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We report the epitaxial growth of (010) β-(AlxGa1−x)2O3 using tritertiarybutylaluminum (TTBAl) as an aluminum gas precursor in a hybrid molecular beam epitaxy (h-MBE) system. In conventional MBE systems, a thermal effusion cell is typically used to supply Al. However, in an oxide MBE system, using a conventional Al effusion cell can cause difficulties due to the oxidation of the Al source during growth. This often requires breaking the vacuum frequently to reload Al. Our approach utilizes TTBAl, a gaseous Al source, via a h-MBE to circumvent the oxidation issues associated with traditional solid Al sources. We investigated the growth conditions of β-(AlxGa1−x)2O3, varying TTBAl supply and growth temperature. For this purpose, we utilized both elemental Ga and Ga-suboxide as Ga precursors. Controllable and repeatable growth of β-(AlxGa1−x)2O3 with Al compositions ranging from 1% to 25% was achieved. The impurity incorporation and crystal quality of the resulting β-(AlxGa1−x)2O3 films were also studied. Using TTBAl as a gaseous precursor in h-MBE has proven to maintain stable Al supply, enabling the controlled growth of high-quality β-(AlxGa1−x)2O3 films.
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Epitaxial growth of α-(Al x Ga1− x )2O3 by suboxide molecular-beam epitaxy at 1 µm/h
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.
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- Award ID(s):
- 1719875
- PAR ID:
- 10549069
- Publisher / Repository:
- AIP Publishing
- Date Published:
- Journal Name:
- APL Materials
- Volume:
- 12
- Issue:
- 4
- ISSN:
- 2166-532X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript
- Journal Article:
- https://doi.org/10.1063/5.0170095
