We here present an experimental study on (010)-oriented β-Ga2O3 thin films homoepitaxially grown by plasma assisted molecular beam epitaxy. We study the effect of substrate treatments (i.e., O-plasma and Ga-etching) and several deposition parameters (i.e., growth temperature and metal-to-oxygen flux ratio) on the resulting Ga2O3 surface morphology and growth rate. In situ and ex-situ characterizations identified the formation of (110) and (1¯10)-facets on the nominally oriented (010) surface induced by the Ga-etching of the substrate and by several growth conditions, suggesting (110) to be a stable (yet unexplored) substrate orientation. Moreover, we demonstrate how metal-exchange catalysis enabled by an additional In-flux significantly increases the growth rate (>threefold increment) of monoclinic Ga2O3 at high growth temperatures, while maintaining a low surface roughness (rms < 0.5 nm) and preventing the incorporation of In into the deposited layer. This study gives important indications for obtaining device-quality thin films and opens up the possibility to enhance the growth rate in β-Ga2O3 homoepitaxy on different surfaces [e.g., (100) and (001)] via molecular beam epitaxy.
We present a systematic study on the influence of the miscut orientation on structural and electronic properties in the homoepitaxial growth on off-oriented β-Ga2O3 (100) substrates by metalorganic chemical vapour phase epitaxy. Layers grown on (100) substrates with 6° miscut toward the [001¯] direction show high electron mobilities of about 90 cm2 V−1 s−1 at electron concentrations in the range of 1–2 × 1018 cm−3, while layers grown under identical conditions but with 6° miscut toward the [001] direction exhibit low electron mobilities of around 10 cm2 V−1 s−1. By using high-resolution scanning transmission electron microscopy and atomic force microscopy, we find significant differences in the surface morphologies of the substrates after annealing and of the layers in dependence on their miscut direction. While substrates with miscuts toward [001¯] exhibit monolayer steps terminated by (2¯01) facets, mainly bilayer steps are found for miscuts toward [001]. Epitaxial growth on both substrates occurs in step-flow mode. However, while layers on substrates with a miscut toward [001¯] are free of structural defects, those on substrates with a miscut toward [001] are completely twinned with respect to the substrate and show stacking mismatch boundaries. This twinning is promoted at step edges by transformation of the (001)-B facets into (2¯01) facets. Density functional theory calculations of stoichiometric low index surfaces show that the (2¯01) facet has the lowest surface energy following the (100) surface. We conclude that facet transformation at the step edges is driven by surface energy minimization for the two kinds of crystallographically inequivalent miscut orientations in the monoclinic lattice of β-Ga2O3.
We experimentally demonstrate how In-mediated metal-exchange catalysis (MEXCAT) allows us to widen the deposition window for β-Ga2O3 homoepitaxy to conditions otherwise prohibitive for its growth via molecular beam epitaxy (e.g., substrate temperatures ≥800 °C) on the major substrate orientations, i.e., (010), (001), (2¯01), and (100) 6°-offcut. The obtained crystalline qualities, surface roughnesses, growth rates, and In-incorporation profiles are shown and compared with different experimental techniques. The growth rates, Γ, for fixed growth conditions are monotonously increasing with the surface free energy of the different orientations with the following order: Γ(010) > Γ(001) > Γ(2¯01) > Γ(100). Ga2O3 surfaces with higher surface free energy provide stronger bonds to the surface ad-atoms or ad-molecules, resulting in decreasing desorption, i.e., a higher incorporation/growth rate. The structural quality in the case of (2¯01), however, is compromised by twin domains due to the crystallography of this orientation. Notably, our study highlights β-Ga2O3 layers with high structural quality grown by MEXCAT-MBE not only in the most investigated (010) orientation but also in the (100) and (001) ones. In particular, MEXCAT on the (001) orientation results in both growth rate and structural quality comparable to the ones achievable with (010), and the limited incorporation of In associated with the MEXCAT deposition process does not change the insulating characteristics of unintentionally doped layers. The (001) surface is therefore suggested as a valuable alternative orientation for devices.
Homoepitaxial (100) β-Ga2O3 films were grown on substrates with miscut angles of 2°, 4°, and 6° toward [001¯] by metal organic vapor phase epitaxy. Step-flow growth mode, resulting in smooth film surfaces and high crystalline quality, could only be achieved if the diffusion length on the film surface corresponds approximately to the width of the terraces. Otherwise, 2D islands or step-bunching is obtained, which results in a deteriorated crystalline quality and reduced Hall mobility of the electrons. By varying the growth parameters such as the O2/Ga ratio, Ar push gas flow, and chamber pressure, the diffusion length could be adjusted so that step-flow growth mode could be achieved at all miscut angles. Furthermore, the growth rate could remarkably be increased from 1.6 nm/min to 4.3 nm/min. For homoepitaxial β-Ga2O3 films grown in step-flow growth mode, TEM measurements revealed a high crystalline quality, which is correlated with a high Hall mobility of 131 cm2/V s at a carrier concentration of 1.6 × 1017cm−3, which is comparable with β-Ga2O3 single crystal bulk values. This study clearly points out the high potential of β-Ga2O3 films for high performance MOSFETs if the influence of the deposition parameters on the structural and electrical properties is well understood.
In this paper, the growth of orthorhombic and monoclinic (Al x Ga1 − x )2O3 thin films on (00.1) Al2O3 by tin-assisted pulsed laser deposition is investigated as a function of oxygen pressure p(O2) and substrate temperature T g . For certain growth conditions, defined by T g ≥ 580°C and p(O2) ≤ 0.016 mbar, the orthorhombic κ-polymorph is stabilized. For T g = 540°C and p(O2) ≤ 0.016 mbar, the κ-, and the β-, as well as the spinel γ-polymorph coexist, as illustrated by XRD 2θ-ω-scans. Further employed growth parameters result in thin films with a monoclinic β-gallia structure. For all polymorphs, p(O2) and T g affect the formation and desorption of volatile suboxides, and thereby the growth rate and the cation composition. For example, low oxygen pressures lead to low growth rates and enhanced Al incorporation. This facilitates the structural engineering of polymorphic, ternary (Al,Ga)2O3 via selection of the relevant process parameters. Transmission electron microscopy (TEM) studies of a κ - (Al0.13Ga0.87)2O3 thin film reveal a more complex picture compared to that derived from x-ray diffraction measurements. Furthermore, this study presents the possibility of controlling the phase formation, as well as the Al-content, of thin films based on the choice of their growth conditions.
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