Abstract
This PhD deals with the epitaxial growth, structural and optical properties of AlyGa1-yN quantum dots (QDs) grown on AlxGa1-xN (0001) by molecular beam epitaxy (MBE), with the aim to study their potential as a novel route for efficient ultraviolet (UV) emitters.First, we have studied the growth of GaN QDs using either plasma MBE (PAMBE) or ammonia MBE (NH3-MBE) to find the most adapted nitrogen source for the fabrication of UV emitting QDs. It was shown that the growth process is better controlled using PAMBE, leading to the growth of GaN QDs with higher densities, better size uniformity and up to three times higher photoluminescence (PL) intensities. Also, the influence of the epitaxial strain on the QD self-assembling process was studied by fabricating GaN QDs on different AlxGa1-xN surfaces (with 0.5 ≤ x ≤ 0.7). We showed that QDs with higher densities and smaller sizes (heights) are formed by using a larger lattice-mismatch (i.e. a higher xAl composition). However, photoluminescence (PL) measurements indicated a strong redshift in the emission energy as the Al content of the AlxGa1-xN template increases due to the increase of the internal electric field discontinuity from 3 to 5.3 MV/cm.Next, in-depth investigations of the growth conditions and optical properties of Al0.1Ga0.9N QDs / Al0.5Ga0.5N were done presenting the different challenges to be solved to grow efficient QDs. Changing the growth procedure, especially the post-growth annealing step, has shown a modification of the QD shape from elongated QDs, formed with an annealing at 740°C, to symmetric QDs, formed with an annealing at a temperature around or above 800°C. An additional band emission at lower energies was also observed for QDs grown with a lower annealing temperature (740°C). This additional band emission was attributed to the formation of QDs with higher heights and a reduced Al composition less than the nominal one of 10 % (i.e. forming Ga-rich QDs). The influence of the annealing step performed at higher temperature has been shown to strongly decrease the PL emission from this additional QD family. In addition, this annealing step strongly impacted the QD shape and led to an improvement of the QD radiative efficiency by a factor 3. Then, the AlxGa1-xN barrier composition (0.5 ≤ x ≤ 0.7), the AlyGa1-yN QD composition (0.1 ≤ y ≤ 0.4) as well as the deposited amount were varied in order to assess the range of accessible emission energies. Also, the influence of varying the AlxGa1-xN barrier composition on the QD formation was studied. By varying these growth conditions, the QD wavelength emission was shifted from the UVA down to the UVC range, reaching a minimum wavelength emission of 270 - 275 nm (for water and air purification applications) with a high radiative efficiency. Time resolved photoluminescence (TRPL) combined with temperature dependent PL measurements enabled us to determine the internal quantum efficiencies (IQE) of AlyGa1-yN QDs / AlxGa1-xN (0001). IQE values between 50 % and 66 % were found at low temperature, combined with the ability to reach a PL integrated intensity ratio, between 300 K and 9 K, up to 75 % for GaN QDs and 46 % for AlyGa1-yN QDs (versus 0.5 % in a similar quantum well structure emitting in the UVC range).Finally, the demonstration of AlyGa1-yN QD-based light emitting diode prototypes, emitting in the whole UVA range, using GaN and Al0.1Ga0.9N QDs, and in the UVB range down to 305 nm with Al0.2Ga0.8N QDs active regions, was shown.