[en] Indium incorporation and surface morphology of InAlN layers grown on (0001) GaN by plasma-assisted molecular beam epitaxy were investigated as a function of the impinging In flux and the substrate temperature in the 450-610 deg. C range. In incorporation was found to decrease with substrate temperature due to thermal decomposition of the growing layer, while for a given temperature it increased with the impinging In flux until stoichiometry was reached at the growth front. The InN losses during growth followed an Arrhenius behavior characterized by an activation energy of 2.0 eV. A growth diagram highly instrumental to identify optimum growth conditions was established

[en] We investigate the influence of modified growth conditions during the spontaneous formation of GaN nanowires (NWs) on Si(111) in plasma-assisted molecular beam epitaxy. We find that a two-step growth approach, where the substrate temperature is increased during the nucleation stage, is an efficient method to gain control over the area coverage, average diameter, and coalescence degree of GaN NW ensembles. Furthermore, we also demonstrate that the growth conditions employed during the incubation time that precedes nanowire nucleation do not influence the properties of the final nanowire ensemble. Therefore, when growing GaN NWs at elevated temperatures or with low Ga/N ratios, the total growth time can be reduced significantly by using more favorable growth conditions for nanowire nucleation during the incubation time. (paper)

[en] AlN layers with thicknesses between 2 and 14 nm were grown on Si(111) substrates by molecular beam epitaxy. The effect of the AlN layer thickness on the morphology and nucleation time of spontaneously formed GaN nanowires (NWs) was investigated by scanning electron microscopy and line-of-sight quadrupole mass spectrometry, respectively. We observed that the alignment of the NWs grown on these layers improves with increasing layer thickness while their nucleation time decreases. Our results show that 4 nm is the smallest thickness of the AlN layer that allows the growth of well-aligned NWs with short nucleation time. Such an AlN buffer layer was successfully employed, together with a patterned SiO_x mask, for the selective-area growth (SAG) of vertical GaN NWs. In addition, we fabricated light-emitting diodes (LEDs) from NW ensembles that were grown by means of self-organization phenomena on bare and on AlN-buffered Si substrates. A careful characterization of the optoelectronic properties of the two devices showed that the performance of NW-LEDs on bare and AlN-buffered Si is similar. Electrical conduction across the AlN buffer is facilitated by a high number of grain boundaries that were revealed by transmission electron microscopy. These results demonstrate that grainy AlN buffer layers on Si are compatible both with the SAG of GaN NWs and LED operation. Therefore, this study is a first step towards the fabrication of LEDs on Si substrates based on homogeneous NW ensembles. (paper)

[en] The morphology of GaN samples grown by plasma-assisted molecular beam epitaxy on Si(111) was systematically studied as a function of impinging Ga/N flux ratio and growth temperature (730-850 deg. C). Two different growth regimes were identified: compact and nanocolumnar. A growth diagram was established as a function of growth parameters, exhibiting the transition between growth regimes, and showing under which growth conditions GaN cannot be grown due to thermal decomposition and Ga desorption. Present results indicate that adatoms diffusion length and the actual Ga/N ratio on the growing surface are key factors to achieve nanocolumnar growth.

[en] We investigate the structural and optical properties of spontaneously formed GaN nanowires with different degrees of coalescence. This quantity is determined by an analysis of the cross-sectional area and perimeter of the nanowires obtained by plan-view scanning electron microscopy. X-ray diffraction experiments are used to measure the inhomogeneous strain in the nanowire ensembles as well as the orientational distribution of the nanowires. The comparison of the results obtained for GaN nanowire ensembles prepared on bare Si(111) and AlN buffered 6H-SiC(000 1-bar ) reveals that the main source of the inhomogeneous strain is the random distortions caused by the coalescence of adjacent nanowires. The magnitude of the strain inhomogeneity induced by nanowire coalescence is found not to be determined solely by the coalescence degree, but also by the mutual misorientation of the coalesced nanowires. The linewidth of the donor-bound exciton transition in photoluminescence spectra does not exhibit a monotonic increase with the coalescence degree. In contrast, the comparison of the root mean square strain with the linewidth of the donor-bound exciton transition reveals a clear correlation: the higher the strain inhomogeneity, the larger the linewidth. (paper)

[en] Low-temperature photoluminescence is studied in detail in GaN nanocolumns (NCs) grown by plasma-assisted molecular beam epitaxy under various conditions (substrate temperature and impinging Ga/N flux ratio). The relative intensities of the different emission lines, in particular those related to structural defects, appear to be correlated with the growth conditions, and clearly linked to the NC sample morphology. We demonstrate, in particular, that all lines comprised between 3.10 and 3.42 eV rapidly lose intensity when the growth conditions are such that the NC coalescence is reduced. The well-known line around 3.45 eV, characteristic of GaN NC samples, shows, however, a behavior that is exactly the opposite of the other lines, namely, for growth conditions leading to reduced NC coalescence, this line tends to become more prominent, thus proving to be intrinsic to individual GaN NCs.

[en] Thermal decomposition of wurtzite (0001)-oriented GaN was analyzed: in vacuum, under active N exposure, and during growth by rf plasma-assisted molecular beam epitaxy. The GaN decomposition rate was determined by measurements of the Ga desorption using in situ quadrupole mass spectrometry, which showed Arrhenius behavior with an apparent activation energy of 3.1 eV. Clear signatures of intensity oscillations during reflection high-energy electron diffraction measurements facilitated complementary evaluation of the decomposition rate and highlighted a layer-by-layer decomposition mode in vacuum. Exposure to active nitrogen, either under vacuum or during growth under N-rich growth conditions, strongly reduced the GaN losses due to GaN decomposition

[en] An alternative approach is presented for the plasma-assisted molecular beam epitaxy of high-quality GaN. Under N-rich growth conditions, an unexpected layer-by-layer growth mode was found for a wide range of growth temperatures in the GaN thermal decomposition regime (>750 deg. C). Consequently, superior surface morphologies with roughness of less than 1 nm (rms) have been achieved. For lightly Si-doped GaN films, room-temperature electron mobilities exceeding 1100 cm²/V s were measured, surpassing the commonly insulating nature of GaN grown under N-rich conditions at low temperature

[en] A study of AlInGaN epilayers, grown by plasma-assisted molecular beam epitaxy, was performed using spatially resolved x-ray microanalysis and luminescence spectroscopy in order to investigate competition between the incorporation of In, Al, and Ga as a function of the growth temperature in the 565-660 deg. C range and the nominal AlN mole fraction. The samples studied have AlN and InN mole fractions in the ranges of 4%-30% and 0%-16%, respectively. Composition measurements show the effect of decreasing temperature to be an increase in the incorporation of InN, accompanied by a small but discernible decrease in the ratio of GaN to AlN mole fractions. The incorporation of In is also shown to be significantly increased by decreasing the Al mole fraction. Optical emission peaks, observed by cathodoluminescence mapping and by photoluminescence, provide further information on the epilayer compositions as a function of substrate temperature, and the dependencies of peak energy and linewidth are plotted

[en] We present a comprehensive description of the self-assembled nucleation and growth of GaN nanowires (NWs) by plasma-assisted molecular beam epitaxy on amorphous Al_x O_y buffers (a-Al_x O_y) prepared by atomic layer deposition. The results are compared with those obtained on nitridated Si(111). Using line-of-sight quadrupole mass spectrometry, we analyze in situ the incorporation of Ga starting from the incubation and nucleation stages till the formation of the final nanowire ensemble and observe qualitatively the same time dependence for the two types of substrates. However, on a-Al_x O_y the incubation time is shorter and the nucleation faster than on nitridated Si. Moreover, on a-Al_x O_y we observe a novel effect of decrease in incorporated Ga flux for long growth durations which we explain by coalescence of NWs leading to reduction of the GaN surface area where Ga may reside. Dedicated samples are used to analyze the evolution of surface morphology. In particular, no GaN nuclei are detected when growth is interrupted during the incubation stage. Moreover, for a-Al_x O_y, the same shape transition from spherical cap-shaped GaN crystallites to the NW-like geometry is found as it is known for nitridated Si. However, while the critical radius for this transition is only slightly larger for a-Al_x O_y than for nitridated Si, the critical height is more than six times larger for a-Al_x O_y. Finally, we observe that in fully developed NW ensembles, the substrate no longer influences growth kinetics and the same N-limited axial growth rate is measured on both substrates. We conclude that the same nucleation and growth processes take place on a-Al_x O_y as on nitridated Si and that these processes are of a general nature. Quantitatively, nucleation proceeds somewhat differently, which indicates the influence of the substrate, but once shadowing limits growth processes to the upper part of the NW ensemble, they are not affected anymore by the type of substrate. (paper)