Self-Repairable Silicon Anodes Using a Multifunctional Binder for High-Performance Lithium-Ion Batteries.

Despite of extremely high theoretical capacity of Si (3579 mAh g-1 ), Si anodes suffer from pulverization and delamination of the electrodes induced by large volume change during charge/discharge cycles. To address those issues, herein, self-healable and highly stretchable multifunctional binders, polydioxythiophene:polyacrylic acid:phytic acid (PEDOT:PAA: PA, PDPP) that provide Si anodes with self-healability and excellent structural integrity is designed. By utilizing the self-healing binder, Si anodes self-repair cracks and damages of Si anodes generated during cycling. For the first time, it is demonstrated that Si anodes autonomously self-heal artificially created cracks in electrolytes under practical battery operating conditions. Consequently, this self-healable Si anode can still deliver a reversible capacity of 2312 mAh g-1 after 100 cycles with remarkable initial Coulombic efficiency of 94%, which is superior to other reported Si anodes. Moreover, the self-healing binder possesses enhanced Li-ion diffusivity with additional electronic conductivity, providing excellent rate capability with a capacity of 2084 mAh g-1 at a very high C-rate of 5 C.

Morphological-Electrical Property Relation in Cu(In,Ga)(S,Se)2 Solar Cells: Significance of Crystal Grain Growth and Band Grading by Potassium Treatment.

Solution-processed Cu(In,Ga)(S,Se)2  (CIGS) has a great potential for the production of large-area photovoltaic devices at low cost. However, CIGS solar cells processed from solution exhibit relatively lower performance compared to vacuum-processed devices because of a lack of proper composition distribution, which is mainly instigated by the limited Se uptake during chalcogenization. In this work, a unique potassium treatment method is utilized to improve the selenium uptake judiciously, enhancing grain sizes and forming a wider bandgap minimum region. Careful engineering of the bandgap grading structure also results in an enlarged space charge region, which is favorable for electron-hole separation and efficient charge carrier collection. Besides, this device processing approach has led to a linearly increasing electron diffusion length and carrier lifetime with increasing the grain size of the CIGS film, which is a critical achievement for enhancing photocurrent yield. Overall, 15% of power conversion efficiency is achieved in solar cells processed from environmentally benign solutions. This approach offers critical insights for precise device design and processing rules for solution-processed CIGS solar cells.

High-efficiency red electroluminescent device based on multishelled InP quantum dots.

We report on the synthesis of highly fluorescent red-emitting InP quantum dots (QDs) and their application to the fabrication of a high-efficiency QD-light-emitting diode (QLED). The core/shell heterostructure of the QDs is elaborately tailored toward a multishelled structure with a composition-gradient ZnSeS intermediate shell and an outer ZnS shell. Using the resulting InP/ZnSeS/ZnS QDs as an emitting layer, all-solution-processible red InP QLEDs are fabricated with a hybrid multilayered device structure having an organic hole transport layer (HTL) and an inorganic ZnO nanoparticle electron transport layer. Two HTLs of poly(9-vinlycarbazole) or poly[(9,9-dioctylfluorenyl-2,7-diyl)-co-(4,4'-(N-(4-sec-butylphenyl))diphenyl-amine), whose hole mobilities are different by at least three orders of magnitude, are individually applied for QLED fabrication and such HTL-dependent device performances are compared. Our best red device displays exceptional figures of merit such as a maximum luminance of 2849 cd/m2, a current efficiency of 4.2 cd/A, and an external quantum efficiency of 2.5%.

Analysis of wide color gamut of green/red bilayered freestanding phosphor film-capped white LEDs for LCD backlight.

In this study, we propose green/red bilayered freestanding phosphor film-capped white light-emitting diodes (W-LEDs) using InGaN blue LEDs and narrowband red and green phosphors to realize a wide color gamut in a liquid crystal display (LCD) backlight system. The narrowband K2SiF6:Mn4+ (KSF) red and SrGa2S4:Eu2+ (SGS) green phosphors are synthesized using a facile etching synthetic process and flux-aided solid state reaction under a H2S atmosphere, respectively, and the freestanding phosphor films are fabricated using a delamination method with water-soluble polymer, polystyrene sulfonic acid, PEDOT/PSS, and interlayered phosphor film. Various phosphor concentrations of green/red bilayered freestanding phosphor film-capped W-LEDs exhibit a correlated color temperature (CCT) and luminous efficacy range of 11,390 K ~6,540 K and 99 lm/W ~124 lm/W, respectively, with an applied current of 60 mA. The W-LED with green (12.5 wt%)/red (40 wt%) bilayered phosphor film, which exhibited luminous efficacy of 105 lm/W at the CCT of 8,330 K, is selected and the color gamut of the bare LED and phosphor RG and the filtered RGB triangle is calculated to be more than ~95% and ~86.4%, respectively, relative to the NTSC in the 1931 CIE color coordinates space.

Improved performance of dye-sensitized solar cells using dual-function TiO(2) nanowire photoelectrode.

A unique, hierarchically structured, aggregated TiO(2) nanowire (A-TiO(2)-nw) is prepared by solvothermal synthesis and used as a dual-functioning photoelectrode in dye-sensitized solar cells (DSSCs). The A-TiO(2)-nw shows improved light scattering compared to conventional TiO(2) nanoparticles (TiO(2)-np) and dramatically enhanced dye adsorption compared to conventional scattering particles (CSP). The A-TiO(2)-nw is used as a scattering layer for bilayer photoelectrodes (TiO(2)-np/A-TiO(2)-nw) in DSSCs to compare the cell performance to that of devices using state-of-the-art photoelectrode architectures (TiO(2)-np/CSP). The DSSCs fabricated using bilayers of TiO(2)-np/A-TiO(2)-nw show improved power conversion efficiency (9.1%) and current density (14.88 mA cm(-2)) compared to those using single-layer TiO(2)-np (7.6% and 11.84 mA cm(-2)) or TiO(2)-np/CSP bilayer structures (8.7% and 13.81 mA cm(-2)). The unique contribution of the A-TiO(2)-nw layers to the device performance is confirmed by studying the incident photon-to-current efficiency. The enhanced external quantum efficiencies at approximately 520 nm and 650 nm clearly reveal the dual functionality of A-TiO(2)-nw. These unique properties of A-TiO(2)-nw may be applied in other devices utilizing light-scattering n-type semiconductor.

Color-by-blue display using blue quantum dot light-emitting diodes and green/red color converting phosphors.

We report a novel full-color display based on the generation of full-color by a highly efficient blue QD-LED light approach, or so called color-by-blue QD-LED display. This newly proposed color-by-blue QD-LED display combines a blue CdZnS/ZnS QD-LED blue subpixel and excitation source with front-emitting green/red phosphor subpixels. It is carefully estimated that the detailed display characteristics as well as full color-conversion and reasonable device efficiency of blue, green, and red satisfy the minimum requirements for display application. Also, we would like to emphasize that the proposed blue, green, and red device shows maximum luminance of 1570, 12920, and 3120 cd/m², respectively, luminous efficiency of 1.5, 12.1, and 2.5 cd/A, respectively, and external quantum efficiency of 6.8, 2.8, and 2.0%, respectively. It is expected that full color generation by color-by-blue QD-LED will lead to further technological advancements in the area of efficient and facile display applications.

Quantum-dot-based white lighting planar source through downconversion by blue electroluminescence.

We report the unprecedented fabrication of a planar white lighting quantum dot light-emitting diode (QD-LED) through integrating a CdZnS QD-based blue electroluminescence (EL) device with a free-standing polymethyl methacrylate (PMMA) composite film embedded with orange-emitting Cu-In-S (CIS) green-greenish yellow-emitting Cu-In-Ga-S (CIGS) QDs. The hybrid device successfully generates bicolored white emission that comprises blue EL and downconverted QD photoluminescence. The hybrid QD-LEDs loaded with the composite film embedded with one type of QDs exhibit a limited white spectral coverage, consequently producing low values (<65) in color rendering index (CRI). Thus, the QD-PMMA film consisting of a blend of green CIGS and orange CIS QD downconverters is applied for obtaining a higher-CRI white light through the spectral extension, resulting in a much improved CRI of 75-77. Various EL performances of the hybrid planar white device versus the reference blue QD-LED are also characterized in details.

Coaxial RuO2-ITO nanopillars for transparent supercapacitor application.

Supercapacitive properties of ruthenium oxide (RuO2) nanoparticles electrodeposited onto the indium tin oxide (ITO) nanopillars were investigated. Compared to conventional planar current collectors, this coaxially nanostructured current collector-electrode system can provide increased contact for efficient charge transport, and the internanopillar spacing allows easy access of electrolyte ions. The morphological and electrochemical properties depended on the thickness of the RuO2 layers, i.e., the number of electrodeposition cycles. A maximum specific capacitance, Csp, of 1235 F/g at a scan rate of 50 mV/s was achieved for the 30-cycle deposited RuO2-ITO nanopillars. The other capacitive properties such as electrochemical reversibility and Csp retention at high scan rates also improved greatly.

Fabrication of solution processed 3D nanostructured CuInGaS2 thin film solar cells.

In this study we demonstrate the fabrication of CuInGaS2 (CIGS) thin film solar cells with a three-dimensional (3D) nanostructure based on indium tin oxide (ITO) nanorod films and precursor solutions (Cu, In and Ga nitrates in alcohol). To obtain solution processed 3D nanostructured CIGS thin film solar cells, two different precursor solutions were applied to complete gap filling in ITO nanorods and achieve the desirable absorber film thickness. Specifically, a coating of precursor solution without polymer binder material was first applied to fill the gap between ITO nanorods followed by deposition of the second precursor solution in the presence of a binder to generate an absorber film thickness of ∼1.3 µm. A solar cell device with a (Al, Ni)/AZO/i-ZnO/CdS/CIGS/ITO nanorod/glass structure was constructed using the CIGS film, and the highest power conversion efficiency was measured to be ∼6.3% at standard irradiation conditions, which was 22.5% higher than the planar type of CIGS solar cell on ITO substrate fabricated using the same precursor solutions.

Enhancement mechanism of quantum yield in core/shell/shell quantum dots of ZnS-AgIn5S8/ZnIn2S4/ZnS.

To achieve a high quantum yield (QY) of nanomaterials suitable for optical applications, we improved the optical properties of AgIn5S8 (AIS) quantum dots (QDs) by employing an alloyed-core/inner-shell/outer-shell (ZAIS/ZIS/ZnS) structure. We also investigated the mechanism of optical transitions to clarify the improvement of QYs. In AIS, the low-energy absorption near the band edge region is attributed to the weakly allowed band gap transition, which gains oscillator strength through state intermixing and electron-phonon coupling. The main photoluminescence is also ascribed to the weakly allowed band gap transition with characteristics of self-trapped excitonic emission. With alloying/shelling processes, the weakly allowed transition is enhanced by the evolution of the electronic structures in the alloyed core, which improves the band gap emission. In shelled structures, the nonradiative process is reduced by the reconstructed lattice and passivated surface, ultimately leading to a high QY of 85% in ZAIS/ZIS/ZnS. These findings provide new insights into the optical transitions of AIS because they challenge previous conclusions. In addition, our work elucidates the mechanism behind the enhancement of QY accomplished through alloying/shelling processes, providing strategies to optimize nontoxic QDs for various applications using a green chemistry approach.

Toward scatter-free phosphors in white phosphor-converted light-emitting diodes: reply to comments.

This is a reply to the comments by Hu et al. directed to a previous paper "Toward scatter-free phosphors in white phosphor-converted light-emitting diodes" by Park et al., [Opt. Express 20(9), 10218 (2012)].

Polarized white light from LEDs using remote-phosphor layer sandwiched between reflective polarizer and light-recycling dichroic filter.

This study introduces an efficient polarized, white phosphor-converted, light-emitting diode (pc-LED) using a remote phosphor film sandwiched between a reflective polarizer film (RPF) and a short-wavelength pass dichroic filter (SPDF). The on-axis brightness of polarized white light emission of a RPF/SPDF-sandwiched phosphor film over a blue LED, showed greater recovery than that of a conventional unpolarized remote phosphor film over blue LED, due to the recycling effect of yellow light from an SPDF. The relative luminous efficacy of an RPF/SPDF-sandwiched phosphor film was made 1.40 times better by adding an SPDF on the backside of an RPF-capped phosphor film. A polarization ratio of 0.84 was demonstrated for a white LED with an RPF/SPDF-sandwiched phosphor film, in good agreement with the measured results from the RPF-only sample.

Improved color coordinates of green monochromatic pc-LED capped with a band-pass filter.

This study introduces a "greener" green monochromatic phosphor-converted light-emitting diode (pc-LED) using a band-pass filter (BPF) combined with a long-pass dichroic filter (LPDF) and a short-pass dichroic filter (SPDF) to improve the color quality of our previously developed LPDF-capped green pc-LED. This can also address the drawbacks of III-V semiconductor-type green LEDs, which show a low luminous efficacy and a poor current dependence of the efficacy and color coordinates compared to blue semiconductor-type LEDs. The optical properties of green monochromatic pc-LEDs using a BPF are compared with those of LPDF-capped green pc-LEDs, which have a broad band spectrum, and III-V semiconductor-type green LEDs by changing the transmittance wavelength range of the BPF and the peak wavelength of the green phosphors. BPF-capped green monochromatic pc-LEDs provide a high luminous efficacy (134 lm/W at 60 mA), and "greener" 1931 Commission Internationale d'Eclairage (CIE; CIEx, CIEy) color coordinates (0.24, 0.66) owing to the narrowed emission spectrum. We also propose a two-dimensional (2D) polystyrene (PS) microbead (2-µm diameter) monolayer as a scattering layer to overcome the poor angular dependence of the color coordinates of the transmitted light through a nano-multilayered dichroic filter such as an LPDF or BPF. The 2D PS scattering layer improves the angular dependence of the green color emitted from a BPF-capped green pc-LED with only 3% loss of luminous efficacy.

Visible cathodoluminescence of quantum dot films by direct irradiation of electron beam and its materialization as a field emission device.

The field emission (FE) device based on quantum dot (QD) films as a cathodoluminescent (CL) material has not emerged yet due to the relatively low quantum efficiency and weak photostability of nanocrystals (NCs). Here we improve film stability and luminescence yields by preparing neat films of well-packed core-multishell QDs using spray coating method and then using low-temperature atomic layer deposition (ALD) to infill the pores of these films with metal oxides to produce inorganic nanocomposites. The ALD coatings to protect oxidation and degradation by electrons prevent internal atomic and molecular diffusion and decrease surface trap densities of QD films. Furthermore, the CL of the core-multishell QD films is 2.4 times higher than before ALD infilling. We fabricate the FE device by combining cathode structure with carbon nanotube (CNT) emitters and anode plates with QD thin film and successfully can get brilliant images of the light-emitting FE device. Our research opens a way for developing new quantum optoelectronics with high-performance.

Soft, adhesive and conductive composite for electroencephalogram signal quality improvement.

Since electroencephalogram (EEG) is a very small electrical signal from the brain, it is very vulnerable to external noise or motion artifact, making it difficult to measure. Therefore, despite the excellent convenience of dry electrodes, wet electrodes have been used. To solve this problem, self-adhesive and conductive composites using carbon nanotubes (CNTs) in adhesive polydimethylsiloxane (aPDMS), which can have the advantages of both dry and wet electrodes, have been developed by mixing them uniformly with methyl group-terminated PDMS. The CNT/aPDMS composite has a low Young's modulus, penetrates the skin well, has a high contact area, and excellent adhesion and conductivity, so the signal quality is enhanced. As a result of the EEG measurement test, although it was a dry electrode, results comparable to those of a wet electrode were obtained in terms of impedance and motion noise. It also shows excellent biocompatibility in a human fibroblast cell test and a week-long skin reaction test, so it can measure EEG with high signal quality for a long period of time.

Molecular Mechanism of Selective Al2O3 Atomic Layer Deposition on Self-Assembled Monolayers.

Area-selective atomic layer deposition (AS-ALD) of insulating metallic oxide layers could be a useful nanopatterning technique for making increasingly complex semiconductor circuits. Although the alkanethiol self-assembled monolayer (SAM) has been considered promising as an ALD inhibitor, the low inhibition efficiency of the SAM during ALD processes makes its wide application difficult. We investigated the deposition mechanism of Al2O3 on alkanethiol-SAMs using temperature-dependent vibrational sum-frequency-generation spectroscopy. We found that the thermally induced formation of gauche defects in the SAMs is the main causative factor deteriorating the inhibition efficiency. Here, we demonstrate that a discontinuously temperature-controlled ALD technique involving self-healing and dissipation of thermally induced stress on the structure of SAM substantially enhances the SAM's inhibition efficiency and enables us to achieve 60 ALD cycles (6.6 nm). We anticipate that the present experimental results on the ALD mechanism on the SAM surface and the proposed ALD method will provide clues to improve the efficiency of AS-ALD, a promising nanoscale patterning and manufacturing technique.

Development and Verification of a 480 nm Blue Light Enhanced/Reduced Human-Centric LED for Light-Induced Melatonin Concentration Control.

With the inherent sleep and wake cycle regulated by natural sunlight, the human body has evolved over millennia to be active during the day and to rest at night. However, maintaining an optimal 24 h cycle has become increasingly problematic in modern society as more people spend the majority of the day indoors. Many research groups have reported that inadequate artificial lighting interferes with melatonin production and disrupts the circadian rhythm. This study considered biological functions for light-emitting diodes (LEDs) of next-generation illumination, and LED packages and spectra suitable for both daytime and nighttime applications were designed. The prepared daytime human-centric (HC)-LEDs had a melanopic/photopic (M/P) ratio that was up to 26% higher than that of conventional (c)-LEDs, whereas the nighttime HC-LEDs exhibited up to a 26% lower M/P ratio compared to the c-LEDs. Nevertheless, because the HC-LED is designed to have almost the same color coordinates as the c-LED having the same correlated-color temperature (CCT), there is no change in the perceived color. To substantiate the biological effect, melatonin level data were obtained from 22 voluntary participants in c- and HC-LED lighting environments. In the HC-LED lighting environment, melatonin was suppressed by 21.9% after waking, and nocturnal melatonin secretion was increased by up to 12.2%. As human-centric lighting, our HC-LEDs are expected to become an essential element for modern life, where people spend most of their time indoors.

Isolation of Bovine Milk Exosome Using Electrophoretic Oscillation Assisted Tangential Flow Filtration with Antifouling of Micro-ultrafiltration Membrane Filters.

Tangent flow-driven ultrafiltration (TF-UF) is an efficient isolation process of milk exosomes without morphological deformation. However, the TF-UF approach with micro-ultrafiltration SiNx membrane filters suffers from the clogging and fouling of micro-ultrafiltration membrane filter pores with large bioparticles. Thus, it is limited in the long term, continuous isolation of large quantities of exosomes. In this work, we introduced electrophoretic oscillation (EPO) in the TF-UF approach to remove pore clogging and fouling of with micro-ultrafiltration SiNx membrane filters by large bioparticles. As a result, the combined EPO-assisted TF (EPOTF) filtration can isolate large quantities of bovine milk exosomes without deformation. Furthermore, several morphological and biological analyses confirmed that the EPOTF filtration approach could isolate the milk exosomes in high concentrations with high purity and intact morphology. In addition, the uptake test of fluorescent-labeled exosomes by the keratinocyte cells visualized the biological function of purified exosomes. Hence, compared to the TF-UF process, the EPOTF filtration produced a higher yield of bovine milk exosomes without stopping the filtering process for over 200 h. Therefore, this isolation process enables scalable and continuous production of morphologically intact exosomes from bovine milk, suggesting that high-quality exosome purification is possible for future applications such as drug nanocarriers, diagnosis, and treatments.

Toward scatter-free phosphors in white phosphor-converted light-emitting diodes.

Scatter-free phosphors promise to suppress the scattering loss of conventional micro-size powder phosphors in white phosphor-converted light-emitting diodes (pc-LEDs). Large micro-size cube phosphors (~100 µm) are newly designed and prepared as scatter-free phosphors, combining the two scatter-free conditions of particles based on Mie's scattering theory; the grain size or grain boundary was smaller than 50 nm and the particle size was larger than 30 µm. A careful evaluation of the conversion efficiency and packaging efficiency of the large micro-size cube phosphor-based white pc-LED demonstrated that large micro-size cube phosphors are an outstanding potential candidate for scatter-free phosphors in white pc-LEDs. The luminous efficacy and packaging efficiency of the Y(3)Al(5)O(12):Ce(3+) large micro-size cube phosphor-based pc-LEDs were 123.0 lm/W and 0.87 at 4300 K under 300 mA, which are 17% and 34% higher than those of commercial powder phosphor-based white LEDs (104.8 lm/W and 0.65), respectively. In addition, the introduction of large micro-size cube phosphors can reduce the wide variation in optical properties as a function of both the ambient temperature and applied current compared with those of conventional powder phosphor-based white LEDs.

Highly-efficient, tunable green, phosphor-converted LEDs using a long-pass dichroic filter and a series of orthosilicate phosphors for tri-color white LEDs.

This study introduces a long-pass dichroic filter (LPDF) on top of a phosphor-converted LED (pc-LED) packing associated with each corresponding tunable orthosilicate ((Ba,Sr)2SiO4:Eu) phosphor in order to fabricate tunable green pc-LEDs. These LPDF-capped green pc-LEDs provide luminous efficacies between 143­173 lm/W at 60 mA in a wavelength range between 515 and 560 nm. These tunable green pc-LEDs can replace green semiconductor-type III-V LEDs, which present challenges with respect to generating high luminous efficacy. We also introduce the highly-efficient tunable green pc-LEDs into tri-color white LED systems that combine an InGaN blue LED and green/red full down-converted pc-LEDs. The effect of peak wavelength in the tunable green pc-LEDs on the optical properties of a tri-color package white LED is analyzed to determine the proper wavelength of green color for tri-color white LEDs. The tri-color white LED provides excellent luminous efficacy (81.5­109 lm/W) and a good color rendering index (64­87) at 6500 K of correlated color temperature (CCT) with the peak wavelength of green pc-LEDs. The luminous efficacy of the LPDF-capped green monochromatic pc-LED and tri-color package with tunable green pc-LEDs can be increased by improving the external quantum efficiency of blue LEDs and the conversion efficiency of green pc-LEDs.