Extrinsic hydrophobicity-controlled silver nanoparticles as efficient and stable catalysts for CO2 electrolysis.

To realize economically feasible electrochemical CO2 conversion, achieving a high partial current density for value-added products is particularly vital. However, acceleration of the hydrogen evolution reaction due to cathode flooding in a high-current-density region makes this challenging. Herein, we find that partially ligand-derived Ag nanoparticles (Ag-NPs) could prevent electrolyte flooding while maintaining catalytic activity for CO2 electroreduction. This results in a high Faradaic efficiency for CO (>90%) and high partial current density (298.39 mA cm‒2), even under harsh stability test conditions (3.4 V). The suppressed splitting/detachment of Ag particles, due to the lipid ligand, enhance the uniform hydrophobicity retention of the Ag-NP electrode at high cathodic overpotentials and prevent flooding and current fluctuations. The mass transfer of gaseous CO2 is maintained in the catalytic region of several hundred nanometers, with the smooth formation of a triple phase boundary, which facilitate the occurrence of CO2RR instead of HER. We analyze catalyst degradation and cathode flooding during CO2 electrolysis through identical-location transmission electron microscopy and operando synchrotron-based X-ray computed tomography. This study develops an efficient strategy for designing active and durable electrocatalysts for CO2 electrolysis.

Ultrasensitive Near-Infrared InAs Colloidal Quantum Dot-ZnON Hybrid Phototransistor Based on a Gradated Band Structure.

Amorphous metal oxide semiconductor phototransistors (MOTPs) integrated with colloidal quantum dots (QDs) (QD-MOTPs) are promising infrared photodetectors owing to their high photoconductive gain, low off-current level, and high compatibility with pixel circuits. However, to date, the poor mobility of conventional MOTPs, such as indium gallium zinc oxide (IGZO), and the toxicity of lead (Pb)-based QDs, such as lead sulfide and lead selenide, has limited the commercial applications of QD-MOTPs. Herein, an ultrasensitive QD-MOTP fabricated by integrating a high-mobility zinc oxynitride (ZnON)-based MOTP and lead-free indium arsenide (InAs) QDs is demonstrated. A new gradated bandgap structure is introduced in the InAs QD layer that absorbs infrared light, which prevents carriers from moving backward and effectively reduces electron-hole recombination. Chemical, optical, and structural analyses confirm the movement of the photoexcited carriers in the graded band structure. The novel QD-MOTP exhibits an outstanding performance with a responsivity of 1.15 × 105 A W-1 and detectivity of 5.32 × 1016 Jones at a light power density of 2 µW cm-2 under illumination at 905 nm.

Structural, optical, and magnetic properties of Ag+, Mn+ and Ar+ ions implanted ZnO thin films: effect of implantation dose and stopping energy.

Herein, we systematically studied the effect of various excitation processes on the structural, optical, and magnetic properties of ZnO films implanted with 80 keV Ar+, 110 keV Mn+, and 190 keV Ag+ ions. Four different doses of 1 × 1013, 1 × 1014, 1 × 1015, and 2 × 1016 ions per cm2 were used for implantation. It was observed that the structural, optical, and magnetic properties of the implanted samples were dominantly affected at the highest dose of 2 × 1016 ions per cm2. For lower doses, insignificant changes in these properties were observed. A comparison of various processes involved in the implantation process shows that both the electronic excitation and nuclear excitation processes are responsible for the changes in the structural, optical, and magnetic properties of the implanted ZnO films.

SWIR imaging using PbS QD photodiode array sensors.

We fabricated a 1 × 10 PbS QD photodiode array with multiple stacked QD layers with high-resolution patterning using a customized photolithographic process. The array showed the average responsivity of 5.54 × 10-3 A/W and 1.20 × 10-2 A/W at 0 V and -1 V under 1310- nm short-wavelength infrared (SWIR) illumination. The standard deviation of the pixel responsivity was under 10%, confirming the uniformity of the fabrication process. The response time was 2.2 ± 0.13 ms, and the bandwidth was 159.1 Hz. A prototype 1310-nm SWIR imager demonstrated that the QD photodiode-based SWIR image sensor is a cost-effective and practical alternative for III-V SWIR image sensors.

Exploring dopant effects in stannic oxide nanoparticles for CO2 electro-reduction to formate.

The electrosynthesis of formate from CO2 can mitigate environmental issues while providing an economically valuable product. Although stannic oxide is a good catalytic material for formate production, a metallic phase is formed under high reduction overpotentials, reducing its activity. Here, using a fluorine-doped tin oxide catalyst, a high Faradaic efficiency for formate (95% at 100 mA cm-2) and a maximum partial current density of 330 mA cm-2 (at 400 mA cm-2) is achieved for the electroreduction of CO2. Furthermore, the formate selectivity (≈90%) is nearly constant over 7 days of operation at a current density of 100 mA cm-2. In-situ/operando spectroscopies reveal that the fluorine dopant plays a critical role in maintaining the high oxidation state of Sn, leading to enhanced durability at high current densities. First-principle calculation also suggests that the fluorine-doped tin oxide surface could provide a thermodynamically stable environment to form HCOO* intermediate than tin oxide surface. These findings suggest a simple and efficient approach for designing active and durable electrocatalysts for the electrosynthesis of formate from CO2.

An Artificial Tactile Neuron Enabling Spiking Representation of Stiffness and Disease Diagnosis.

Mechanical properties of biological systems provide useful information about the biochemical status of cells and tissues. Here, an artificial tactile neuron enabling spiking representation of stiffness and spiking neural network (SNN)-based learning for disease diagnosis is reported. An artificial spiking tactile neuron based on an ovonic threshold switch serving as an artificial soma and a piezoresistive sensor as an artificial mechanoreceptor is developed and shown to encode the elastic stiffness of pressed materials into spike frequency evolution patterns. SNN-based learning of ultrasound elastography images abstracted by spike frequency evolution rate enables the classification of malignancy status of breast tumors with a recognition accuracy up to 95.8%. The stiffness-encoding artificial tactile neuron and learning of spiking-represented stiffness patterns hold a great promise for the identification and classification of tumors for disease diagnosis and robot-assisted surgery with low power consumption, low latency, and yet high accuracy.

Interplay of sidewall damage and light extraction efficiency of micro-LEDs.

This Letter describes the impact of shape on micro light-emitting diodes (µLEDs), analyzing 400 µm2 area µLEDs with various mesa shapes (circular, square, and stripes). Appropriate external quantum efficiency (EQE) can yield internal quantum efficiency (IQE) which decreases with increasing peripheral length of the mesas. However, light extraction efficiency (ηe) increased with increasing mesa periphery. We introduce analysis of Jpeak (the current at peak EQE) since it is proportional to the non-radiative recombination. Etching the sidewalls using tetramethylammonium hydroxide (TMAH) increased the peak EQE and decreased the sidewall dependency of Jpeak. Quantitatively, the TMAH etching reduced non-radiative surface recombination by a factor of four. Hence, shrinking µLEDs needs an understanding of the relationship between non-radiative recombination and ηe, where analyzing Jpeak can offer new insights.

Realization of an Artificial Visual Nervous System using an Integrated Optoelectronic Device Array.

Human behavior (e.g., the response to any incoming information) has very complex forms and is based on the response to consecutive external stimuli entering varied sensory receptors. Sensory adaptation is an elementary form of the sensory nervous system known to filter out irrelevant information for efficient information transfer from consecutive stimuli. As bioinspired neuromorphic electronic system is developed, the functionality of organs shall be emulated at a higher level than the cell. Because it is important for electronic devices to possess sensory adaptation in spiking neural networks, the authors demonstrate a dynamic, real-time, photoadaptation process to optical irradiation when repeated light stimuli are presented to the artificial photoreceptor. The filtered electrical signal generated by the light and the adapting signal produces a specific range of postsynaptic states through the neurotransistor, demonstrating changes in the response according to the environment, as normally perceived by the human brain. This successfully demonstrates plausible biological sensory adaptation. Further, the ability of this circuit design to accommodate changes in the intensity of bright or dark light by adjusting the sensitivity of the artificial photoreceptor is demonstrated. Thus, the proposed artificial photoreceptor circuits have the potential to advance neuromorphic device technology by providing sensory adaptation capabilities.

Design of mid-infrared filter array based on plasmonic metal nanodiscs array and its application to on-chip spectrometer.

Mid-infrared wavelengths are called the molecular fingerprint region because it contains the fundamental vibrational modes inherent to the substances of interest. Since the mid-infrared spectrum can provide non-destructive identification and quantitative analysis of unknown substances, miniaturized mid-infrared spectrometers for on-site diagnosis have attained great concern. Filter-array based on-chip spectrometer has been regarded as a promising alternative. In this study, we explore a way of applying a pillar-type plasmonic nanodiscs array, which is advantageous not only for excellent tunability of resonance wavelength but also for 2-dimensional integration through a single layer process, to the multispectral filter array for the on-chip spectrometer. We theoretically and experimentally investigated the optical properties of multi-periodic triangular lattices of metal nanodiscs array that act as stopband filters in the mid-infrared region. Soft-mold reverse nanoimprint lithography with a subsequent lift-off process was employed to fabricate the multispectral filter array and its filter function was successfully extracted using a Fourier transform infrared microscope. With the measured filter function, we tested the feasibility of target spectrum reconstruction using a Tikhonov regularization method for an ill-posed linear problem and evaluated its applicability to the infrared spectroscopic sensor that monitors an oil condition. These results not only verify that the multispectral filter array composed of stopband filters based on the metal nanodiscs array when combined with the spectrum reconstruction technique, has great potential for use to a miniaturized mid-infrared on-chip spectrometer, but also provide effective guidance for the filter design.

Sputtering-deposited amorphous SrVOx-based memristor for use in neuromorphic computing.

The development of brain-inspired neuromorphic computing, including artificial intelligence (AI) and machine learning, is of considerable importance because of the rapid growth in hardware and software capacities, which allows for the efficient handling of big data. Devices for neuromorphic computing must satisfy basic requirements such as multilevel states, high operating speeds, low energy consumption, and sufficient endurance, retention and linearity. In this study, inorganic perovskite-type amorphous strontium vanadate (a-SrVOx: a-SVO) synthesized at room temperature is utilized to produce a high-performance memristor that demonstrates nonvolatile multilevel resistive switching and synaptic characteristics. Analysis of the electrical characteristics indicates that the a-SVO memristor illustrates typical bipolar resistive switching behavior. Multilevel resistance states are also observed in the off-to-on and on-to-off transition processes. The retention resistance of the a-SVO memristor is shown to not significantly change for a period of 2 × 104 s. The conduction mechanism operating within the Ag/a-SVO/Pt memristor is ascribed to the formation of Ag-based filaments. Nonlinear neural network simulations are also conducted to evaluate the synaptic behavior. These results demonstrate that a-SVO-based memristors hold great promise for use in high-performance neuromorphic computing devices.

Self-catalytic-grown SnO x nanocones for light outcoupling enhancement in organic light-emitting diodes.

Light extraction in organic light-emitting diodes (OLEDs) was improved by applying SnO x nanocones grown via thermal annealing in a low-O2 atmosphere. SnO x was easily fabricated through thermal processing after Sn deposition. The diameter of the SnO x nanocones was controlled by changing the deposition thickness of Sn. The SnO x nanocones induced strong Mie scattering, which reduced the total internal reflection in the glass substrate. Consequently, the OLED with SnO x nanocones exhibited a 23% increase in the external quantum efficiency compared with a reference device.

Optimization of tunable guided-mode resonance filter based on refractive index modulation of graphene.

To fabricate a tunable optical filter with a fast response in the near infrared region, a tunable guided-mode resonance (GMR) filter using graphene was proposed and its performance was optimized. In this study, a rigorous coupled wave analysis method was employed to systematically investigate the effects of geometrical configuration of graphene-integrated GMR filters and the optical properties of constituent materials including graphene on their spectral response in terms of tunability and extinction ratio. It was found that as the graphene is located close to the waveguide and the evanescent-field strength at the interface increases, the GMR filter exhibits better tunability. The bandwidth of the filter could be drastically reduced by adopting a low-index contrast grating layer, so that the extinction ratio of an optical signal could be greatly improved from 0.91 dB to 27.99 dB as the index contrast decreased from 0.99 to 0.47, respectively. Furthermore, new practical device designs, that is easy to fabricate and effectively implement the electric-field doping of graphene at low gate voltage, were also suggested and theoretically validated. These results demonstrate not only the excellent potential of a graphene-based tunable GMR filter but also provide practical design guidelines for optimizing the device performance.

Solid-State Carbon-Doped GaN Schottky Diodes by Controlling Dissociation of the Graphene Interlayer with a Sputtered AlN Capping Layer.

Carbon-doped GaN (GaN:C) Schottky diodes are prepared by controlling the destruction status of the graphene interlayer (GI) on the substrate. The GI without a sputtered AlN capping layer (CL) was destroyed because of ammonia precursor etching behavior in a high-temperature epitaxy. The damaged GI, like nanographite as a solid-state carbon doping source, incorporated the epitaxial growth of the GaN layer. The secondary ion mass spectroscopy depth profile indicated that the carbon content in the GaN layer can be tuned further by optimizing the sputtering temperature of AlN CL because of the better capping ability of high crystalline quality AlN CL on GI being achieved at higher temperature. The edge-type threading dislocation density and carbon concentration of the GaN:C layer with an embedded 550 °C-grown AlN CL on a GI substrate can be significantly reduced to 2.28 × 109 cm-2 and ∼2.88 × 1018 cm-3, respectively. Thus, a Ni-based Schottky diode with an ideality factor of 1.5 and a barrier height of 0.72 eV was realized on GaN:C. The series resistance increased from 28 kΩ at 303 K to 113 kΩ at 473 K, while the positive temperature coefficient (PTC) of series resistance was ascribed to the carbon doping that induced the compensation effect and lattice scattering effect. The decrease of the donor concentration was confirmed by temperature-dependent capacitance-voltage (C-V-T) measurement. The PTC characteristic of GaN:C Schottky diodes created by dissociating the GI as a carbon doping source should allow for the future use of high-voltage Schottky diodes in parallel, especially in high-temperature environments.

Improved angular color uniformity and hydrothermal reliability of phosphor-converted white light-emitting diodes by using phosphor sedimentation.

We investigated the effect of phosphor deposition methods on the correlated color temperature (CCT), luminous flux and thermal characteristics of packaged white light-emitting diodes (WLEDs) for use in mobile display products. For both the samples, the CCT decreased with increasing viewing angle. Phosphor sedimentation samples displayed much better angular color uniformity than phosphor dispersion samples. The phosphor sedimentation sample had higher luminous flux and luminous efficacy at 20 mA than the phosphor dispersion sample. The phosphor sedimentation sample displayed much better high-temperature/humidity (85 °C/85%) reliability and lower package temperatures compared with the phosphor dispersion sample.

Flexible ITO films with atomically flat surfaces for high performance flexible perovskite solar cells.

We report high performance flexible Sn-doped In2O3 (ITO) films prepared by in-line type vertical plasma arc ion plating for high performance flexible perovskite solar cells. Even at room temperature deposition, the ion-plated ITO film showed a low sheet resistance of 15.75 Ohm per square, a high average optical transmittance of 85.88% and a small outer bending radius of 5 mm because energetic ITO ions accelerated to the substrate led to better crystallinity and adhesion than sputtered ITO films. In addition, the ion-plated ITO films showed atomically flat and smooth surfaces due to different growth mechanisms and the absence of resputtering effects during the ion plating process. Flexible perovskite solar cells fabricated on the ion-plated ITO electrodes showed a higher power conversion efficiency of 16.8% than the sputtered ITO-based perovskite solar cell, indicating the potential of ion plated ITO films as promising flexible and transparent electrodes for perovskite solar cells.

Light output performance of red AlGaInP-based light emitting diodes with different chip geometries and structures.

We investigated the optical and electrical properties of red AlGaInP light-emitting diodes (LEDs) as functions of chip size, p-cladding layer thickness, and the number of multi-quantum wells (MQWs). External quantum efficiency (EQE) decreased with decreasing chip size. The ideality factor gradually increased from 1.47 to 1.95 as the chip size decreased from 350 µm to 15 µm. This indicates that the smaller LEDs experienced larger carrier loss due to Shockley-Read-Hall nonradiative recombination at sidewall defects. S parameter, defined as ∂lnL/∂lnI, increased with decreasing chip size. Simulations and experimental results showed that smaller LEDs with 5 pairs of MQWs had over 30% higher IQE at 5 A/cm2 than the LED with 20 pairs of MQWs. These results show that the optimization of the number of QWs is needed to obtain maximum EQE of micro-LEDs.

An Optically Flat Conductive Outcoupler Using Core/Shell Ag/ZnO Nanochurros.

Transparent conductive electrodes (TCEs) featuring a smooth surface are indispensable for preserving pristine electrical characteristics in optoelectronic and transparent electronic devices. For high-efficiency organic light emitting diodes (OLEDs), a high outcoupling efficiency, which is crucial, is only achieved by incorporating a wavelength-scale undulating surface into a TCE layer, but this inevitably degrades device performance. Here, an optically flat, high-conductivity TCE composed of core/shell Ag/ZnO nanochurros (NCs) is reported embedded within a resin film on a polyethylene terephthalate substrate, simultaneously serving as an efficient outcoupler and a flexible substrate. The ZnO NCs are epitaxially grown on the {100} planes of a pentagonal Ag core and the length of ZnO shells is precisely controlled by the exposure time of Xe lamp. Unlike Ag nanowires films, the Ag/ZnO NCs films markedly boost the optical tunneling of light. Green-emitting OLEDs (2.78 × 3.5 mm2 ) fabricated with the Ag/ZnO TCE exhibit an 86% higher power efficiency at 1000 cd m-2 than ones with an Sn-doped indium oxide TCE. A full-vectorial electromagnetic simulation suggests the suppression of plasmonic absorption losses within their Ag cores. These results provide a feasibility of multifunctional TCEs with synthetically controlled core/shell nanomaterials toward the development of high-efficiency LED and solar cell devices.

High efficiency ultraviolet GaN-based vertical light emitting diodes on 6-inch sapphire substrate using ex-situ sputtered AlN nucleation layer.

We demonstrated the growth of crack-free high-quality GaN-based UV vertical LEDs (VLEDs) (λ = 365 nm) on 6-inch sapphire substrates by using an ex-situ sputtered AlN nucleation layer (NL) and compared their performance with that of UV VLEDs with an in situ low temperature (LT) AlGaN NL. The X-ray diffraction (XRD) results showed that the ex-situ AlN sample contained lower densities of screw-type and edge-type threading dislocations than the in situ AlGaN NL sample. The micro-Raman results revealed that the ex-situ AlN sample was under more compressive stress than the in situ AlGaN sample. As the current was increased, the electroluminescence peaks of both of the samples blue-shifted, reached a minimum wavelength at 1000 mA, and then slightly red-shifted. Packaged VLEDs with the ex-situ AlN NL yielded 6.5% higher light output power at 500 mA than that with the in situ AlGaN NL. The maximum EQEs of the VLED with the in situ AlGaN and ex-situ AlN NLs were 43.7% and 48.2%, respectively. Based on the XRD and Raman results, the improved light output power of the ex-situ AlN sample is attributed to the lower density of TDs.

Use of a patterned current blocking layer to enhance the light output power of InGaN-based light-emitting diodes.

We employed a patterned current blocking layer (CBL) to enhance light output power of GaN-based light-emitting diodes (LEDs). Nanoimprint lithography (NIL) was used to form patterned CBLs (a diameter of 260 nm, a period of 600, and a height of 180 nm). LEDs (chip size: 300 × 800 µm2) fabricated with no CBL, a conventional SiO2 CBL, and a patterned SiO2 CBL, respectively, exhibited forward-bias voltages of 3.02, 3.1 and 3.1 V at an injection current of 20 mA. The LEDs without and with CBLs gave series resistances of 9.8 and 11.0 Ω, respectively. The LEDs with a patterned SiO2 CBL yielded 39.6 and 11.9% higher light output powers at 20 mA, respectively, than the LEDs with no CBL and conventional SiO2 CBL. On the basis of emission images and angular transmittance results, the patterned CBL-induced output enhancement is attributed to the enhanced light extraction and current spreading.

Formation of an indium tin oxide nanodot/Ag nanowire electrode as a current spreader for near ultraviolet AlGaN-based light-emitting diodes.

Indium tin oxide (ITO) nanodots (NDs) were combined with Ag nanowires (Ag NWs) as a p-type electrode in near ultraviolet AlGaN-based light-emitting diodes (LEDs) to increase light output power. The Ag NWs were 30 ± 5 nm in diameter and 25 ± 5 µm in length. The transmittance of 10 nm-thick ITO-only was 98% at 385 nm, while the values for ITO ND/Ag NW were 83%-88%. ITO ND/Ag NW films showed lower sheet resistances (32-51 Ω sq-1) than the ITO-only film (950 Ω sq-1). LEDs (chip size: 300 × 800 µm2) fabricated using the ITO NDs/Ag NW electrodes exhibited higher forward-bias voltages (3.52-3.75 V at 20 mA) than the LEDs with the 10 nm-thick ITO-only electrode (3.5 V). The LEDs with ITO ND/Ag NW electrodes yielded a 24%-62% higher light output power (at 20 mA) than those with the 10 nm-thick ITO-only electrode. Furthermore, finite-difference time-domain (FDTD) simulations were performed to investigate the extraction efficiency. Based on the emission images and FDTD simulations, the enhanced light output with the ITO ND/Ag NW electrodes is attributed to improved current spreading and better extraction efficiency.