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.
more »
« less
Rotationally Aligned Hexagonal Boron Nitride on Sapphire by High-Temperature Molecular Beam Epitaxy
Hexagonal boron nitride (hBN) has been grown on sapphire substrates by ultrahigh-temperature molecular beam epitaxy (MBE). A wide range of substrate temperatures and boron fluxes have been explored, revealing that high crystalline quality hBN layers are grown at high substrate temperatures, >1600℃ , and low boron fluxes, ∼1 × 10%& Torr beam equivalent pressure. In situ reflection high-energy electron diffraction revealed the growth of hBN layers with 60° rotational symmetry and the [112+ 0] axis of hBN parallel to the [11+ 00] axis of the sapphire substrate. Unlike the rough, polycrystalline films previously reported, atomic force microscopy and transmission electron microscopy characterization of these films demonstrate smooth, layered, few-nanometer hBN films on a nitridated sapphire substrate. This demonstration of high-quality hBN growth by MBE is a step toward its integration into existing epitaxial growth platforms, applications, and technologies.
more »
« less
- Award ID(s):
- 1719875
- PAR ID:
- 10151947
- Date Published:
- Journal Name:
- Physical review and Physical review letters index
- ISSN:
- 0094-0003
- Page Range / eLocation ID:
- 1-6
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
null (Ed.)Abstract Superconducting resonators with high quality factors have been fabricated from aluminum films, suggesting potential applications in quantum computing. Improvement of thin film crystal quality and removal of void and pinhole defects will improve quality factor and functional yield. Epitaxial aluminum films with superb crystallinity, high surface smoothness, and interface sharpness were successfully grown on the c-plane of sapphire using sputter beam epitaxy. This study assesses the effects of varying substrate preparation conditions and growth and prebake temperatures on crystallinity and smoothness. X-ray diffraction and reflectivity measurements yield extensive Laue oscillations and Kiessig thickness fringes for films grown at 200 °C under 15 mTorr Ar, indicating excellent crystallinity and surface smoothness; moreover, an additional substrate preparation procedure which involves (1) a modified substrate cleaning procedure and (2) prebake at 700 °C in 20 mTorr O 2 is shown by atomic force microscopy to yield nearly pinhole-free film growth while maintaining epitaxy and high crystal quality. The modified cleaning procedure is environmentally friendly and eliminates the acid etch steps common to conventional sapphire preparation, suggesting potential industrial application both on standard epitaxial and patterned surface sapphire substrates.more » « less
-
Transparent conducting oxides, such as Ga-doped ZnO (GZO) and Al-doped ZnO (AZO) are attractive materials for high-performance plasmonic devices operating at telecommunication wavelengths. In this contribution, we compare the growth of epsilon-near-zero GZO and AZO films on sapphire by two different deposition techniques: molecular beam epitaxy (MBE) and atomic layer deposition (ALD). For MBE of GZO, a multiple buffer consisted of a high-temperature MgO layer, a low-temperature ZnO, followed by a high-temperature ZnO layer is employed to assure the crystalline quality of the GZO film. By controlling the growth parameters, including Ga doping level, VI/II ratio, substrate temperature, we are able to produce GZO films at 350 °C with electron mobility between 30 and 50 cm2/V.s, electron concentration up to 7×1020 cm-3, and resistivity down to 2.5×10-4 Ω.cm. For ALD of AZO, without using any buffer, by reducing the Al pulse duration, we are able to grow the AZO films under a large ratio of Al to Zn pulses of 1:6, which improves the activation of Al as an effective dopant. Hence AZO films with electron concentration above 7×1020 cm-3, electron mobility between 10 and 20 cm2/V.s, and resistivity below 6×10-4 Ω.cm have been obtained at 250 °C. The corresponding epsilon-near-zero point in the ALD-grown material was tuned down to 1470 nm. Our data indicate that the ALD method provides a low-temperature route to plasmonic TCOs for telecommunication wavelength range. Effect of electron mobility on optical loss and, therefore, plasmonic figure of merit is discussed.more » « less
-
Abstract The structural properties of co-deposited ultrathin PtSe 2 films grown at low temperatures by molecular beam epitaxy on c-plane Al 2 O 3 are studied. By simultaneously supplying a Se flux from a Knudsen cell and Pt atoms from an electron-beam evaporator, crystalline (001)-oriented PtSe 2 films were formed between 200 °C and 300 °C. The long separation between substrate and electron beam evaporator of about 60 cm ensured minimal thermal load. At optimum deposition temperatures, a ten times or even higher supply rate of Se compared to Pt ensured that the pronounced volatility of the Se was compensated and the PtSe 2 phase was formed and stabilized at the growth front. Postgrowth anneals under a Se flux was found to dramatically improve the crystalline quality of the films. Even before the postgrowth anneal in Se, the crystallinity of PtSe 2 films grown with the co-deposition method was superior to films realized by thermal assisted conversion. Postgrowth annealed films showed Raman modes with narrower peaks and more than twice the intensity. Transmission electron microscopy investigations revealed that the deposited material transitioned to a two-dimensional layered structure only after the postgrowth anneal. PtSe 2 growth was found to start as single layer islands that preferentially nucleated at atomic steps of the substrate and progressed in a layer-by-layer like fashion. A close to ideal wetting behavior resulted in coalesced PtSe 2 films after depositing about 1.5 PtSe 2 layers. Detailed Raman investigation of the observed PtSe 2 layer breathing modes of films grown under optimized co-deposition conditions revealed an interlayer coupling force constant of 5.0–5.6 × 10 19 N m −3 .more » « less
-
A seemingly simple oxide with a rutile structure, RuO2, has been shown to possess several intriguing properties ranging from strain-stabilized superconductivity to a strong catalytic activity. Much interest has arisen surrounding the controlled synthesis of RuO2 films, but unfortunately, utilizing atomically controlled deposition techniques, such as molecular beam epitaxy (MBE), has been difficult due to the ultra-low vapor pressure and low oxidation potential of Ru. Here, we demonstrate the growth of epitaxial, single crystalline RuO2 films on different substrate orientations using the novel solid-source metal–organic (MO) MBE. This approach circumvents these issues by supplying Ru using a “pre-oxidized” solid MO precursor containing Ru. High-quality epitaxial RuO2 films with a bulk-like room-temperature resistivity of 55 μΩ cm were obtained at a substrate temperature as low as 300 °C. By combining x-ray diffraction, transmission electron microscopy, and electrical measurements, we discuss the effect of substrate temperature, orientation, film thickness, and strain on the structure and electrical properties of these films. Our results illustrating the use of a novel solid-source metal–organic MBE approach pave the way to the atomic-layer controlled synthesis of complex oxides of “stubborn” metals, which are not only difficult to evaporate but also hard to oxidize.more » « less