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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.
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First-principles surface energies for monoclinic Ga2O3 and Al2O3 and consequences for cracking of (Al x Ga1− x )2O3
Crack formation limits the growth of (AlxGa1−x)2O3 epitaxial films on Ga2O3 substrates. We employ first-principles calculations to determine the brittle fracture toughness of such films for three growth orientations of the monoclinic structure: [100], [010], and [001]. Surface energies and elastic constants are computed for the end compounds—monoclinic Ga2O3 and Al2O3—and used to interpolate to (AlxGa1−x)2O3 alloys. The appropriate crack plane for each orientation is determined, and the corresponding critical thicknesses are calculated based on Griffith’s theory, which relies on the balance between elastic energy and surface energy. We obtain lower bounds for the critical thickness, which compare well with available experiments. We also perform an in-depth analysis of surface energies for both relaxed and unrelaxed surfaces, providing important insights into the factors that determine the relative stability of different surfaces. Our study provides physical insights into surface stability, crack planes, and the different degrees of crack formation in (AlxGa1−x)2O3 films for different growth orientations.
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- Award ID(s):
- 1725797
- PAR ID:
- 10595142
- Publisher / Repository:
- American Institute of Physics
- Date Published:
- Journal Name:
- APL Materials
- Volume:
- 8
- Issue:
- 9
- ISSN:
- 2166-532X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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