An Ultrahigh Efficiency Excitonic Micro-LED.

High efficiency micro-LEDs, with lateral dimensions as small as one micrometer, are desired for next-generation displays, virtual/augmented reality, and ultrahigh-speed optical interconnects. The efficiency of quantum well LEDs, however, is reduced to negligibly small values when scaled to such small dimensions. Here, we show such a fundamental challenge can be overcome by developing nanowire excitonic LEDs. Harnessing the large exciton oscillator strength of quantum-confined nanostructures, we demonstrate a submicron scale green-emitting LED having an external quantum efficiency and wall-plug efficiency of 25.2% and 20.7%, respectively, the highest values reported for any LEDs of this size to our knowledge. We established critical factors for achieving excitonic micro-LEDs, including the epitaxy of nanostructures to achieve strain relaxation, the utilization of semipolar planes to minimize polarization effects, and the formation of nanoscale quantum-confinement to enhance electron-hole wave function overlap. This work provides a viable path to break the efficiency bottleneck of nanoscale optoelectronics.

InGaN micro-light-emitting diodes monolithically grown on Si: achieving ultra-stable operation through polarization and strain engineering.

Micro or submicron scale light-emitting diodes (µLEDs) have been extensively studied recently as the next-generation display technology. It is desired that µLEDs exhibit high stability and efficiency, submicron pixel size, and potential monolithic integration with Si-based complementary metal-oxide-semiconductor (CMOS) electronics. Achieving such µLEDs, however, has remained a daunting challenge. The polar nature of III-nitrides causes severe wavelength/color instability with varying carrier concentrations in the active region. The etching-induced surface damages and poor material quality of high indium composition InGaN quantum wells (QWs) severely deteriorate the performance of µLEDs, particularly those emitting in the green/red wavelength. Here we report, for the first time, µLEDs grown directly on Si with submicron lateral dimensions. The µLEDs feature ultra-stable, bright green emission with negligible quantum-confined Stark effect (QCSE). Detailed elemental mapping and numerical calculations show that the QCSE is screened by introducing polarization doping in the active region, which consists of InGaN/AlGaN QWs surrounded by an AlGaN/GaN shell with a negative Al composition gradient along the c-axis. In comparison with conventional GaN barriers, AlGaN barriers are shown to effectively compensate for the tensile strain within the active region, which significantly reduces the strain distribution and results in enhanced indium incorporation without compromising the material quality. This study provides new insights and a viable path for the design, fabrication, and integration of high-performance µLEDs on Si for a broad range of applications in on-chip optical communication and emerging augmented reality/mixed reality devices, and so on.

High performance langasite based SAW NO2 gas sensor using 2D g-C3N4@TiO2 hybrid nanocomposite.

Nitrogen dioxide (NO2) gas has emerged as a severe air pollutant that causes damages to the environment, human life and global ecosystems etc. However, the currently available NO2 gas sensors suffers from insufficient selectivity, sensitivity and long response times that impeding their practical applicability for room temperature (RT) gas sensing. Herein, we report a high performance langasite (LGS) based surface acoustic wave (SAW) RT NO2 gas sensor using 2-dimensional (2D) g-C3N4@TiO2 nanoplates (NP) with {001} facets hybrid nanocomposite as a chemical interface. The g-C3N4@TiO2 NP/LGS SAW device showed a significant negative frequency shift (∆f) of ~19.8 kHz which is 2.4 fold higher than that of the pristine TiO2 NP/LGS SAW sensor toward 100 ppm of NO2 at RT. In addition, the hybrid SAW device fascinatingly exhibited a fast response/recovery time with a low detection limit, high selectivity, and an effective long term stability toward NO2 gas. It also exhibited an enhanced and robust negative frequency shifts under various relative humidity conditions ranging from 20% to 80% for 100 ppm of NO2 gas. The high performance of the g-C3N4 @TiO2 NP/LGS SAW gas sensor can be attributed to the enhanced mass loading effect which was assisted by the large surface area, oxygen vacancies, OH and amine functional groups of the n-n hybrid heterojunction of g-C3N4@TiO2 NP that provide abundant active sites for the adsorption and diffusion of NO2 gas molecules. These results emphasize the significance of the integration of 2D materials with metal oxides for SAW based RT gas sensing technology holds great promise in environmental protection.

Proliferation of the Light and Gas Interaction with GaN Nanorods Grown on a V-Grooved Si(111) Substrate for UV Photodetector and NO2 Gas Sensor Applications.

Although excellent milestones of III-nitrides in optoelectronic devices have been achieved, the focus on the optimization of their geometrical structure for multiple applications is very rare. To address this issue, we exclusively designed a prototype device to enhance the photoconversion efficiency and gas interaction capabilities of GaN nanorods (NRs) grown on a V-grooved Si(100) substrate with Si(111) facets for photodetector and gas sensor applications. Photoluminescence studies have demonstrated an increased surface-to-volume ratio and light trapping for GaN NRs grown on V-grooved Si(111). GaN NRs on V-grooved Si(100) with Si(111) facets exhibited high photodetection performance in terms of photoresponsivity (217 mA/cm2), detectivity (3 × 1013 Jones), and external quantum efficiency (2.73 × 105%) compared to GaN NRs grown on plain Si(111). Owing to the robust interconnection between NRs and a high surface-to-volume ratio, the GaN NRs grown on V-grooved Si(100) with Si(111) facets probed for NO2 detection with the assistance of photonic energy. The photo-assisted sensing makes it possible to detect NO2 gas at the ppb level at room temperature, resulting in significant power reduction. The device showed high selectivity to NO2 against other target gases, such as NO, H2S, H2, NH3, and CO. The device showed excellent long-term stability at room temperature; the humidity effect on the device performance was also examined. The excellent device performance was due to the following: (i) benefited from the V-grooved Si structure, GaN NRs significantly trapped the incident light, which promoted high photocurrent conversion efficiency and (ii) GaN NRs grown on V-grooved Si(100) with Si(111) facets increased the surface-to-volume ratio and thus improved the gas interaction with a better diffusion ratio and high light trapping, which resulted in increased response/recovery times. These results represent an important forward step in prototype devices for multiple applications in materials research.

Ag Nanowire-Plasmonic-Assisted Charge Separation in Hybrid Heterojunctions of Ppy-PEDOT:PSS/GaN Nanorods for Enhanced UV Photodetection.

The surface states, poor carrier life, and other native defects in GaN nanorods (NRs) limit their utilization in high-speed and large-gain ultraviolet (UV) photodetection applications. Making a hybrid structure is one of the finest strategies to overcome such impediments. In this work, a polypyrrole (Ppy)-poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS)/GaN NRs hybrid structure is introduced for self-powered UV photodetection applications. This hybrid structure yields high photodetection performance, while pristine GaN NRs showed negligible photodetection properties. The ability of the photodetector is further boosted by functionalizing the hybrid structure with Ag nanowires (NWs). The Ag NWs-functionalized hybrid structure exhibited a responsivity of 3.1 × 103 (A/W), detectivity of 3.19 × 1014 Jones, and external quantum efficiency of 1.06 × 106 (%) under a UV illumination of λ = 382 nm. This high photoresponse is due to the huge photon absorption rising from the localized surface plasmonic effect of a Ag NWs network. Also, the Ag NWs significantly improved the rising and falling times, which were noted to be 0.20 and 0.21 s, respectively. The model band diagram was proposed with the assistance of X-ray photoelectron spectroscopy to explore the origin of the superior performance of the Ag NWs-decorated Ppy-PEDOT:PSS/GaN NRs photodetector. The proposed hybrid structure seems to be a promising candidate for the development of high-performance UV photodetectors.

Hydrogen passivation: a proficient strategy to enhance the optical and photoelectrochemical performance of InGaN/GaN single-quantum-well nanorods.

Recently, III-nitride semiconductor nanostructures, especially InGaN/GaN quantum well nanorods (NRs), have been established as a promising material of choice for nanoscale optoelectronics and photoelectrochemical (PEC) water-splitting applications. Due to the large number of surface states, III-nitride NRs suffer from low quantum efficiency. Therefore, control of the surface states is necessary to improve device performance in real-time applications. In this work, we investigated the effect of hydrogen plasma treatment on the optical properties of InGaN/GaN single-quantum-well (SQW) NRs. The low-temperature photoluminescence (PL) studies revealed that yellow and green emissions overlapped and the yellow band is more dominant in the pristine InGaN/GaN SQW NRs. However, the emission corresponding to yellow luminescence was strongly suppressed and the green emission is more intensified in hydrogenated InGaN/GaN SQW NRs. Furthermore, the time-resolved PL spectroscopy studies revealed that the carrier lifetimes of hydrogenated InGaN/GaN SQW NRs are relatively short compared to the pristine InGaN/GaN SQW, indicating the effective reduction of non-radiative centers. From the PEC measurement, the photocurrent density of hydrogenated InGaN/GaN SQW NRs in the H2SO4 solution is found to be 5 mA cm-2 at -0.48 V versus reversible hydrogen electrode, which is 3.5-fold larger than that of pristine ones. These findings shed new light on the significance of surface treatment on the optical properties and thus nanostructured photoelectrodes for PEC applications.

Hydrogenation-produced In2O3/InN core-shell nanorod and its effect on NO2 gas sensing behavior.

In this work, for the first time, we have made InN/In2O3 core-shell heterostructure by hydrogen plasma treatment. InN nanorods (NRs) were grown by using plasma-assisted molecular beam epitaxy, and hydrogen plasma treatment was performed by using reactive ion etching at room temperature. From x-ray photoemission spectroscopy studies, it was observed that the bonding partner of In changes from N to O and N 1s completely disappeared in the hydrogenated InN NRs. Furthermore, high-resolution transmission electron microscopy revealed the formation of InN/In2O3 core-shell NRs by hydrogenation plasma treatment. The resistance of pristine InN NRs was decreased in NO2 ambient. Interestingly, the resistance of the InN/In2O3 core-shell was increased while introducing NO2 gas. InN NR surface exhibits downward band bending due to the electron accumulation, in NO2 ambient, and the surface band bending was decreased due to the increase in the bulk conduction channel. This reversed gas sensing behavior in InN/In2O3 core-shell NRs was attributed to the increase in depletion layer while reducing the conduction channel width by the absorption of NO2. The InN/In2O3 coreshell NRs exhibited a response of 22.43% at 50 °C, which was 5.11 times higher than that of pristine InN NRs.

Enhancing the Charge Carrier Separation and Transport via Nitrogen-Doped Graphene Quantum Dot-TiO2 Nanoplate Hybrid Structure for an Efficient NO Gas Sensor.

Herein, we demonstrate the ultraviolet (UV) light activated high-performance room-temperature NO gas sensor based on nitrogen-doped graphene quantum dots (NGQDs)-decorated TiO2 hybrid structure. TiO2 employed in the form of {001} facets exposed rectangular nanoplate morphology, which is highly reactive for the adsorption of active oxygen species. NGQD layers are grown on TiO2 nanoplates by graphitization of precursors via hydrothermal treatment. The decoration of NGQDs on the TiO2 surface dramatically enhanced the efficiency of gas and carriers exchange, charge carrier separation and transportation, and oxygen vacancies, which eventually improved the sensing performance. At room temperature, the TiO2@NGQDs hybrid structure exhibited a response of 12.0% to 100 ppm NO, which is 4.8 times higher compared to that of pristine TiO2 nanoplates. The response of TiO2@NGQDs hybrid structure is further upgraded by employing the ultraviolet light illumination and manipulating the operating temperature. Under the UV (λ = 365 nm) illumination at room temperature, the hybrid structure response escalated to ∼31.1% for 100 ppm NO. On the other hand, the tailoring of working temperature yielded a response of ∼223% at an optimum operating temperature of 250 °C. The NO gas-sensing mechanism of TiO2@NGQDs nanoplate's hybrid structure sensors under UV illumination and different working temperatures is discussed.

A novel low-temperature resistive NO gas sensor based on InGaN/GaN multi-quantum well-embedded p-i-n GaN nanorods.

In gas sensors, metal oxide semiconductors have been considered as favorable resistive-type toxic gas sensing materials. However, the higher temperature operation of metal oxides becomes a barrier for their wide range of applications in explosive and flammable gas environments. In this regard, great efforts have been devoted to reducing the operating temperature of the sensor. We demonstrated a chemical resistor-type NO gas sensor based on p-i-n GaN nanorods (NRs) consisting of InGaN/GaN multi-quantum wells (MQW). The sensor exhibited superior NO gas sensing performance to p-type GaN NRs. Furthermore, it also showed a remarkably improved response and fast recovery under UV irradiation (λ = 367 nm) of different UV intensities (7 to 20 mw cm-2) under reverse bias. The sensing performance of MQW-embedded p-i-n GaN NRs was enhanced with the boosted response by 4-fold at 35 °C under UV irradiation. The significant decrease in the resistance of the sensor under UV irradiation was mainly due to the extraction of photo-generated carriers under reverse bias, which can enhance the ionization of oxygen molecules. In addition, the effect of relative humidity (30%-60%) on the gas sensing performance was also manifested in this study. The selectivity of the sensor was determined by using other gases (NO, NO2, O2, NH3, H2S, CO, and H2), which exhibited a low response towards all tested gases other than NO. The experimental results demonstrated that p-i-n GaN NRs with InGaN/GaN MQW is a promising material for the detection of NO gas. Specific emphasis was laid on the enhanced response of p-i-n GaN NRs in reverse bias under UV irradiation.

High performance UV photodetectors using Nd3+ and Er3+ single- and co-doped DNA thin films.

Even though lanthanide ion (Ln3+)-doped DNA nanostructures have been utilized in various applications, they are rarely employed for photovoltage generating devices because of difficulties in designing DNA-based devices that generate voltages under light illumination. Here, we constructed DNA lattices made of synthetic strands and DNA thin films extracted from salmon (SDNA) with single-doping of Nd3+ or Er3+ and co-doping of Nd3+/Er3+ for high performance UV detection. The topological change of the DNA double-crossover (DX) lattices during the course of annealing was estimated from atomic force microscope (AFM) images to find the optimum concentration of Ln3+ ([Ln3+]O). No topological disturbance in DNA DX lattices were observed up to [Ln3+]O, and significant enhancement in the physical properties was obtained at [Ln3+]O. The interactions between Ln3+ and SDNA were examined using spectroscopic methods of UV-visible, Raman, and X-ray photoelectron spectroscopy (XPS). Current and photovoltage measurements for Ln3+-doped SDNA thin films under UV illumination with varying power intensities were conducted. Under UV illumination, the photocurrent and photovoltage of Ln3+-doped SDNA thin films increased with increasing applied external voltages and input power intensities, respectively. In addition, we observed considerable increases in photovoltage responses, i.e., 5-fold increase for Nd3+, 10-fold for Er3+, and 13-fold for Nd3+/ Er3+, compared to the pristine SDNA due to the additional charge carriers generated in Ln3+-doped SDNA thin films. Device performance was measured in terms of photovoltage responsivity and retention characteristics. These phenomena indicate the high stability and substantial endurance characteristics of Ln3+-doped SDNA thin films.

DNA nanostructures doped with lanthanide ions for highly sensitive UV photodetectors.

Deoxyribonucleic acid (DNA) and lanthanide ions (Ln3+) exhibit exceptional optical properties that are applicable to the development of nanoscale devices and sensors. Although DNA nanostructures and Ln3+ ions have been investigated for use in the current state of technology for more than a few decades, researchers have yet to develop DNA and Ln3+ based ultra-violet (UV) photodetectors. Here, we fabricate Ln3+ (such as holmium (Ho3+), praseodymium (Pr3+), and ytterbium (Yb3+))‒doped double crossover (DX)‒DNA lattices through substrate-assisted growth and salmon DNA (SDNA) thin films via a simple drop-casting method on oxygen (O2) plasma-treated substrates for high performance UV photodetectors. Topological (AFM), optical (UV-vis absorption and FTIR), spectroscopic (XPS), and electrical (I‒V and photovoltage) measurements of the DX‒DNA and SDNA thin films doped with various concentrations of Ln3+ ([Ln3+]) are explored. From the AFM analysis, the optimum concentrations of various Ln3+ ([Ln3+]O) are estimated (where the phase transition of Ln3+‒doped DX‒DNA lattices takes place from crystalline to amorphous) as 1.2 mM for Ho3+, 1.5 mM for Pr3+, and 1.5 mM for Yb3+. The binding modes and chemical states are evaluated through optical and spectroscopic analysis. From UV-vis absorption studies, we found that as the [Ln3+] was increased, the absorption intensity decreased up to [Ln3+]O, and increased above [Ln3+]O. The variation in FTIR peak intensities in the nucleobase and phosphate regions, and the changes in XPS peak intensities and peak positions detected in the N 1 s and P 2p core spectra of Ln3+‒doped SDNA thin films clearly indicate that the Ln3+ ions are properly bound between the bases (through chemical intercalation) and to the phosphate backbone (through electrostatic interactions) of the DNA molecules. Finally, the I‒V characteristics and time-dependent photovoltage of Ln3+‒doped SDNA thin films are measured both in the dark and under UV LED illuminations (λLED = 382 nm) at various illumination powers. The photocurrent and photovoltage of Ln3+‒doped SDNA thin films are enhanced up to the [Ln3+]O compared to pristine SDNA due to the charge carriers generated from both SDNA and Ln3+ ions upon the absorption of light. From our observations, the photovoltages as function of illumination power suggest higher responsivities, and the photovoltages as function of time are almost constant which indicates the stability and retention characteristics of the Ln3+‒doped SDNA thin films. Hence, our method which provides an efficient doping of Ln3+ into the SDNA with a simple fabrication process might be useful in the development of high-performance optoelectronic devices and sensors.

A study of the red-shift of a neutral donor bound exciton in GaN nanorods by hydrogenation.

In this paper we account for the physics behind the exciton peak shift in GaN nanorods (NRs) due to hydrogenation. GaN NRs were selectively grown on a patterned Ti/Si(111) substrate using plasma-assisted molecular beam epitaxy, and the effect of hydrogenation on their optical properties was investigated in detail using low-temperature photoluminescence measurements. Due to hydrogenation, the emissions corresponding to the donor-acceptor pair and yellow luminescence in GaN NRs were strongly suppressed, while the emission corresponding to the neutral to donor bound exciton (D0X) exhibited red-shift. Thermal annealing of hydrogenated GaN NRs demonstrated the recovery of the D0X and deep level emission. To determine the nature of the D0X peak shift due to hydrogenation, comparative studies were carried out on various diameters of GaN NRs, which can be controlled by different growth conditions and wet-etching times. Our experimental results reveal that the D0X shift depends on the diameter of the GaN NRs after hydrogenation. The results clearly demonstrate that the hydrogenation leads to band bending of GaN NRs as compensated by hydrogen ions, which causes a red-shift in the D0X emission.