potential use in photodetector applications. By self-assembly of QD nanocrystals on an Si/SiOx substrate, a highly ordered and densely packed PbS QD superlattice with a microscale size is obtained. The results demonstrate that annealing treatment induces mesocrystalline superlattices with preferred growth orientation, achieved by dislodging ligands. The improved orientation and electronic coupling of the mesocrystalline superlattices exhibit superior photodetector performance compared to disordered QD structures and closely packed superlattices. This improved performance is attributed to atomic alignment between QDs, leading to enhanced electronic coupling. The findings suggest that these mesocrystalline superlattices have promising potential for the next generation of QD optoelectronic devices.

Wide field-of-view light-field displays based on thin-encapsulated self-emissive displays.

A wide field of view (FOV) is required to improve the user experience in mobile applications of light-field displays (LFDs). However, the FOV of liquid-crystal-display-based LFDs is narrow owing to the thick gap between the light-direction-control element and the pixel plane. The thin-encapsulated self-emissive displays, such as organic light-emitting diodes (OLEDs), are beneficial for widening the FOV without losing spatial resolution. With OLEDs, a 72-degree FOV, 12-view, 166-ppi LFD with smooth motion parallax is demonstrated. A moiré-free parallax barrier of arctan (1/4) slant angle is used to reconcile the triangular sub-pixel pattern of OLEDs, and further doubles the spatial resolution by aligning sub-pixels into a single column, instead of the conventional two columns. The effects of crosstalk due to the wide slits on the three-dimensional image quality are analyzed.

Ultra-bright green InGaN micro-LEDs with brightness over 10M nits.

An investigation of electrical and optical properties of InGaN micro-scale light-emitting diodes (micro-LEDs) emitting at ∼530 nm is carried out, with sizes of 80, 150, and 200 µm. The ITO as a current spreading layer (CSL) provides excellent device performance. Over 10% external quantum efficiency (EQE) and wall-plug efficiency (WPE), and ultra-high brightness (> 10M nits) green micro-LEDs are realized. In addition, it is observed that better current spreading in smaller devices results in higher EQE and brightness. Superior green micro-LEDs can provide an essential guarantee for a variety of applications.

Exploring superlattice DBR effect on a micro-LED as an electron blocking layer.

The role of a superlattice distributed Bragg reflector (SL DBR) as the p-type electron blocking layer (EBL) in a GaN micro-light-emitting diode (micro-LED) is numerically investigated to improve wall-plug efficiency (WPE). The DBR consists of AlGaN/GaN superlattice (high refractive index layer) and GaN (low refractive index layer). It is observed that the reflectivity of the p-region and light extraction efficiency (LEE) increase with the number of DBR pairs. The AlGaN/GaN superlattice EBL is well known to reduce the polarization effect and to promote hole injection. Thus, the superlattice DBR structure shows a balanced carrier injection and results in a higher internal quantum efficiency (IQE). In addition, due to the high refractive-index layer replaced by the superlattice, the conductive DBR results in a lower operation voltage. As a result, WPE is improved by 22.9% compared to the identical device with the incorporation of a conventional p-type EBL.

Dual Role of Quantum Dots as Color Conversion Layer and Suppression of Input Light for Full-Color Micro-LED Displays.

In micro-light-emitting diode (micro-LED) displays with color-conversion layers, a facile and efficient technology getting rid of the use of the color filters leads to a big technical leap in cost-effective fabrication. In this study, it is demonstrated that quantum dot (QD) color conversion layers can significantly suppress residual blue excitation light because of the high extinction coefficients of QDs, ∼0.1% transmittance of blue light for green and red core/shell CdSe/ZnS QD film with thickness of less than 17 µm, and produce green and red colors. Incorporation of TiO2 nanoparticles into QD solutions enhances more than 10% of the luminous intensity by the scattering effect. It is found that the suppression of QD reabsorption is essential to achieve a high color-conversion efficiency. Our results provide a clear path to a cost-effective fabrication of QD conversion layer micro-LED displays over the full range of their applications.

Micro-light-emitting diodes with quantum dots in display technology.

Micro-light-emitting diodes (µ-LEDs) are regarded as the cornerstone of next-generation display technology to meet the personalised demands of advanced applications, such as mobile phones, wearable watches, virtual/augmented reality, micro-projectors and ultrahigh-definition TVs. However, as the LED chip size shrinks to below 20 µm, conventional phosphor colour conversion cannot present sufficient luminance and yield to support high-resolution displays due to the low absorption cross-section. The emergence of quantum dot (QD) materials is expected to fill this gap due to their remarkable photoluminescence, narrow bandwidth emission, colour tuneability, high quantum yield and nanoscale size, providing a powerful full-colour solution for µ-LED displays. Here, we comprehensively review the latest progress concerning the implementation of µ-LEDs and QDs in display technology, including µ-LED design and fabrication, large-scale µ-LED transfer and QD full-colour strategy. Outlooks on QD stability, patterning and deposition and challenges of µ-LED displays are also provided. Finally, we discuss the advanced applications of QD-based µ-LED displays, showing the bright future of this technology.

Single molecule and single cell epigenomics.

Dynamically regulated changes in chromatin states are vital for normal development and can produce disease when they go awry. Accordingly, much effort has been devoted to characterizing these states under normal and pathological conditions. Chromatin immunoprecipitation followed by sequencing (ChIP-seq) is the most widely used method to characterize where in the genome transcription factors, modified histones, modified nucleotides and chromatin binding proteins are found; bisulfite sequencing (BS-seq) and its variants are commonly used to characterize the locations of DNA modifications. Though very powerful, these methods are not without limitations. Notably, they are best at characterizing one chromatin feature at a time, yet chromatin features arise and function in combination. Investigators commonly superimpose separate ChIP-seq or BS-seq datasets, and then infer where chromatin features are found together. While these inferences might be correct, they can be misleading when the chromatin source has distinct cell types, or when a given cell type exhibits any cell to cell variation in chromatin state. These ambiguities can be eliminated by robust methods that directly characterize the existence and genomic locations of combinations of chromatin features in very small inputs of cells or ideally, single cells. Here we review single molecule epigenomic methods under development to overcome these limitations, the technical challenges associated with single molecule methods and their potential application to single cells.

Heterojunction PbS nanocrystal solar cells with oxide charge-transport layers.

Oxides are commonly employed as electron-transport layers in optoelectronic devices based on semiconductor nanocrystals, but are relatively rare as hole-transport layers. We report studies of NiO hole-transport layers in PbS nanocrystal photovoltaic structures. Transient fluorescence experiments are used to verify the relevant energy levels for hole transfer. On the basis of these results, planar heterojunction devices with ZnO as the photoanode and NiO as the photocathode were fabricated and characterized. Solution-processed devices were used to systematically study the dependence on nanocrystal size and achieve conversion efficiency as high as 2.5%. Optical modeling indicates that optimum performance should be obtained with thinner oxide layers than can be produced reliably by solution casting. Room-temperature sputtering allows deposition of oxide layers as thin as 10 nm, which enables optimization of device performance with respect to the thickness of the charge-transport layers. The best devices achieve an open-circuit voltage of 0.72 V and efficiency of 5.3% while eliminating most organic material from the structure and being compatible with tandem structures.

A generic method for rational scalable synthesis of monodisperse metal sulfide nanocrystals.

A rational synthetic method is developed to produce monodisperse metal sulfide nanocrystals (NCs) in organic nonpolar solutions by using (NH(4))(2)S as a sulfide precursor. (NH(4))(2)S is stabilized in an organic primary amine solution and exhibits high reactivity toward metal complexes. This novel technique exhibits wide applicability for organic phase metal sulfide NC synthesis: a large variety of monodisperse NCs have been synthesized, including Cu(2)S, CdS, SnS, ZnS, MnS, Ag(2)S, and Bi(2)S(3). The stoichiometric reactions between (NH(4))(2)S and metal salts afford high conversion yields, and large-scale production of monodisperse NCs (more than 30 g) can be synthesized in a single reaction. The high reactivity of (NH(4))(2)S enables low temperature (<100 °C) syntheses, and the air-stable materials (such as CdS NCs) can be produced in air. Moreover, this low-temperature technique can be used to produce small size NCs which are difficult to be synthesized by the conventional high temperature methods, such as sub-5 nm Ag(2)S and Bi(2)S(3) quantum dots.

Exciton relaxation in PbSe nanorods.

Measurements of the picosecond-time-scale dynamics of photoexcited electrons in PbSe nanorods are reported. The intraband (1Π â†’ 1Σ) relaxation occurs with a time constant of ~500 fs, which corresponds to a fast energy-relaxation rate of ~0.6 eV/ps. The biexciton lifetime in PbSe nanorods is significantly (3-4 times) longer than the lifetime of PbSe quantum dots with the same energy gap, roughly as expected considering the increased volume. The multiexciton lifetimes of PbSe nanorods scale as expected for a bimolecular recombination mechanism. Implications of the observed relaxations will be discussed.

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.

Far-infrared absorption of PbSe nanorods.

Measurements of the far-infrared absorption spectra of PbSe nanocrystals and nanorods are presented. As the aspect ratio of the nanorods increases, the Fröhlich sphere resonance splits into two peaks. We analyze this splitting with a classical electrostatic model, which is based on the dielectric function of bulk PbSe but without any free-carrier contribution. Good agreement between the measured and calculated spectra indicates that resonances in the local field factors underlie the measured spectra.

Control of electron transfer from lead-salt nanocrystals to TiO2.

The roles of solvent reorganization energy and electronic coupling strength on the transfer of photoexcited electrons from PbS nanocrystals to TiO(2) nanoparticles are investigated. We find that the electron transfer depends only weakly on the solvent, in contrast to the strong dependence in the nanocrystal-molecule system. This is ascribed to the larger size of the acceptor in this system, and is accounted for by Marcus theory. The electronic coupling of the PbS and TiO(2) is varied by changing the length, aliphatic and aromatic structure, and anchor groups of the linker molecules. Shorter linker molecules consistently lead to faster electron transfer. Surprisingly, linker molecules of the same length but distinct chemical structures yield similar electron transfer rates. In contrast, the electron transfer rate can vary dramatically with different anchor groups.

Photogenerated exciton dissociation in highly coupled lead salt nanocrystal assemblies.

Internanocrystal coupling induced excitons dissociation in lead salt nanocrystal assemblies is investigated. By combining transient photoluminescence spectroscopy, grazing incidence small-angle X-ray scattering, and time-resolved electric force microscopy, we show that excitons can dissociate, without the aid of an external bias or chemical potential gradient, via tunneling through a potential barrier when the coupling energy is comparable to the exciton binding energy. Our results have important implications for the design of nanocrystal-based optoelectronic devices.

Role of solvent dielectric properties on charge transfer from PbS nanocrystals to molecules.

Transfer of photoexcited charge from PbS nanocrystals to ligand molecules is investigated in different solvents. We find that the charge transfer rate increases dramatically with solvent dielectric constant. This trend is accounted for by a modified Marcus theory that incorporates only static dielectric effects. The choice of solvent allows significant control of the charge transfer process. As an important example, we find that PbS nanocrystals dispersed in water exhibit charge transfer rates 1000 times higher than the same nanocrystals in organic solvent. Rapid charge extraction will be important to efficient nanocrystal-based photovoltaic and photodetector devices.

PbSe nanocrystal excitonic solar cells.

We report the design, fabrication, and characterization of colloidal PbSe nanocrystal (NC)-based photovoltaic test structures that exhibit an excitonic solar cell mechanism. Charge extraction from the NC active layer is driven by a photoinduced chemical potential energy gradient at the nanostructured heterojunction. By minimizing perturbation to PbSe NC energy levels and thereby gaining insight into the "intrinsic" photovoltaic properties and charge transfer mechanism of PbSe NC, we show a direct correlation between interfacial energy level offsets and photovoltaic device performance. Size dependent PbSe NC energy levels were determined by cyclic voltammetry and optical spectroscopy and correlated to photovoltaic measurements. Photovoltaic test structures were fabricated from PbSe NC films sandwiched between layers of ZnO nanoparticles and PEDOT:PSS as electron and hole transporting elements, respectively. The device current-voltage characteristics suggest a charge separation mechanism that is distinct from previously reported Schottky devices and consistent with signatures of excitonic solar cells. Remarkably, despite the limitation of planar junction structure, and without film thickness optimization, the best performing device shows a 1-sun power conversion efficiency of 3.4%, ranking among the highest performing NC-based solar cells reported to date.

Electrogenerated chemiluminescence from PbS quantum dots.

We report the first observation of electrogenerated chemiluminescence (ECL) from PbS quantum dots (QDs). Different ECL intensities are observed for different ligands used to passivate the QDs, which indicates that ECL is sensitive to surface chemistry, with the potential to serve as a powerful probe of surface states and charge transfer dynamics in QDs. In particular, passivation of the QD surfaces with trioctylphosphine (TOP) increases ECL intensity by 3 orders of magnitude when compared to passivation with oleic acid alone. The observed overlap of the ECL and photoluminescence spectra suggests a significant reduction of deep surface trap states from the QDs passivated with TOP.

Electron injection from colloidal PbS quantum dots into titanium dioxide nanoparticles.

Injection of photoexcited electrons from colloidal PbS quantum dots into TiO(2) nanoparticles is investigated. The electron affinity and ionization potential of PbS quantum dots, inferred from cyclic voltammetry measurements, show strong size dependence due to quantum confinement. On the basis of the measured energy levels, photoexcited electrons should transfer efficiently from the quantum dots into TiO(2) only for quantum-dot diameter below approximately 4.3 nm. Continuous-wave fluorescence spectra and fluorescence transients of PbS quantum dots coupled to titanium dioxide nanoparticles are consistent with electron transfer for small quantum dots. The measured electron transfer time is surprisingly slow ( approximately 100 ns), and implications of this for future photovoltaics will be discussed. Initial results obtained from solar cells sensitized with PbS quantum dots are presented.

Near-infrared fluorescence imaging with water-soluble lead salt quantum dots.

A simple procedure for transferring PbS and PbSe quantum dots into water is presented, along with characterization of the resulting water-soluble quantum dots. The external surface of the water-soluble quantum dots include carboxylic groups, which will allow target-specific labeling of cells. As a first example, near-infrared fluorescence imaging of human colon cancer cells is demonstrated using these water-soluble near-infrared fluorophores.