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We have demonstrated a new class of phosphor-free white LEDs with the use of tunnel junction structure in nonpolar core-shell InGaN nanowires. It is confirmed that the tunnel junction based nanowire LEDs can eliminate the use of the resistive p-GaN:Mg contact layer, leading to significantly enhanced hole injection and dramatically reduced voltage loss. The nonpolar core-shell nanowire heterostructure showed the enhanced carrier injection efficiency through the widened shell n-GaN contact area. The TEM analysis verified that the core-shell Al tunnel junction layers were uniformly grown on nonpolar surfaces of the GaN wurtzite crystal nanowire structure. We have also showed the monolithic integration of multiple-color emission on a single chip by using the multiple-stacked tunnel junction core-shell nanowire heterostructure. Compared to the conventional film based quantum well LEDs, the demonstrated nonpolar core-shell tunnel junction nanowire LEDs will be a very promising candidate for future solid-state lighting applications as well as phosphor-free white LEDs.
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Cathodoluminescence (CL) imaging spectroscopy provides two-dimensional optical excitation images of photonic nanostructures with a deep-subwavelength spatial resolution. So far, CL imaging was unable to provide a direct measurement of the excitation and emission probabilities of photonic nanostructures in a spatially resolved manner. Here, we demonstrate that by mapping the cathodoluminescence autocorrelation function g(2) together with the CL spectral distribution the excitation and emission rates can be disentangled at every excitation position. We use InGaN/GaN quantum wells in GaN nanowires with diameters in the range 200-500 nm as a model system to test our new g(2) mapping methodology and find characteristic differences in excitation and emission rates both between wires and within wires. Strong differences in the average CL intensity between the wires are the result of differences in the emission efficiencies. At the highest spatial resolution, intensity variations observed within wires are the result of excitation rates that vary with the nanoscale geometry of the structures. The fact that strong spatial variations observed in the CL intensity are not only uniquely linked to variations in emission efficiency but also linked to excitation efficiency has profound implications for the interpretation of the CL data for nanostructured geometries in general.
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Multicolor single InGaN/GaN dot-in-nanowire light emitting diodes (LEDs) were fabricated on the same substrate using selective area epitaxy. It is observed that the structural and optical properties of InGaN/GaN quantum dots depend critically on nanowire diameters. Photoluminescence emission of single InGaN/GaN dot-in-nanowire structures exhibits a consistent blueshift with increasing nanowire diameter. This is explained by the significantly enhanced indium (In) incorporation for nanowires with small diameters, due to the more dominant contribution for In incorporation from the lateral diffusion of In adatoms. Single InGaN/GaN nanowire LEDs with emission wavelengths across nearly the entire visible spectral were demonstrated on a single chip by varying the nanowire diameters. Such nanowire LEDs also exhibit superior electrical performance, with a turn-on voltage â¼2 V and negligible leakage current under reverse bias. The monolithic integration of full-color LEDs on a single chip, coupled with the capacity to tune light emission characteristics at the single nanowire level, provides an unprecedented approach to realize ultrasmall and efficient projection display, smart lighting, and on-chip spectrometer.
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We report the controlled synthesis of InGaN/GaN multiple quantum well (MQW) uniaxial (c-plane) and coaxial (m-plane) nanowire (NW) heterostructures by metalorganic chemical vapor deposition. Two kinds of heterostructure NW light-emitting diodes (LEDs) have been fabricated: (1) 10 pairs of InGaN/GaN MQW layers in the c-plane on the top of n-GaN NWs where Mg-doped p-GaN NW is axially grown (2) p-GaN/10 pairs of InGaN/GaN shell structure were surrounded by n-GaN core. Here, we discuss a comparative analysis based on the m-plane and the c-plane oriented InGaN/GaN MQW NW arrays. High-resolution transmission electron microscopy studies revealed that the barrier and the well structures of MQW were observed to be substantially clear with regular intervals while the interface regions were extremely sharp. The c-plane and m-plane oriented MQW single NW was utilized for the parallel assembly fabrication of the LEDs via a focused ion beam. The polarization induced effects on the c-plane and m-plane oriented MQW NWs were precisely compared via power dependence electroluminescence. The electrical properties of m-plane NWs exhibited superior characteristics than that of c-plane NWs owing to the absence of piezoelectric polarization fields. According to this study, high-quality m-plane coaxial NWs can be utilized for the realization of high-brightness LEDs.
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We report the growth of high-quality nonpolar (m-plane) and semipolar (r-plane) multiple quantum well (MQW) nanowires (NWs) for high internal quantum efficiency light emitting diodes (LEDs) without polarization. Highly aligned and uniform In(x)Ga(1-x)N/GaN MQW layers are grown coaxially on the {1-100} sidewalls of hexagonal c-axis n-GaN NWs on Si(111) substrates by a pulsed flow metal-organic chemical vapor deposition (MOCVD) technique. The photoluminescence (PL) measurements reveal that the wavelength and intensity of an MQW structure with various pairs (2-20) are very stable and possess composition-dependent emission ranging from 369 to 600 nm. The cathodoluminescence (CL) spectrum of individual In(x)Ga(1-x)N/GaN MQW NW is dominated by band-edge emission at 369 and 440 nm with a relatively homogeneous profile of parallel alignment. High-resolution transmission electron microscopy (HR-TEM) studies of coaxial InxGa1-xN/GaN MQW NWs measured along the [0001] and [2-1-10] zone axes reveal that the grown NWs are uniform with six nonpolar m-plane facets without any dislocations and stacking faults. The p-GaN/In(x)Ga(1-x)N/GaN MQW/n-GaN NW coaxial LEDs show a current rectification with a sharp onset voltage at 2.65 V in the forward bias. The linear enhancement of power output could be attributed to the elimination of piezoelectric fields in the In(x)Ga(1-x)N/GaN MQW active region. The superior performance of coaxial NW LEDs is observed in comparison with that of thin film LEDs. Overall, the feasibility of obtaining low defect and strain free m-plane coaxial NWs using pulsed MOCVD can be utilized for the realization of high-power LEDs without an efficiency droop. These kinds of coaxial NWs are viable high surface area MQW structures which can be used to enhance the efficiency of LEDs.
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Despite the considerable potential of AlGaN-based ultraviolet-B light-emitting diodes (UV-B LEDs) in various applications such as phototherapy, UV curing, plant growth, and analytical technology, their development is still ongoing due to low luminescence efficiency. In this study, we introduced a novel epitaxial growth mechanism to effectively control the height and thickness of AlGaN multiple wells (MWs) on AlGaN nanorod structures using horizontal reactor-based metal-organic chemical vapor deposition (MOCVD). By adjusting the H2 carrier gas flow rate, we could control the growth boundary layer's thickness, successfully separating the AlGaN well and p-AlGaN layer from the substrate. Cathodoluminescence (CL) measurements confirmed the stability of the core-shell AlGaN quantum wells as a highly stable nonpolarized structure, with the wavelength peak remaining almost unchanged under various injection currents. Furthermore, transmission electron microscopy (TEM) provided clear evidence of differentiation, highlighting the distinct formation of the 275 nm AlGaN core and the 295 nm AlGaN shell structure. The developed AlGaN MW structure, characterized by these rectification features, not only demonstrated a significantly improved electroluminescence (EL) peak intensity but also exhibited a much lower leakage current compared to the conventional core-shell AlGaN structure. The newly proposed growth mechanism and advanced nonpolarized core-shell AlGaN structure are expected to serve as excellent alternatives for substantially enhancing the efficiency of the next generation of high-efficiency UV LEDs.
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Long-term societal prosperity depends on addressing the world's energy and environmental problems, and photocatalysis has emerged as a viable remedy. Improving the efficiency of photocatalytic processes is fundamentally achieved by optimizing the effective utilization of solar energy and enhancing the efficient separation of photogenerated charges. It has been demonstrated that the fabrication of III-V semiconductor-based photocatalysts is effective in increasing solar light absorption, long-term stability, large-scale production and promoting charge transfer. This focused review explores on the current developments in III-V semiconductor materials for solar-powered photocatalytic systems. The review explores on various subjects, including the advancement of III-V semiconductors, photocatalytic mechanisms, and their uses in H2 conversion, CO2 reduction, environmental remediation, and photocatalytic oxidation and reduction reactions. In order to design heterostructures, the review delves into basic concepts including solar light absorption and effective charge separation. It also highlights significant advancements in green energy systems for water splitting, emphasizing the significance of establishing eco-friendly systems for CO2 reduction and hydrogen production. The main purpose is to produce hydrogen through sustainable and ecologically friendly energy conversion. The review intends to foster the development of greener and more sustainable energy source by encouraging researchers and developers to focus on practical applications and advancements in solar-powered photocatalysis.
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Intersubband (intraband) transitions allow absorption of photons in the infrared spectral regime, which is essential for IR-photodetector and optical communication applications. Among various technologies, nanodisks embedded in nanowires offer a unique opportunity to be utilized in intraband devices due to the ease of tuning the fundamental parameters such as strain distribution, band energy, and confinement of the active region. Here, we show the transverse electric polarized intraband absorption using InGaN/GaN nanodisks cladded by AlGaN. Fourier transform infrared reflection (FTIR) measurement confirms absorption of normal incident in-plane transverse electric polarized photons in the mid-IR regime (wavelength of ~ 15 µm) at room temperature. The momentum matrix of the nanodisk energy states indicates electron transition from the ground state s into the px or py orbital-like excited states. Furthermore, the absorption characteristics depending on the indium composition and nanowire diameter exhibits tunability of the intraband absorption spectra within the nanodisks. We believe nanodisks embedded nanowires is a promising technology for achieving tunable detection of photons in the IR spectrum.
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In group III-nitride based semiconductor structures, the incorporation of high-indium-composition InGaN has been severely limited by extremely inefficient strain-induced polarization fields and prohibitively large defect densities. So far, there is no clear approach to solve this issue. Here, we have shown a new approach to incorporate high concentrations of indium in the InGaN structure by using a non-polar quasi-quantum dot heterostructure. This unique epitaxial growth was achieved by integrating a 1-dimensional nanowire and a 0-dimensional quantum dot structure using an MOCVD system. The formation of a high-efficiency quantum-sliding heterostructure and high-quality nanowire structure was confirmed by FE-SEM and TEM measurements. Furthermore, it has been suggested that such a quantum-dot structure can dramatically improve radiative recombination through a new sliding bandgap mechanism. We also found that non-polar quantum dots can not only incorporate more indium than conventional multi-quantum well structures grown on the nanowire structure, but also significantly improve crystalline quality. The PL results verified that the wavelength of quantum dots fabricated on the nanowire structure can easily shift up to 913 nm. The first demonstration in the integration of nanowire and quantum dot structures will open a new avenue to break through the limitations of high indium incorporation in photonic semiconductor systems.
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One-dimensional nanowires based on Group III-nitride materials are emerging as one of the most promising structures for applications of light-emitting diodes (LEDs), laser diodes (LDs), solar cells, and photocatalysts. However, leading to the so-called "green gap" in photonics, the fabrication of high concentration indium gallium nitride (InGaN) and long-InGaN structures remains still challenging. In this study, we performed simulations for structural modeling of uniform temperature distribution in a nanowire epitaxy, and have successfully developed high-concentration InGaN and long-InGaN nanowire heterostructures on silicon (Si) substrate using molecular beam epitaxy (MBE) system. From scanning electron microscope (SEM) and transmission electron microscope (TEM) results, it was confirmed that the various doped-InGaN nanowire structures show much higher crystal quality compared to conventional nanowire structures. By introducing a new three-step modulated growth technique, the n-/p-InGaN active regions were greatly increased and the optical properties were also dramatically improved due to reduced phase separation. In addition, a multi-band p-InGaN/GaN heterostructure was successfully fabricated with the core-shell nanowire structures, which enable the emission of light in the entire visible spectral range, and protect the InGaN surface from surface recombination. This paper offers important insight into the design and epitaxial growth of InGaN nanowire heterostructures.
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Surface-emitting semiconductor lasers have been widely used in data communications, sensing, and recently in Face ID and augmented reality glasses. Here, we report the first achievement of an all-epitaxial, distributed Bragg reflector (DBR)-free electrically injected surface-emitting green laser by exploiting the photonic band edge modes formed in dislocation-free gallium nitride nanocrystal arrays, instead of using conventional DBRs. The device operates at ~523 nm and exhibits a threshold current of ~400 A/cm2, which is over one order of magnitude lower compared to previously reported blue laser diodes. Our studies open a new paradigm for developing low-threshold surface-emitting laser diodes from the ultraviolet to the deep visible (~200 to 600 nm), wherein the device performance is no longer limited by the lack of high-quality DBRs, large lattice mismatch, and substrate availability.
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Ternary III-nitride-based nanowires with highly efficient light-emitting properties are essential for a broad range of applications. By using the selective area molecular-beam epitaxy method, InGaN/AlGaN quantum disks (QDs) embedded in hexagonal GaN nanowires were successfully grown. With the help of atomic-scale-resolved transmission electron microscopy and atom probe tomography, atomic ordering and other related structural information, such as crystallography and local chemistry, have been unambiguously revealed to provide unique insights into the exceptionally strong photoluminescence enhancements. A boomerang-shaped InGaN/AlGaN QD was identified, and atomic-level 1 : 1 periodic chemical ordering within the boomerang shaped AlGaN layers along the c-direction was revealed, confirming the preferential site occupation of Al-atoms. This type of growth provides a strong suppression of the quantum-confined Stark effect and is thus likely a very strong contributor to the exceptional properties. This work therefore enables us to directly establish the key structural elements necessary to understand the exceptionally strong emission exhibited by these materials. Optimization of the configurations of QDs could be an alternative design tool for developing various advanced LED device applications with well-designed structure and desirable optical properties.
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This article describes the growth and device characteristics of vertically aligned high-quality uniaxial p-GaN/InxGa1-xN/GaN multiple quantum wells (MQW)/n-GaN nanowires (NWs) on Si(111) substrates grown by metal-organic chemical vapor deposition (MOCVD) technique. The resultant nanowires (NWs), with a diameter of 200-250 nm, have an average length of 2 µm. The feasibility of growing high-quality NWs with well-controlled indium composition MQW structure is demonstrated. These resultant NWs grown on Si(111) substrates were utilized for fabricating vertical-type light-emitting diodes (LEDs). The steep and intense photoluminescence (PL) and cathodoluminescence (CL) spectra are observed, based on the strain-free NWs on Si(111) substrates. High-resolution transmission electron microscopy (HR-TEM) analysis revealed that the MQW NWs are grown along the c-plane with uniform thickness. The current-voltage (I-V) characteristics of these NWs exhibited typical p-n junction LEDs and showed a sharp onset voltage at 2.75 V in the forward bias. The output power is linearly increased with increasing current. The result indicates that the pulsed MOCVD technique is an effective method to grow uniaxial p-GaN/InxGa1-xN/GaN MQW/n-GaN NWs on Si(111), which is more advantageous than other growth techniques, such as molecular beam epitaxy. These results suggest the uniaxial NWs are promising to allow flat-band quantum structures, which can enhance the efficiency of LEDs.