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We report the use of suboxide molecular-beam epitaxy (S-MBE) to grow α-(AlxGa1−x)2O3 films on (110) sapphire substrates over the 0 < x < 0.95 range of aluminum content. In S-MBE, 99.98% of the gallium-containing molecular beam arrives at the substrate in a preoxidized form as gallium suboxide (Ga2O). This bypasses the rate-limiting step of conventional MBE for the growth of gallium oxide (Ga2O3) from a gallium molecular beam and allows us to grow fully epitaxial α-(AlxGa1−x)2O3 films at growth rates exceeding 1 µm/h and relatively low substrate temperature (Tsub = 605 ± 15 °C). The ability to grow α-(AlxGa1−x)2O3 over the nominally full composition range is confirmed by Vegard’s law applied to the x-ray diffraction data and by optical bandgap measurements with ultraviolet–visible spectroscopy. We show that S-MBE allows straightforward composition control and bandgap selection for α-(AlxGa1−x)2O3 films as the aluminum incorporation x in the film is linear with the relative flux ratio of aluminum to Ga2O. The films are characterized by atomic-force microscopy, x-ray diffraction, and scanning transmission electron microscopy (STEM). These α-(AlxGa1−x)2O3 films grown by S-MBE at record growth rates exhibit a rocking curve full width at half maximum of ≊ 12 arc secs, rms roughness <1 nm, and are fully commensurate for x ≥ 0.5 for 20–50 nm thick films. STEM imaging of the x = 0.78 sample reveals high structural quality and uniform composition. Despite the high structural quality of the films, our attempts at doping with silicon result in highly insulating films. 

In this work, the structural and electrical properties of metalorganic chemical vapor deposited Si-doped β-(Al x Ga 1−x ) 2 O 3 thin films grown on (010) β-Ga 2 O 3 substrates are investigated as a function of Al composition. The room temperature Hall mobility of 101 cm 2 /V s and low temperature peak mobility (T = 65 K) of 1157 cm 2 /V s at carrier concentrations of 6.56 × 10 17 and 2.30 × 10 17  cm −3 are measured from 6% Al composition samples, respectively. The quantitative secondary ion mass spectroscopy (SIMS) characterization reveals a strong dependence of Si and other unintentional impurities, such as C, H, and Cl concentrations in β-(Al x Ga 1−x ) 2 O 3 thin films, with different Al compositions. Higher Al compositions in β-(Al x Ga 1−x ) 2 O 3 result in lower net carrier concentrations due to the reduction of Si incorporation efficiency and the increase of C and H impurity levels that act as compensating acceptors in β-(Al x Ga 1−x ) 2 O 3 films. Lowering the growth chamber pressure reduces Si concentrations in β-(Al x Ga 1−x ) 2 O 3 films due to the increase of Al compositions as evidenced by comprehensive SIMS and Hall characterizations. Due to the increase of lattice mismatch between the epifilm and substrate, higher Al compositions lead to cracking in β-(Al x Ga 1−x ) 2 O 3 films grown on β-Ga 2 O 3 substrates. The (100) cleavage plane is identified as a major cracking plane limiting the growth of high-quality Si-doped (010) β-(Al x Ga 1−x ) 2 O 3 films beyond the critical thicknesses, which leads to highly anisotropic and inhomogeneous behaviors in terms of conductivity. 

We report the use of suboxide molecular-beam epitaxy (S-MBE) to grow β-Ga2O3 at a growth rate of ∼1 µm/h with control of the silicon doping concentration from 5 × 1016 to 1019 cm−3. In S-MBE, pre-oxidized gallium in the form of a molecular beam that is 99.98% Ga2O, i.e., gallium suboxide, is supplied. Directly supplying Ga2O to the growth surface bypasses the rate-limiting first step of the two-step reaction mechanism involved in the growth of β-Ga2O3 by conventional MBE. As a result, a growth rate of ∼1 µm/h is readily achieved at a relatively low growth temperature (Tsub ≈ 525 °C), resulting in films with high structural perfection and smooth surfaces (rms roughness of <2 nm on ∼1 µm thick films). Silicon-containing oxide sources (SiO and SiO2) producing an SiO suboxide molecular beam are used to dope the β-Ga2O3 layers. Temperature-dependent Hall effect measurements on a 1 µm thick film with a mobile carrier concentration of 2.7 × 1017 cm−3 reveal a room-temperature mobility of 124 cm2 V−1 s−1 that increases to 627 cm2 V−1 s−1 at 76 K; the silicon dopants are found to exhibit an activation energy of 27 meV. We also demonstrate working metal–semiconductor field-effect transistors made from these silicon-doped β-Ga2O3 films grown by S-MBE at growth rates of ∼1 µm/h. 

β-Ga2O3 is a promising ultra-wide bandgap semiconductor whose properties can be further enhanced by alloying with Al. Here, using atomic-resolution scanning transmission electron microscopy, we find the thermodynamically unstable γ-phase is a ubiquitous structural defect in both β-(AlxGa1−x)2O3 films and doped β-Ga2O3 films grown by molecular beam epitaxy. For undoped β-(AlxGa1−x)2O3 films, we observe γ-phase inclusions between nucleating islands of the β-phase at lower growth temperatures (∼500–600 °C). In doped β-Ga2O3, a thin layer of the γ-phase is observed on the surfaces of films grown with a wide range of n-type dopants and dopant concentrations. The thickness of the γ-phase layer was most strongly correlated with the growth temperature, peaking at about 600 °C. Ga interstitials are observed in the β-phase, especially near the interface with the γ-phase. By imaging the same region of the surface of a Sn-doped β-(AlxGa1−x)2O3 after ex situ heating up to 400 °C, a γ-phase region is observed to grow above the initial surface, accompanied by a decrease in Ga interstitials in the β-phase. This suggests that the diffusion of Ga interstitials toward the surface is likely the mechanism for growth of the surface γ-phase and more generally that the more-open γ-phase may offer diffusion pathways to be a kinetically favored and early forming phase in the growth of Ga2O3. However, more modeling and simulation of the γ-phase and the interstitials are needed to understand the energetics and kinetics, the impact on electronic properties, and how to control them.