新工艺生长的InGaN量子点的结构与电学性质研究

利用金属有机化学气相沉积（MOCVD）技术，采用一种称为低温钝化的新生和方法成功地生长出多层InGaN/GaN量子点。这种方法是对GaN表面进行钝化并在低温下生长，从而增加表面吸附原子的迁移势垒。采用原子力显微镜清楚地观察到该方法生长的样品中岛状的量子点。从量子点样品的I-V特性曲线观察到了共振隧穿引起的负阻效应，其中的锯齿状峰形归因于零维量子点的共振隧穿。     

Cathodoluminescence study of crystalline quality of (Al, In, Ga)N heterostructures

Wurtzite InGaN/GaN and AlGaN/GaN heterostructures grown by metal organic vapor phase epitaxy were studied using cathodoluminescence (CL) combined with secondary electron microscopy (SEM) and scanning transmission electron microscopy (STEM). The surface morphology of samples containing InGaN layers is dominated by three types of defects: mesa-like hexagonal structures, hexagonal pyramids and micropipes. At the positions of pyramids the whole epilayer is thicker than at defect free positions, while at the positions of micropipes the whole epilayer is much thinner. The luminescence efficiency as well as the emission wavelength are influenced by these defects. In SL structures an increasing SL period thickness in the growth direction was observed. Panchromatic CL images show intensity inhomogeneity in both InGaN/GaN and AlGaN/GaN heterostructure, which are related to local variations of the interface quality. In AlGaN/GaN SQW structures a broad deep-level luminescence band at around 543 nm was observed, which is generally absent in InGaN/GaN heterostructures. This deep-level emission is strongly enhanced in defect positions.     

Growth of InGaN quantum dots with AlGaN barrier layers via modified droplet epitaxy

The growth of c-plane InGaN quantum dots via modified droplet epitaxy with AlGaN barrier layers is reported. The growth of the AlGaN layer underlying the InGaN quantum dot layer was carried out under H₂ at 1050 °C, while the capping AlGaN layer was grown at the same temperature (710 °C) and using the same carrier gas (N₂) as that used to grow the InGaN quantum dot layer to prevent decomposition of the InGaN. Atomic force microscopy of InGaN epilayers grown and annealed on high temperature AlGaN using identical growth conditions used for the quantum dot samples highlighted a narrower distribution of nanostructure heights than that obtained for similar growth on GaN. Scanning transmission electron microscopy (STEM) imaging combined with energy dispersive X-ray (EDX) analysis revealed the presence of a thin high aluminium content layer at the surface of both AlGaN layers, which is believed to be related to loss of Ga during temperature ramping processes. Micro-photoluminescence studies carried out at low temperature revealed near resolution-limited peaks while time-resolved measurements on these peaks demonstrated mono-exponential decay times between 1 and 4 ns, showing that quantum dots had successfully been formed between the AlGaN barriers. Temperature-dependant measurement of the emission lines revealed that quenching of the peak often occurred at ∼60–70 K, with some of the peaks exhibiting significant line broadening whilst others remained narrow.     

Full-color InGaN/GaN dot-in-a-wire light emitting diodes on silicon

We report on the achievement of a new class of nanowire light emitting diodes (LEDs), incorporating InGaN/GaN dot-in-a-wire nanoscale heterostructures grown directly on Si(111) substrates. Strong emission across nearly the entire visible wavelength range can be realized by varying the dot composition. Moreover, we have demonstrated phosphor-free white LEDs by controlling the indium content in the dots in a single epitaxial growth step. Such devices can exhibit relatively high internal quantum efficiency (>20%) and no apparent efficiency droop for current densities up to ~ 200 A cm(-2).     

Electrically driven quantum dot/wire/well hybrid light-emitting diodes

Electrically driven quantum dot, wire, and well hybrid light-emitting diodes are demonstrated by using nanometer-sized pyramid structures of GaN. InGaN quantum dots, wires, and wells are formed at the tops, edges, and sidewalls of pyramids, respectively. The hybrid light-emitting diodes containing low-dimensional quantum structures are good candidates for broad-band highly efficient visible lighting sources.     

Investigations of selectively grown GaN/InGaN epitaxial layers

We have studied GaN/InGaN heterostructures grown by selective area low pressure metalorganic vapor phase epitaxy (LP-MOVPE). A GaN layer already grown on the c-face of sapphire has been used as substrate, partly masked by SiO₂. In a second epitaxial step a GaN/InGaN single heterostructure and GaN/InGaN/GaN double heterostructures were grown on the unmasked rectangular fields. We obtained good selectivity for GaN and for InGaN. A larger growth rate as compared to planar epitaxy and strong growth enhancement at the edges was observed. Spatially resolved measurements of the luminescence show an increase in indium incorporation of about 80% at the edges. Besides the larger indium offering at the edges, this is due to an enhanced growth rate. Very smooth facets are obtained. The influence of pressure on the surface morphology and growth enhancement was investigated.     

p-Type modulation doped InGaN/GaN dot-in-a-wire white-light-emitting diodes monolithically grown on Si(111)

Full-color, catalyst-free InGaN/GaN dot-in-a-wire light-emitting diodes (LEDs) were monolithically grown on Si(111) by molecular beam epitaxy, with the emission characteristics controlled by the dot properties in a single epitaxial growth step. With the use of p-type modulation doping in the dot-in-a-wire heterostructures, we have demonstrated the most efficient phosphor-free white LEDs ever reported, which exhibit an internal quantum efficiency of ～56.8%, nearly unaltered CIE chromaticity coordinates with increasing injection current, and virtually zero efficiency droop at current densities up to ～640 A/cm(2). The remarkable performance is attributed to the superior three-dimensional carrier confinement provided by the electronically coupled dot-in-a-wire heterostructures, the nearly defect- and strain-free GaN nanowires, and the significantly enhanced hole transport due to the p-type modulation doping.     

Multi-quantum-well nanowire heterostructures for wavelength-controlled lasers

Rational design and synthesis of nanowires with increasingly complex structures can yield enhanced and/or novel electronic and photonic functions. For example, Ge/Si core/shell nanowires have exhibited substantially higher performance as field-effect transistors and low-temperature quantum devices compared with homogeneous materials, and nano-roughened Si nanowires were recently shown to have an unusually high thermoelectric figure of merit. Here, we report the first multi-quantum-well (MQW) core/shell nanowire heterostructures based on well-defined III-nitride materials that enable lasing over a broad range of wavelengths at room temperature. Transmission electron microscopy studies show that the triangular GaN nanowire cores enable epitaxial and dislocation-free growth of highly uniform (InGaN/GaN)n quantum wells with n=3, 13 and 26 and InGaN well thicknesses of 1-3 nm. Optical excitation of individual MQW nanowire structures yielded lasing with InGaN quantum-well composition-dependent emission from 365 to 494 nm, and threshold dependent on quantum well number, n. Our work demonstrates a new level of complexity in nanowire structures, which potentially can yield free-standing injection nanolasers.     

Structural and optical properties of InGaN/GaN nanowire heterostructures grown by PA-MBE

The structural and optical properties of InGaN/GaN nanowire heterostructures grown by plasma-assisted molecular beam epitaxy have been studied using a combination of transmission electron microscopy, electron tomography and photoluminescence spectroscopy. It is found that, depending on In content, the strain relaxation of InGaN may be elastic or plastic. Elastic relaxation results in a pronounced radial In content gradient. Plastic relaxation is associated with the formation of misfit dislocations at the InGaN/GaN interface or with cracks in the InGaN nanowire section. In all cases, a GaN shell was formed around the InGaN core, which is assigned to differences in In and Ga diffusion mean free paths.     

MBE grown InGaN quantum dots and quantum wells: effects of in-plane localization

InGaN/GaN heterostructure samples were grown by molecular beam epitaxy using ammonia as a nitrogen precursor. The growth of InGaN/GaN self-assembled quantum dots was monitored in situ by reflection high energy electron diffraction intensity oscillations. Atomic force microscopy scans showed a very high density of InGaN islands, 1×10¹¹ cm⁻², well above the dislocation density. This could explain the increased radiative efficiency of these samples compared to homogeneous quantum wells. Light emitting diodes (LEDs) with InGaN active layers buried in GaN were realized. Electroluminescence and photocurrent spectra of these LEDs evidence a strong Stokes shift that can be attributed to high localization of carriers in InGaN layers.     

White emission by self-regulated growth of InGaN/GaN quantum wells on in situ self-organized faceted n-GaN islands

The in situ self-organization of three-dimensional n-GaN islands of distinct sidewall faceting was realized by initial low V/III ratio growth under high reactor pressure followed by variations of the V/III ratio and reactor pressure. The naturally formed faceted islands with top and sidewall facets of various specific polar angles may serve as an ideal template for self-regulated growth of the InGaN/GaN multiple quantum wells (MQWs), i.e. the growth behavior is specific polar angle dependent. Further, the growth behavior and luminescence properties of the InGaN/GaN MQWs on various facets of different specific polar angles are directly compared and discussed. Tetrachromatic white emissions (blue, cyan, green, and red) from single-chip phosphor-free InGaN/GaN MQWs are realized by color tuning through island shaping, shape variations, and self-regulated growth of the InGaN/GaN MQWs.     

A Ge/Si heterostructure nanowire-based double quantum dot with integrated charge sensor

One proposal for a solid-state-based quantum bit (qubit) is to control coupled electron spins on adjacent semiconductor quantum dots. Most experiments have focused on quantum dots made from III-V semiconductors; however, the coherence of electron spins in these materials is limited by hyperfine interactions with nuclear spins. Ge/Si core/shell nanowires seem ideally suited to overcome this limitation, because the most abundant nuclei in Ge and Si have spin zero and the nanowires can be chemically synthesized defect-free with tunable properties. Here, we present a double quantum dot based on Ge/Si nanowires in which we can completely control the coupling between the dots and to the leads. We also demonstrate that charge on the double dot can be detected by coupling it capacitively to an adjacent nanowire quantum dot. The double quantum dot and integrated charge sensor serve as an essential building block to form a solid-state qubit free of nuclear spin.     

Study on modulating the indium composition in InGaN quantum wells to improve the luminous efficiency of GaN LED

This study primarily used metal-organic chemical vapor deposition to grow gallium nitride (GaN) light-emitting diode (LED) structures with InGaN quantum wells (QWs). During the InGaN QW growing process, an identical concentration of trimethylindium gas was prepared and introduced at different times (Before(B), Middle(M), and After(A)) into the QW structures for an investigation of the variation in GaN LED luminous efficacy. Because of segregation resulting from the different concentrations of In content of the InGaN QWs during the process and because of the stress resulting from lattice mismatch between atoms, the interaction between segregation and stress forms quantum dots (QDs). Under processes with the appropriate parameters, the QDs can improve the luminous efficacy of GaN LEDs. Postprocess LEDs were measured for their electroluminescence, photoluminescence, cathodoluminescence, thermal stability, light output power, and external quantum efficiency. The QW structures were analyzed and observed using high-resolution transmission electron microscopy. The results revealed that the Before (B) LED had the greatest light output power at 46.6 mW, an increase of approximately 15.6%. Thermal annealing was then used to treat the LED at 850 °C, after which the photoluminescence intensity increased by 1.7 times.

     

Photonic crystal-assisted light extraction from a colloidal quantum dot/GaN hybrid structure

We present a study of the light extraction from CdSe/ZnS core/shell colloidal quantum dot thin films deposited on quantum well InGaN/GaN photonic crystal structures. The two-dimensional photonic crystal defined by nanoimprint lithography is used to efficiently extract the guided light modes originating from both the quantum dot thin films and the InGaN quantum wells. Far-field photoluminescence spectra are used to measure the extraction enhancement factor of the quantum dot emission (x1.4). Microphotoluminescence measurements show that the guided mode effective extraction lengths range between 70 and 180 microm, depending on the wavelength of light.     

Multi-wavelength emitting InGan/GaN quantum well grown on V-shaped gan(1101) microfacet

InGaN/GaN multiple quantum wells (MQWs) were successfully grown on the inclined GaN(1101) microfacets. Conventional photolithography and subsequent growth of GaN were employed to generate the V-shaped microfacets along (1120) direction. The well-developed microfacets observed by scanning electron microscopy and the clear transmission electron microscope interfacial images indicated that the MQW was successfully grown on the GaN microfacets. Interestingly, cathodoluminescence (CL) spectra measured on the microfacets showed a continuous change in the luminescence peak positions. The CL peaks were shifted to a longer wavelength from 420 nm to 440 nm as the probing points were changed along upward direction. This could be attributed to the nonuniform distribution of the In composition and/or the wavefunction overlapping between adjacent wells. Present works thus propose a novel route to fabricate a monolithic white light emitting diode without phosphors by growing the InGaN/GaN MQWs on (1101) facet.     

Interplay of confinement, strain, and piezoelectric effects in the optical spectrum of GaN quantum dots

We theoretically investigated excitonic states, energy and oscillator strength of optical transitions in GaN quantum dots characterized by different size, shape, interface, and substrate. On the basis of our multi-band model we determined that the piezoelectric field-induced red shift of the ground state transition, observed in recent experiments, can manifest itself only in strained GaN/AIN dots with the dot height larger than 3 nm. It was also established that the oscillator strength of the red-shifted transitions is small (< 0.05) and decreases fast with increasing the dot size, while the strength of ground state transitions in c-GaN/c-AIN and GaN/dielectric dots is large (approximately 0.4-0.7) and almost independent of the dot size.     

Investigation of V-defects formation in InGaN/GaN multiple quantum well grown on sapphire

In the growth of InGaN multiple quantum well structure, V-pits has been observed to be initiated at the threading dislocations which propagate to the quantum well layers with high indium composition and substantially thick InGaN well. A set of samples with varying indium well thickness (3-7.6 nm) and composition (10-30%) are grown and characterized by photoluminescence (PL), X-ray diffraction, transmission electron microscopy and atomic force microscopy. The indium content and the layer thicknesses in InGaN/GaN quantum well are determined by high-resolution X-ray diffraction (XRD) and TEM imaging. With indium composition exceeding 10%, strain at the InGaN/GaN interface leads to the generation of V-pits at the interlayers of the MQW. Higher indium composition and increase in thickness of a period (InGaN well plus the GaN barrier) appear to enhance pits generation. With thicker InGaN well and reduction in thickness of GaN to InGaN (or the R ratio), pit density is substantially reduced, but it results in greater inhomogeneity in the distribution of indium in the InGaN well. This leads to a broadened PL emission and affect the PL emission intensity.     

Luminescence and lasing in GaN epitaxial layers and InGaN/GaN quantum well heterostructures under optical and electron-beam excitation

Interrelation between stimulated and excitonic emission intensity of GaN epitaxial layers and yellow luminescence intensity as well as correlation between photoluminescence and laser properties of InGaN based multiple quantum well heterostructures was investigated. It was found among all studied undoped GaN epitaxial layers that the higher intensity of the yellow luminescence and so the higher concentration of the yellow luminescence related centres the higher is the excitonic, electron–hole plasma and stimulated emission intensity. It was shown that a small Stokes shift and a high ratio of the luminescence intensity from InGaN quantum well layers to the photoluminescence intensity from GaN barrier layers indicate high laser quality of the multiple quantum well heterostructures. The lowest full width at half maximum of the laser line was 0.04 nm, the highest operating temperature was 585 K, the lowest threshold was 100 kW cm⁻², the highest characteristic temperature was 164 K and the highest wavelength was 442.5 nm. The far-field patterns of the laser emission from the MQW lasers consist of two approximately symmetrical high brightness spots localized at angles =±30–35°.     

Semiconductor Nanowire Light‐Emitting Diodes Grown on Metal: A Direction Toward Large‐Scale Fabrication of Nanowire Devices

Bottom‐up nanowires are attractive for realizing semiconductor devices with extreme heterostructures because strain relaxation through the nanowire sidewalls allows the combination of highly lattice mismatched materials without creating dislocations. The resulting nanowires are used to fabricate light‐emitting diodes (LEDs), lasers, solar cells, and sensors. However, expensive single crystalline substrates are commonly used as substrates for nanowire heterostructures as well as for epitaxial devices, which limits the manufacturability of nanowire devices. Here, nanowire LEDs directly grown and electrically integrated on metal are demonstrated. Optical and structural measurements reveal high‐quality, vertically aligned GaN nanowires on molybdenum and titanium films. Transmission electron microscopy confirms the composition variation in the polarization‐graded AlGaN nanowire LEDs. Blue to green electroluminescence is observed from InGaN quantum well active regions, while GaN active regions exhibit ultraviolet emission. These results demonstrate a pathway for large‐scale fabrication of solid state lighting and optoelectronics on metal foils or sheets.     

Auger recombination in III-nitride nanowires and its effect on nanowire light-emitting diode characteristics

We have measured the Auger recombination coefficients in defect-free InGaN nanowires (NW) and InGaN/GaN dot-in-nanowire (DNW) samples grown on (001) silicon by plasma-assisted molecular beam epitaxy. The nanowires have a density of ～1 × 10(11) cm(-2) and exhibit photoluminescence emission peak at λ ～ 500 nm. The Auger coefficients as a function of excitation power have been derived from excitation dependent and time-resolved photoluminescence measurements over a wide range of optical excitation power density. The values of C(0), defined as the Auger coefficient at low excitation, are 6.1 × 10(-32) and 4.1 × 10(-33) cm(6)·s(-1) in the NW and DNW samples, respectively, which are in reasonably good agreement with theoretical predictions for InGaN alloy semiconductors. Light-emitting diodes made with the NW and DNW samples exhibit no efficiency droop up to an injection current density of 400 A/cm(2).