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Using low-temperature cathodoluminescence spectroscopy, we study the properties of N- and Al-polar AlN layers grown by molecular beam epitaxy on bulk AlN{0001}. Compared to the bulk AlN substrate, layers of both polarities feature a suppression of deep-level luminescence, a total absence of the prevalent donor with an exciton binding energy of 28 meV, and a much increased intensity of the emission from free excitons. The dominant donor in these layers is characterized by an associated exciton binding energy of 13 meV. The observation of excited exciton states up to the exciton continuum allows us to directly extract the $\Gamma_{5}$ free exciton binding energy of 57 meV.

An accurate knowledge of the optical constants (refractive index $n$ and extinction coefficient $k$) of ScN is crucial for understanding the optical properties of this binary nitride semiconductor as well as for its use in optoelectronic applications. Using spectroscopic ellipsometry in a spectral range from far infrared to far ultraviolet (0.045-8.5 eV), we determine $n$ and $k$ of ScN layers grown on Al$_{2}$O$_{3}$(0001) substrates by plasma-assisted molecular beam epitaxy. Fits of ellipsometry data return the energies of four oscillators representing critical points in the band structure of ScN, namely, 2.03, 3.89, 5.33, and 6.95 eV. As the infrared range is dominated by free carriers, the vibrational properties of the layers are examined by Raman spectroscopy. Despite the rocksalt structure of ScN, several first-order phonon modes are observed, suggesting a high density of point defects consistent with the high electron density deduced from Hall measurements. Finally, photoluminescence measurements reveal an emission band slightly above the lowest direct bandgap. We attribute the redshift of the peak emission energy from 2.3 to 2.2 eV with increasing layer thickness to a reduction of the O concentration in the layers.

We study the molecular beam epitaxy of AlN nanowires between 950 and 1215 {\deg}C, well above the usual growth temperatures, to identify optimal growth conditions. The nanowires are grown by self-assembly on TiN(111) films sputtered onto Al$_2$O$_3$. Above 1100 {\deg}C, the TiN film is seen to undergo grain growth and its surface exhibits {111} facets where AlN nucleation preferentially occurs. Modelling of the nanowire elongation rate measured at different temperatures shows that the Al adatom diffusion length is maximised at 1150 {\deg}C, which appears to be the optimum growth temperature. However, analysis of the nanowire luminescence shows a steep increase in the deep-level signal already above 1050 {\deg}C, associated with O incorporation from the Al$_2$O$_3$ substrate. Comparison with AlN nanowires grown on Si, MgO and SiC substrates suggests that heavy doping of Si and O by interdiffusion from the TiN/substrate interface increases the nanowire internal quantum efficiency, presumably due to the formation of a SiN$_x$ or AlO$_x$ passivation shell. The outdiffusion of Si and O would also cause the formation of the inversion domains observed in the nanowires. It follows that for optoelectronic and piezoelectric applications, optimal AlN nanowire ensembles should be prepared at 1150 {\deg}C on TiN/SiC substrates and will require an ex situ surface passivation., Comment: Main Paper: 13 pages, 5 figures Supporting Information: 4 pages, 4 figures

Capitalizing on the directed nature of the atomic fluxes in molecular beam epitaxy, we propose and demonstrate the sequential directional deposition of lateral (In,Ga)N shells on GaN nanowires. In this approach, a sub-monolayer thickness of each constituent atomic species, i.e. Ga, In, and N, is deposited subsequently from the same direction by rotating the sample and operating the shutters accordingly. Using multiple iterations of this process, we achieve the growth of homogeneous shells on a single side facet of the nanowires. For higher In content and thus lattice mismatch, we observe a strain-induced bending of the nanowire heterostructures. The incorporation of In and the resulting emission spectra are systematically investigated as a function of both the growth temperature and the In/Ga flux ratio.

Using molecular beam epitaxy, we demonstrate the growth of (In,Ga)N shells emitting in the green spectral range around very thin (35 nm diameter) GaN core nanowires. These GaN nanowires are obtained by self-assembled growth on TiN. We present a qualitative shell growth model accounting for both the three-dimensional nature of the nanostructures as well as the directionality of the atomic fluxes. This model allows us, on the one hand, to optimise the conditions for high and homogeneous In incorporation and, on the other hand, to explain the influence of changes in the growth conditions on the sample morphology and In content. Specifically, the impact of the V/III and In/Ga flux ratios, the rotation speed and the rotation direction are investigated. Notably, with In acting as surfactant, the ternary (In,Ga)N shells are much more homogeneous in thickness along the NW length than their binary GaN counterparts.

GaAs-based nanowires are among the most promising candidates for realizing a monolithical integration of III-V optoelectronics on the Si platform. To realize their full potential for applications as light absorbers and emitters, it is crucial to understand their interaction with light governing the absorption and extraction efficiency, as well as the carrier recombination dynamics determining the radiative efficiency. Here, we study the spontaneous emission of zincblende GaAs/(Al,Ga)As core/shell nanowire arrays by $\mu$-photoluminescence spectroscopy. These ordered arrays are synthesized on patterned Si(111) substrates using molecular beam epitaxy, and exhibit an exceptionally low degree of polytypism for interwire separations exceeding a critical value. We record emission spectra over more than five orders of excitation density for both steady-state and pulsed excitation to identify the nature of the recombination channels. An abrupt Mott transition from excitonic to electron-hole-plasma recombination is observed, and the corresponding Mott density is derived. Combining these experiments with simulations and additional direct measurements of the external quantum efficiency using a perfect diffuse reflector as reference, we are able to extract the internal quantum efficiency as a function of carrier density and temperature as well as the extraction efficiency of the nanowire array. The results vividly document the high potential of GaAs/(Al,Ga)As core/shell nanowires for efficient light emitters integrated on the Si platform. Furthermore, the methodology established in this work can be applied to nanowires of any other materials system of interest for optoelectronic applications.

An accurate knowledge of the lattice parameters of the new nitride Sc$_\textit{x}$Al$_\textit{1-x}$N is essential for understanding the elastic and piezoelectric properties of this compound as well as for the ability to engineer its strain state in heterostructures. Using high-resolution x-ray diffractometry, we determine the lattice parameters of 100-nm-thick undoped Sc$_\textit{x}$Al$_\textit{1-x}$N layers grown on GaN(0001) templates by plasma-assisted molecular beam epitaxy. The Sc content $\textit{x}$ of the layers is measured independently by both x-ray photoelectron spectroscopy and energy-dispersive x-ray spectroscopy and ranges from 0 to 0.25. The in-plane lattice parameter of the layers linearly increases with increasing $\textit{x}$, while their out-of-plane lattice parameter remains constant. Layers with $\textit{x}$ $\approx$ 0.09 are found to be lattice matched to GaN, resulting in a smooth surface and a structural perfection equivalent to that of the GaN underlayer. In addition, a two-dimensional electron gas is induced at the Sc$_\textit{x}$Al$_\textit{1-x}$N/GaN heterointerface, with the highest sheet electron density and mobility observed for lattice-matched conditions.

We investigate the impact of threading dislocations with an edge component (a or a+c-type) on carrier recombination and diffusion in GaN(0001) layers close to the surface as well as in the bulk. To this end, we utilize cathodoluminescence imaging of the top surface of a GaN(0001) layer with a deeply buried (In,Ga)N quantum well. Varying the acceleration voltage of the primary electrons and comparing the signal from the layer and the quantum well enables us to probe carrier recombination at depths ranging from the close vicinity of the surface to the position of the quantum well. Our experiments are accompanied by fully three-dimensional Monte Carlo simulations of carrier drift, diffusion, and recombination in the presence of the surface, the quantum well, and the dislocation, taking into account the dislocation strain field and the resulting piezoelectric field at the dislocation outcrop. Near the surface, this field establishes an exciton dead zone around the dislocation, the extent of which is not related to the carrier diffusion length. However, reliable values of the carrier diffusion length can be extracted from the dipole-like energy shift observed in hyperspectral cathodoluminescence maps recorded around the dislocation outcrop at low acceleration voltages. For high acceleration voltages, allowing us to probe a depth where carrier recombination is unaffected by surface effects, we observe a much stronger contrast than expected from the piezoelectric field alone. This finding provides unambiguous experimental evidence for the strong nonradiative activity of edge threading dislocations in bulk GaN and hence also in buried heterostructures.

We determine the diffusion length of excess carriers in GaN by spatially resolved cathodoluminescence spectroscopy utilizing a single quantum well as carrier collector or carrier sink. Monochromatic intensity profiles across the quantum well are recorded for temperatures between 10 and 300 K. A classical diffusion model accounts for the profiles acquired between 120 and 300 K, while for temperatures lower than 120 K, a quantum capture process has to be taken into account in addition. Combining the diffusion length extracted from these profiles and the effective carrier lifetime measured by time-resolved photoluminescence experiments, we deduce the carrier diffusivity as a function of temperature. The experimental values are found to be close to theoretical ones for the ambipolar diffusivity of free carriers limited only by intrinsic phonon scattering. This agreement is shown to be fortuitous. The high diffusivity at low temperatures instead originates from an increasing participation of excitons in the diffusion process.

We investigate, both theoretically and experimentally, the drift, diffusion, and recombination of excitons in the strain field of an edge threading dislocation intersecting the GaN{0001} surface. We calculate and measure hyperspectral cathodoluminescence maps around the dislocation outcrop for temperatures between 10 to 200 K. Contrary to common belief, the cathodoluminescence intensity contrast is only weakly affected by exciton diffusion, but is caused primarily by exciton dissociation in the piezoelectric field at the dislocation outcrop. Hence, the extension of the dark spots around dislocations in the luminescence maps cannot be used to determine the exciton diffusion length. However, the cathodoluminescence energy contrast, reflecting the local bandgap variation in the dislocation strain field, does sensitively depend on the exciton diffusion length and hence enables its experimental determination.

GaN nanowire ensembles with axial InGaN multi-quantum wells (MQWs) were grown by molecular beam epitaxy. In a series of samples, we varied the In content in the MQWs from almost zero to about 20%. Within the nanowire ensemble, the MQWs fluctuate strongly in composition and size. Statistical information about the composition was obtained from x-ray diffraction and Raman spectroscopy. Photoluminescence at room temperature was obtained in the range from 2.2 eV to 2.5 eV depending on In content. Contrary to planar MQWs, the intensity increases with increasing In content. We compare the observed emission energies with transition energies obtained from a one-dimensional model, and conclude that several mechanisms for carrier localization affect the luminescence of these three-dimensional structures., Comment: This is an author-created, un-copyedited version of an article accepted for publication in Nanotechnology. IOP Publishing Ltd is not responsible for any errors or omissions in this version of the manuscript or any version derived from it. The Version of Record is available online at doi:10.1088/0957-4484/23/45/455203