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Optimizing thermal anneals of Si-implanted β-Ga2O3 is critical for low resistance contacts and selective area doping. We report the impact of annealing ambient, temperature, and time on the activation of room temperature ion-implanted Si in β-Ga2O3 at concentrations from 5 × 1018 to 1 × 1020 cm−3, demonstrating full activation (>80% activation, mobilities >70 cm2/V s) with contact resistances below 0.29 Ω mm. Homoepitaxial β-Ga2O3 films, grown by plasma-assisted molecular beam epitaxy on Fe-doped (010) substrates, were implanted at multiple energies to yield 100 nm box profiles of 5 × 1018, 5 × 1019, and 1 × 1020 cm−3. Anneals were performed in an ultra-high vacuum-compatible quartz furnace at 1 bar with well-controlled gas compositions. To maintain β-Ga2O3 stability, pO2 must be greater than 10−9 bar. Anneals up to pO2 = 1 bar achieve full activation at 5 × 1018 cm−3, while 5 × 1019 cm−3 must be annealed with pO2 ≤ 10−4 bar, and 1 × 1020 cm−3 requires pO2 < 10−6 bar. Water vapor prevents activation and must be maintained below 10−8 bar. Activation is achieved for anneal temperatures as low as 850 °C with mobility increasing with anneal temperatures up to 1050 °C, though Si diffusion has been reported above 950 °C. At 950 °C, activation is maximized between 5 and 20 min with longer times resulting in decreased carrier activation (over-annealing). This over-annealing is significant for concentrations above 5 × 1019 cm−3 and occurs rapidly at 1 × 1020 cm−3. Rutherford backscattering spectrometry (channeling) suggests that damage recovery is seeded from remnant aligned β-Ga2O3 that remains after implantation; this conclusion is also supported by scanning transmission electron microscopy showing retention of the β-phase with inclusions that resemble the γ-phase. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

Strain-engineering is a powerful means to tune the polar, structural, and electronic instabilities of incipient ferroelectrics. KTaO3 is near a polar instability and shows anisotropic superconductivity in electron-doped samples. Here, we demonstrate growth of high-quality KTaO3 thin films by molecular-beam epitaxy. Tantalum was provided by either a suboxide source emanating a TaO2 flux from Ta2O5 contained in a conventional effusion cell or an electron-beam-heated tantalum source. Excess potassium and a combination of ozone and oxygen (10% O3 + 90% O2) were simultaneously supplied with the TaO2 (or tantalum) molecular beams to grow the KTaO3 films. Laue fringes suggest that the films are smooth with an abrupt film/substrate interface. Cross-sectional scanning transmission electron microscopy does not show any extended defects and confirms that the films have an atomically abrupt interface with the substrate. Atomic force microscopy reveals atomic steps at the surface of the grown films. Reciprocal space mapping demonstrates that the films, when sufficiently thin, are coherently strained to the SrTiO3 (001) and GdScO3 (110) substrates. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

We report the in situ, direct epitaxial synthesis of (0001)-oriented PdCoO2 thin films on c-plane sapphire using ozone-assisted molecular-beam epitaxy. The resulting films have smoothness, structural perfection, and electrical characteristics that rival the best in situ grown PdCoO2 thin films in the literature. Metallic conductivity is observed in PdCoO2 films as thin as ∼2.0 nm. The PdCoO2 films contain 180° in-plane rotation twins. Scanning transmission electron microscopy reveals that the growth of PdCoO2 on the (0001) surface of Al2O3 begins with the CoO2 layer. [ABSTRACT FROM AUTHOR]

With nearly complete spin polarization, the ferromagnetic semiconductor europium monoxide could enable next-generation spintronic devices by providing efficient ohmic spin injection into silicon. Spin injection is greatly affected by the quality of the interface between the injector and silicon. Here, we use atomic-resolution scanning transmission electron microscopy in conjunction with electron energy loss spectroscopy to directly image and chemically characterize a series of EuO|Si and EuO|YAlO3 interfaces fabricated using different growth conditions. We identify the presence of europium silicides and regions of disorder at the EuO|Si interfaces, imperfections that could significantly reduce spin injection efficiencies via spin-flip scattering. [ABSTRACT FROM AUTHOR]

The ability to detect individual impurity atoms has been greatly enhanced by the development of aberration-corrected electron microscopes. The reduced depth of focus potentially enables three-dimensional reconstructions of impurity atoms from through-focal series. We test the robustness of this depth-sectioning method for detecting impurity atoms in gate oxides using multislice simulations. For amorphous materials, dopants can be reliably imaged, and are accurately described by a simpler three-dimensional linear imaging model. For crystalline materials, however, channeling artifacts can render the signal uninterpretable. These artifacts can be eliminated by orienting the crystal slightly off the zone axis, which still preserves atomic resolution. [ABSTRACT FROM AUTHOR]

(001)-oriented LaAlO3 films were grown epitaxially on (001) Si substrates utilizing an ultrathin 5 unit-cell-thick SrTiO3 buffer layer. The SrTiO3 layer was grown at ∼250 °C and annealed in vacuum at 550 °C, following an epitaxy-by-periodic-annealing procedure. Upon this buffer layer, the LaAlO3 layer was then grown by codeposition at 580 °C. The rocking curve of the as-grown LaAlO3 film exhibits a full width at half maximum value as small as 0.02°. Atomic force microscopy shows that the surface of the LaAlO3 film has a root-mean-square roughness of 1.3 Å. Scanning transmission electron microscopy reveals that the LaAlO3/SrTiO3 interface and the SrTiO3/Si interfaces are sharp. This high crystalline quality, twin-free, epitaxial LaAlO3 on SrTiO3 on silicon could be relevant to integrating oxides with multiple functionalities on silicon. [ABSTRACT FROM AUTHOR]

Electron energy loss spectroscopy on an aberration-corrected scanning transmission electron microscope was used to map the elemental composition and bonding in a thin film of the multiferroic LuFe2O4 with atomic resolution. A two-dimensional analysis of the fine structure of the O-K edge yielded distinct signals for the two inequivalent oxygen sites in the crystal. Comparison to an ab-initio simulation showed that these two components can be interpreted in terms of the differing hybridization of the O p orbitals to the Lu and Fe d orbitals, thus producing an atomic-resolution map of the local oxygen bonding environment. [ABSTRACT FROM AUTHOR]