Internal quantum efficiency of AlGaN/AlN quantum dot superlattices for electron-pumped ultraviolet sources.

In this paper, we describe the growth and characterization of ≈530 nm thick superlattices (100 periods) of AlxGa1-xN/AlN (0 ⩽ x ⩽ 0.1) Stranski-Krastanov quantum dots (QDs) for application as the active region of electron-beam pumped ultraviolet lamps. Highly dense (>1011 cm-2) QD layers are deposited by molecular beam epitaxy, and we explore the effect of the III/V ratio during the growth process on their optical performance. The study considers structures emitting in the 244-335 nm range at room temperature, with a relative linewidth in the 6%-11% range, mainly due to the QD diameter dispersion inherent in self-assembled growth. Under electron pumping, the emission efficiency remains constant for acceleration voltages below ≈9 kV. The correlation of this threshold with the total thickness of the SL and the penetration depth of the electron beam confirms the homogeneity of the nanostructures along the growth axis. Below the threshold, the emission intensity scales linearly with the injected current. The internal quantum efficiency (IQE) is characterized at low injection, which reveals the material properties in terms of non-radiative processes, and high injection, which emulates carrier injection in operation conditions. In QDs synthesized with III/V ratio <0.75, the IQE remains around 50% from low injection to pumping power densities as high as 200 kW cm-2, being the first kind of nanostructure that present such stable behaviour.

Controlling the shape of a tapered nanowire: lessons from the Burton-Cabrera-Frank model.

The propagation of sidewall steps during the growth of nanowires is calculated in the frame of the Burton-Cabrera-Frank model. The stable shape of the nanowire comprises a cylinder section on top of a cone section: their characteristics are obtained as a function of the radius of the catalyst-nanowire area, the desorption-limited diffusion length of adatoms on the terraces, and the sticking of adatoms at step edges. The comparison with experimental data allows us to evaluate these last two parameters for InP and ZnTe nanowires; it reveals a different behavior for the two materials, related to a difference by an order of magnitude of the desorption-limited diffusion length.

Assessment of AlGaN/AlN superlattices on GaN nanowires as active region of electron-pumped ultraviolet sources.

In this paper, we describe the design and characterization of 400 nm long (88 periods) Al x Ga1-x N/AlN (0 ≤ x ≤ 0.1) quantum dot superlattices deposited on self-assembled GaN nanowires for application in electron-pumped ultraviolet sources. The optical performance of GaN/AlN superlattices on nanowires is compared with the emission of planar GaN/AlN superlattices with the same periodicity and thickness grown on bulk GaN substrates along the N-polar and metal-polar crystallographic axes. The nanowire samples are less sensitive to nonradiative recombination than planar layers, attaining internal quantum efficiencies (IQE) in excess of 60% at room temperature even under low injection conditions. The IQE remains stable for higher excitation power densities, up to 50 kW cm-2. We demonstrate that the nanowire superlattice is long enough to collect the electron-hole pairs generated by an electron beam with an acceleration voltage V A = 5 kV. At such V A, the light emitted from the nanowire ensemble does not show any sign of quenching under constant electron beam excitation (tested for an excitation power density around 8 kW cm-2 over the scale of minutes). Varying the dot/barrier thickness ratio and the Al content in the dots, the nanowire peak emission can be tuned in the range from 340 to 258 nm.

Impact of kinetics on the growth of GaN on graphene by plasma-assisted molecular beam epitaxy.

The growth of GaN on graphene by molecular beam epitaxy was investigated. The most stable epitaxial relationship, i.e. [00.1]-oriented grains, is obtained at high temperature and N-rich conditions, which match those for nanowire growth. Alternatively, at moderate temperature and Ga-rich conditions, several metastable orientations are observed at the nucleation stage, which evolve preferentially towards [00.1]-oriented grains. The dependence of the nucleation regime on growth conditions was assigned to Ga adatom kinetics. This statement is consistent with the calculated graphene/GaN in-plane lattice coincidence and supported by a combination of transmission electron microscopy, x-ray diffraction, photoluminescence, and Raman spectroscopy experiments.

Effect of doping on the far-infrared intersubband transitions in nonpolar m-plane GaN/AlGaN heterostructures.

This paper assesses the effects of Si doping on the properties of nonpolar m-plane GaN/AlGaN quantum wells (QWs) designed for intersubband (ISB) absorption in the far-infrared spectral range. For doping levels up to 3 × 10(12) cm(-2), structural analysis reveals uniform QWs with abrupt interfaces and no epitaxially induced defects. Cathodoluminescence spectroscopy confirms the homogeneity of the multiple QWs along the growth direction. Increasing the doping density in the QWs from 1 × 10(11) cm(-2) to 3 × 10(12) cm(-2) induces a broadening of the photoluminescence as well as a reduction of the exciton localization energy in the alloy. Also, enhancement of the ISB absorption is observed, along with a blue shift and widening of the absorption peak. The magnitude of the ISB absorption saturates for doping levels around 1 × 10(12) cm(-2), and the blue shift and broadening increase less than theoretically predicted for the samples with higher doping levels. This is explained by the presence of free carriers in the excited electron level due to the increase of the Fermi level energy.

Interfacial chemistry in a ZnTe/CdSe superlattice studied by atom probe tomography and transmission electron microscopy strain measurements.

The atomic scale analysis of a ZnTe/CdSe superlattice grown by molecular beam epitaxy is reported using atom probe tomography and strain measurements from high-resolution scanning transmission electron microscopy images. CdTe interfaces were grown by atomic layer epitaxy to prevent the spontaneous formation of ZnSe bonds. Both interfaces between ZnTe and CdSe are composed of alloyed layers of ZnSe. Pure CdTe interfaces are not observed and Zn atoms are also visible in the CdSe layers. This information is critical to design superlattices with the expected optoelectronic properties.

Nonpolar m-plane GaN/AlGaN heterostructures with intersubband transitions in the 5-10 THz band.

This paper assesses intersubband (ISB) transitions in the 1-10 THz frequency range in nonpolar m-plane GaN/AlGaN multi-quantum-wells deposited on free-standing semi-insulating GaN substrates. The quantum wells (QWs) were designed to contain two confined electronic levels, decoupled from the neighboring wells. Structural analysis reveals flat and regular QWs in the two perpendicular in-plane directions, with high-angle annular dark-field scanning transmission electron microscopy images showing inhomogeneities of the Al composition in the barriers along the growth axis. We do not observe extended structural defects (stacking faults or dislocations) introduced by the epitaxial process. Low-temperature ISB absorption from 1.5 to 9 THz (6.3-37.4 meV) is demonstrated, covering most of the 7-10 THz band forbidden to GaAs-based technologies.

Investigation of Photovoltaic Properties of Single Core-Shell GaN/InGaN Wires.

We report the investigation of the photovoltaic properties of core-shell GaN/InGaN wires. The radial structure is grown on m-plane {11̅00} facets of self-assembled c̅-axis GaN wires elaborated by metal-organic vapor phase epitaxy (MOVPE) on sapphire substrates. The conversion efficiency of wires with radial shell composed of thick In0.1Ga0.9N layers and of 30× In0.18Ga0.82N/GaN quantum wells are compared. We also investigate the impact of the contact nature and layout on the carrier collection and photovoltaic performances. The contact optimization results in an improved conversion efficiency of 0.33% and a fill factor of 83% under 1 sun (AM1.5G) on single wires with a quantum well-based active region. Photocurrent spectroscopy demonstrates that the response ascribed to the absorption of InGaN/GaN quantum wells appears at wavelengths shorter than 440 nm.

Probing alloy composition gradient and nanometer-scale carrier localization in single AlGaN nanowires by nanocathodoluminescence.

The optical properties of single AlGaN nanowires grown by plasma-assisted molecular beam epitaxy have been studied by nanocathodoluminescence. Optical emission was found to be position-dependent and to occur in a wide wavelength range, a feature which has been assigned to a composition gradient along the nanowire growth axis, superimposed on local composition fluctuations at the nanometer scale. This behavior is associated with the growth mode of such AlGaN nanowires, which is governed by kinetics, leading to the successive formation of (i) a zone with strong local composition fluctuations followed by (ii) a zone with a marked composition gradient and, eventually, (iii) a zone corresponding to a steady state regime and the formation of a homogeneous alloy.

Growth, structural and optical properties of AlGaN nanowires in the whole composition range.

We report on the growth of AlxGa1-xN nanowires by plasma-assisted molecular beam epitaxy for x in the 0.3-0.8 range. Based on a combination of macro- and micro-photoluminescence, Raman spectroscopy, x-ray diffraction and scanning electron microscopy experiments, it is shown that the structural and optical properties of AlGaN NWs are governed by the presence of compositional fluctuations associated with strongly localized electronic states. A growth model is proposed, which suggests that, depending on growth temperature and metal adatom density, macroscopic composition fluctuations are mostly of kinetic origin and are directly related to the nucleation of the AlGaN nanowire section on top of the GaN nanowire base which is used as a substrate.

Catalyst-assisted hydride vapor phase epitaxy of GaN nanowires: exceptional length and constant rod-like shape capability.

The hydride vapor phase epitaxy (HVPE) process exhibits unexpected properties when growing GaN semiconductor nanowires (NWs). With respect to the classical well-known methods such as metal organic vapor phase epitaxy and molecular beam epitaxy, this near-equilibrium process based on hot wall reactor technology enables the synthesis of nanowires with a constant cylinder shape over unusual length. Catalyst-assisted HVPE shows a record short time process (less than 20 min) coupled to very low precursor consumption. NWs are grown at a fast solidification rate (50 µm h(-1)), facilitated by the high decomposition frequency of the chloride molecules involved in the HVPE process as element III precursors. In this work growth temperature and V/III ratio were investigated to determine the growth mechanism which led to such long NWs. Analysis based on the Ni-Ga phase diagram and the growth kinetics of near-equilibrium HVPE is proposed.

Ultrafast room temperature single-photon source from nanowire-quantum dots.

Epitaxial semiconductor quantum dots are particularly promising as realistic single-photon sources for their compatibility with manufacturing techniques and possibility to be implemented in compact devices. Here, we demonstrate for the first time single-photon emission up to room temperature from an epitaxial quantum dot inserted in a nanowire, namely a CdSe slice in a ZnSe nanowire. The exciton and biexciton lines can still be resolved at room temperature and the biexciton turns out to be the most appropriate transition for single-photon emission due to a large nonradiative decay of the bright exciton to dark exciton states. With an intrinsically short radiative decay time (≈300 ps) this system is the fastest room temperature single-photon emitter, allowing potentially gigahertz repetition rates.

Growth mechanism and properties of InGaN insertions in GaN nanowires.

We demonstrate the strong influence of strain on the morphology and In content of InGaN insertions in GaN nanowires, in agreement with theoretical predictions which establish that InGaN island nucleation on GaN nanowires may be energetically favorable, depending on In content and nanowire diameter. EDX analyses reveal In inhomogeneities between the successive dots but also along the growth direction within each dot, which is attributed to compositional pulling. Nanometer-resolved cathodoluminescence on single nanowires allowed us to probe the luminescence of single dots, revealing enhanced luminescence from the high In content top part with respect to the lower In content dot base.

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.

The structural properties of GaN/AlN core-shell nanocolumn heterostructures.

The growth and structural properties of GaN/AlN core-shell nanowire heterostructures have been studied using a combination of resonant x-ray diffraction, Raman spectroscopy and high resolution transmission electron microscopy experiments. For a GaN core of 20 nm diameter on average surrounded by a homogeneous AlN shell, the built-in strain in GaN is found to agree with theoretical calculations performed using a valence force field model. It is then concluded that for an AlN thickness up to at least 12 nm both core and shell are in elastic equilibrium. However, in the case of an inhomogeneous growth of the AlN shell caused by the presence of steps on the sides of the GaN core, plastic relaxation is found to occur. Consistent with the presence of dislocations at the GaN/AlN interface, it is proposed that this plastic relaxation, especially efficient for AlN shell thickness above 3 nm, is promoted by the shear strain induced by the AlN inhomogeneity.

Quantum transport in GaN/AlN double-barrier heterostructure nanowires.

We investigate electronic transport in n-i-n GaN nanowires with and without AlN double barriers. The nanowires are grown by catalyst-free, plasma-assisted molecular beam epitaxy enabling abrupt GaN/AlN interfaces as well as longitudinal n-type doping modulation. At low temperature, transport in n-i-n GaN nanowires is dominated by the Coulomb blockade effect. Carriers are confined in the undoped middle region, forming single or multiple islands with a characteristic length of approximately 100 nm. The incorporation of two AlN tunnel barriers causes confinement to occur within the GaN dot in between. In the case of a 6 nm thick dot and 2 nm thick barriers, we observe characteristic signatures of Coulomb-blockaded transport in single quantum dots with discrete energy states. For thinner dots and barriers, Coulomb-blockade effects do not play a significant role while the onset of resonant tunneling via the confined quantum levels is accompanied by a negative differential resistance surviving up to approximately 150 K.

Nucleation mechanism of GaN nanowires grown on (111) Si by molecular beam epitaxy.

We have performed a real-time in situ x-ray scattering study of the nucleation of GaN nanowires grown by plasma-assisted molecular beam epitaxy on AlN(0001)/Si(111). The intensity variation of the GaN diffraction peak as a function of time was found to exhibit three different regimes: (i) the deposition of a wetting layer, which is followed by (ii) a supralinear regime assigned to nucleation of almost fully relaxed GaN nanowires, eventually leading to (iii) a steady-state growth regime. Based on scanning electron microscopy and electron microscopy analysis, it is proposed that the granular character of the thin AlN buffer layer may account for the easy plastic relaxation of GaN, establishing that three-dimensional islanding and plastic strain relaxation of GaN are two necessary conditions for nanowire growth.

The structural properties of GaN insertions in GaN/AlN nanocolumn heterostructures.

The strain state of 1 and 2.5 nm thick GaN insertions in GaN/AlN nanocolumn heterostructures has been studied by means of a combination of high resolution transmission electron microscopy, Raman spectroscopy and theoretical modeling. It is found that 2.5 nm thick GaN insertions are partially relaxed, which has been attributed to the presence of dislocations in the external AlN capping layer, in close relationship with the morphology of GaN insertions and with the AlN capping mechanism. The observed plastic relaxation in AlN is consistent with the small critical thickness expected for GaN/AlN radial heterostructures.

CdSe quantum dot formation: alternative paths to relaxation of a strained CdSe layer and influence of the capping conditions.

CdSe/ZnSe quantum dot formation is investigated by studying different steps of the growth. To precisely control the critical thickness of CdSe grown on a ZnSe buffer layer, the CdSe self-regulated growth rate in atomic layer epitaxy growth mode is determined by reflection high-energy electron diffraction (RHEED) measurements for a temperature range between 180 and 280 °C. Then, the two-dimensional-three-dimensional (2D-3D) transition of a strained CdSe layer on (001)-ZnSe induced by the use of amorphous selenium is studied. The formation of CdSe islands is found when 3 monolayers (ML) of CdSe are deposited. When only 2.5 ML of CdSe are deposited, another relaxation mechanism is observed, leading to the appearance of strong undulations on the surface. We also studied the evolution of the surface morphology when 2.7 ML are deposited, to study the boundary between those two phenomena. The influence of capping on quantum dot morphology is investigated. It is found that cadmium is redistributed within the layer during capping. Our results show that the cadmium distribution after capping depends on the capping temperature and on the strain of the CdSe layer. Cadmium incorporation after capping is also studied. It is found that the amount of incorporated cadmium depends on the strain of the CdSe layer before capping.