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In this study, we investigate in situ etching of β-Ga2O3 in a metalorganic chemical vapor deposition system using tert-butyl chloride (TBCl). We report etching of both heteroepitaxial 2¯01-oriented and homoepitaxial (010)-oriented β-Ga2O3 films over a wide range of substrate temperatures, TBCl molar flows, and reactor pressures. We infer that the likely etchant is HCl (g), formed by the pyrolysis of TBCl in the hydrodynamic boundary layer above the substrate. The temperature dependence of the etch rate reveals two distinct regimes characterized by markedly different apparent activation energies. The extracted apparent activation energies suggest that at temperatures below ∼800 °C, the etch rate is likely limited by desorption of etch products. The relative etch rates of heteroepitaxial 2¯01 and homoepitaxial (010) β-Ga2O3 were observed to scale by the ratio of the surface energies, indicating an anisotropic etch. Relatively smooth post-etch surface morphology was achieved by tuning the etching parameters for (010) homoepitaxial films. 

Epitaxial untwinned SrRuO3 thin films were grown on (110)-oriented DyScO3 substrates by molecular-beam epitaxy. We report an exceptional sample with a residual resistivity ratio (RRR), ρ [300 K]/ρ [4 K] of 205 and a ferromagnetic Curie temperature, TC, of 168.3 K. We compare the properties of this sample to other SrRuO3 films grown on DyScO3(110) with RRRs ranging from 8.8 to 205, and also compare it to the best reported bulk single crystal of SrRuO3. We determine that SrRuO3 thin films grown on DyScO3(110) have an enhanced TC as long as the RRR of the thin film is above a minimum electrical quality threshold. This RRR threshold is about 20 for SrRuO3. Films with lower RRR exhibit TCs that are significantly depressed from the intrinsic strain-enhanced value. 

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. 

The unconventional superconductivity in Sr2RuO4 is infamously susceptible to suppression by small levels of disorder such that it has been most commonly studied in extremely high-purity bulk crystals. Here, we harness local structural and spectroscopic scanning transmission electron microscopy measurements in epitaxial thin films of Sr2RuO4 to disentangle the impact of different types of crystalline disorder on superconductivity. We find that cation off-stoichiometry during growth gives rise to two distinct types of disorder: mixed-phase structural inclusions that accommodate excess ruthenium and ruthenium vacancies when the growth is ruthenium-deficient. Several superconducting films host mixed-phase intergrowths, suggesting this microstructural disorder has relatively little impact on superconductivity. In a non-superconducting film, on the other hand, we measure a high density of ruthenium-vacancies (∼14%) with no significant reduction in the crystallinity of the film. The results suggest that ruthenium vacancy disorder, which is hidden to many structural probes, plays an important role in suppressing superconductivity. We discuss the broader implications of our findings to guide the future synthesis of this and other layered systems. 

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. 

Homologous series are layered phases that can have a range of stoichiometries depending on an index n. Examples of perovskite-related homologous series include (ABO3)nAO Ruddlesden–Popper phases and (Bi2O2) (An−1BnO3n+1) Aurivillius phases. It is challenging to precisely control n because other members of the homologous series have similar stoichiometry and a phase with the desired n is degenerate in energy with syntactic intergrowths among similar n values; this challenge is amplified as n increases. To improve the ability to synthesize a targeted phase with precise control of the atomic layering, we apply the x-ray diffraction (XRD) approach developed for superlattices of III–V semiconductors to measure minute deviations from the ideal structure so that they can be quantitatively eradicated in subsequent films. We demonstrate the precision of this approach by improving the growth of known Ruddlesden–Popper phases and ultimately, by synthesizing an unprecedented n = 20 Ruddlesden–Popper phase, (ATiO3)20AO where the A-site occupancy is Ba0.6Sr0.4. We demonstrate the generality of this method by applying it to Aurivillius phases and the Bi2Sr2Can–1CunO2n+4 series of high-temperature superconducting phases. 

We report the growth of superconducting Sr2RuO4 thin films by molecular-beam epitaxy on (110) NdGaO3 substrates with transition temperatures of up to 1.8 K. We calculate and experimentally validate a thermodynamic growth window for the adsorption-controlled growth of superconducting Sr2RuO4 epitaxial thin films. The growth window for achieving superconducting Sr2RuO4 thin films is narrow in growth temperature, oxidant pressure, and ruthenium-to-strontium flux ratio.