Journal of the Korean Physical Society, Vol. 45, December 2004, pp. S840∼S843 Self-Assembled GaN Quantum Dots in GaN/Alx Ga1−x N Structures Grown by PAMBE G. N. Panin,∗ Y. S. Park and T. W. Kang Quantum-functional Semiconductor Research Center and Department of Physics, Dongguk University, Seoul 100-715 T. W. Kim Advanced Semiconductor Research Center, Division of Electrical and Computer Engineering, Hanyang University, Seoul 133-791 K. L. Wang and M. Bao Device Research Laboratory and Department of Electrical Engineering, University of California, Los Angeles, CA 90095-1594 High-resolution scanning electron microscopy (HRSEM), cathodoluminescence (CL) and electron beam induced current (EBIC) techniques were used to investigate the structural, optical and electrical properties of GaN/Alx Ga1−x N structures with self-assembled quantum dots (QDs) grown by molecular beam epitaxy (MBE). The results of the spatially resolved investigations show that GaN QD assemblies divided laterally by a 2D GaN layer can be formed on Al0.4 Ga0.6 N surface. The size and the density of QD assemblies are significantly affected by the surface polarity and the thickness of the GaN epilayer. The CL spectra of the QDs show blue-shifted GaN near-band-gap emission, and the shift is stronger for the Ga-face GaN epilayers. The EBIC measurements indicate reduced non-radiative charge-carrier recombination in the QD regions. PACS numbers: 81.07.Ta; 68.37.Hk; 78.67.Hc Keywords: Quantum Dots, GaN/AlGaN structures, CL, EBIC bility of adjusting the size and density of the assemblies by using different polarities of the GaN surface and the thickness of GaN epilayer was investigated. I. INTRODUCTION Semiconductor QDs have attracted considerable attention due to their promising applications in optoelectronic and electronic devices, such as lasers, photodetectors [1– 9] and single-electron transistors [10] operating at low current and high temperature. Until now, QD structures have been mainly fabricated from materials grown under compressive stress in the Stranski-Krastanov (SK) growth mode, due to the strain-induced self-organizing mechanism. The SK growth mode requires a large lattice mismatch between the wetting and the barrier materials to achieve elastic relaxation through the formation of QDs [11]. The formation of QDs from slightly stressed semiconductors by using a surfactant [12], an ion-sputtering technique [13], or hydrogenation treatment [14] has also been previously demonstrated. In this paper, we report on the self-formation of GaN nanometer-sized dots in local regions of GaN/AlGaN structures by plasma-assisted molecular beam epitaxy (PAMBE). HRSEM, CL and EBIC measurements were carried out to investigate the optical and electrical properties of the structures with QD assemblies. The possi∗ E-mail: II. EXPERIMENTS The GaN/AlGaN structures were grown on sapphire substrates by using a PAMBE system. An inductively coupled radio-frequency (RF) plasma source provided reactive nitrogen gas with a purity of 99.9999 % while Ga and Al with purities of 99.9999 % were evaporated by using a conventional effusion cell. Prior to GaN film growth, the surfaces of chemically cleaned substrates were exposed to an activated nitrogen beam for 10 min, so that they were completely covered with nitridated layers. The deposition of the GaN epilayers on Al0.4 Ga0.6 N layers grown at 550 ◦ C was carried out at a substrate temperature of 750 ◦ C. The thicknesses of GaN epilayers grown on an Al0.4 Ga0.6 N buffer layer of 100-nm thickness were 10 and 20 nm. Ga-face and N-face GaN epilayers were grown by a technique described previously [15]. III. RESULTS AND DISCUSSION g panin@dongguk.edu -S840- Self-Assembled GaN Quantum Dots in GaN/Alx Ga1−x N Structures· · · – G. N. Panin et al. -S841- Fig. 1. SEM images of GaN QD assemblies in GaN layer grown on Al0.4 Ga0.6 N surface in (a) CL, and (b) SE modes. The inset shows a HRSEM image of QDs within the assembly. The QD width is 30 nm. Fig. 3. (a) EBIC image of the GaN/AlGaN structure with a QD assembly, and (b) a line EBIC profile acquired through the assembly. Fig. 2. Cathodoluminescence images of GaN nanodot assemblies grown on Al0.4 Ga0.6 N layers with different surface polarities and thicknesses of the GaN epilayers: Ga-face GaN epilayers with thickness of (a) 10 nm (the dot assembly density is 8 × 106 cm−2 ), and (b) 20 nm (the dot assembly density is 2 × 106 cm−2 ) and N-face GaN epilayers with thickness of (c) 10 nm (the dot assembly density is 4 × 107 cm−2 ), and (d) 20 nm (the dot assembly density is 6 × 106 cm−2 ). HRSEM-CL examination of the GaN/AlGaN structures revealed assemblies of GaN nanodots, which are formed on the Al0.4 Ga0.6 N surface. The size and the density of the GaN QD assemblies divided by a 2D GaN layer are significantly affected by the surface polarity and the thickness of the GaN epilayer. Figure 1 shows SEM images of GaN QD assemblies in GaN/AlGaN structure in CL (Figure 1 (a)) and SE (Figure1 (b)) modes. The inset shows a HRSEM image of GaN QDs with width less than 30 nm. CL images of GaN nanodot assemblies for different surface polarities and thicknesses of the GaN layers are shown in Figure 2. The assemblies with diameters of approximately 2.5- 4 µm were formed in the Ga-face GaN epilayer, while the 1-2 µm assemblies of QDs were formed in the N-face GaN. The thin GaN layer shows small size and high density of nanodot assem- blies and smaller width of dots. The assemblies with size of approximately 100 nm consisting of GaN QDs with width less than 10 nm are observed for the 10-nm GaN layer. The highest density of assemblies (up to 4 × 107 cm−2 ) is observed for the 10-nm N-face GaN epilayers. It should be noted that the GaN nanodots show enhanced luminescence, whereas small Ga droplets, which could be immerged during the initial stage of growth, show strong non-radiative charge carrier recombination (Figure 2 (a): the small dark dots). Figure 3 shows an EBIC image of the GaN/ Al0.4 Ga0.6 N structure with a QD assembly as a circle of 3-µm size with bright contrast. The enhanced EBIC signal of QDs indicates low non-radiative recombination of charge carriers inside the QDs. This is in agreement with the enhanced luminescence of the QD assemblies revealed by CL measurements. Figure 4 shows ultra violet CL spectra of GaN QD assemblies for Ga-face and N-face of GaN epilayers. Three peaks at 3.5, 4.12 and 3.9 eV are observed in the spectra for N-face samples. The peak at 3.5 eV is attributed to neutral donor-bound exciton (Do , X) emissions in GaN [16]. The position of the peak does not depend on the GaN-layer polarity. The peak at 4.12 (4.22) eV is attributed to the Al0.4 Ga0.6 N near-band-gap exciton emission. Some difference in energy position of the peak for the Ga-face sample is attributed to different strains in the Ga-face and N-face GaN structures, which are revealed by XRD measurements. The peak centered at 3.9 eV is related with GaN QD emissions. The peak position depends on the thickness and polarity of the -S842- Fig. 4. 80-K ultra violet CL spectra obtained inside single assemblies in GaN epilayers with different polarities. Circles and rectangles represent the spectra for the Ga-face GaN and the N-face GaN epilayers, respectively. GaN epilayer. The QD luminescence is blue-shifted for the Ga-face GaN epilayer. A peak at 4.07 eV is detected for the Ga-face GaN epilayer of 20-nm thickness. The blue-shift increases as the GaN epilayer thickness decreases. This indicates the formation of smaller QDs with stronger quantum confinement of carriers. It should be noted that the CL spectra of the QD assemblies show broad bands as a result of the QD size dispersion. In order to investigate the origin of QD assembly formation, deep-level CL measurements of the structures were performed. Figure 5 shows deep-level CL spectra obtained at 80 K for (a) the N-face GaN, and (b) the Gaface GaN epilayers with different thickness. Three peaks centered at 2.43, 2.07 and 1.9 eV were observed for the Ga-face GaN epilayers. Their peak intensities depend strongly on the surface polarity and the thickness of the GaN epilayer. The relative intensity of the 2.07-eV luminescence emission increases with decreasing thickness of the GaN epilayer, for both the Ga-face and the N-face GaN layer. For N-polarity of the GaN epilayer, red-shift of the CL peak (2.02 eV) was observed. XRD measurements on the samples indicate a larger tensile strain in the N-face GaN/AlGaN structure. In addition, the CL peak at 1.9 eV shows a relatively enhanced intensity for the N-face GaN epilayers. The peaks at 2.43, 2.07 and 1.9 eV are attributed to defect-related deep-level luminescence [17–19]. Although the origin of this luminescence is not completely understood, different proposed models [20–22] suggest that the emission is due to native point defects and impurities. Our results indicate that impurity-assisted assembly formation takes place. The formation of the assemblies divided by a 2D GaN layer Journal of the Korean Physical Society, Vol. 45, December 2004 Fig. 5. 80-K deep-level CL spectra for (a) the N-face GaN, and (b) the Ga-face GaN epilayers with different thickness. Filled and open symbols represent the spectra for GaN epilayers with thickness of 10 nm and 20 nm, respectively. grown on Alx Ga1−x N surface could be explained by the inhomogeneous stress induced by impurities. The localimpurity induced strain leads to nanodot formation. The lattice mismatch between Al0.4 Ga0.6 N and GaN layers is not enough for effective elastic relaxation through the formation of dots by SK mode. However, the effect of impurities acting as surfactant [12] and strain source [19,23] could result in nanodot formation inside the GaN layer regions with an enhanced impurity concentration. The impurities distributed inhomogeneously in slightly mismatched AlGaN/GaN structures may provide the additional strain leading to the formation of the GaN nanodot assemblies. The density and size of the GaN nanodot assemblies depend on the thicknesses of the GaN epilayers. This correlates with the thickness dependences of the impurity and strain distributions. Gettering of impurities by structural defects might lead to an inhomogeneous impurity distribution and an increase of local strains, with subsequent relaxation through the formation of the QD assemblies. The GaN QD assemblies in the GaN/AlGaN structures show blue-shift of near-GaN-band-gap luminescence, which indicates a small size of dots. These assemblies strongly affect the luminescence and transport properties of the GaN/AlGaN structures. The controllable direct QD formation in local regions can be used for device fabrication. IV. CONCLUSIONS In summary, the QD assembly formation in GaN/AlGaN structures with different polarity of the Self-Assembled GaN Quantum Dots in GaN/Alx Ga1−x N Structures· · · – G. N. Panin et al. GaN layer was investigated through spatially-resolved HRSEM, CL and EBIC measurements. The results show that GaN QD assemblies with enhanced CL and EBIC are formed in local regions of the GaN layer grown on the Al0.4 Ga0.6 N surface. 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