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Creators/Authors contains: "Williams, Michael D"

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  1. Abstract The intersection of superconductivity and ferroelectricity hosts a wide range of exotic quantum phenomena. Here, we report on the observation of superconductivity in high-quality tin telluride films grown by molecular beam epitaxy. Unintentionally doped tin telluride undergoes a ferroelectric transition at ~100 K. The critical temperature of superconductivity increases monotonically with indium concentration. The critical field of superconductivity, however, does not follow the same behavior as critical temperature with indium concentration and exhibits a carrier-density-dependent violation of the Pauli limit. The electron–phonon coupling, according to the McMillan formula, exhibits a systematic enhancement with indium concentration, suggesting a potential violation of Bardeen–Cooper–Schrieffer (BCS) weak coupling at high indium concentrations. 
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  2. We report a two-step film-growth process using suboxide molecular-beam epitaxy (S-MBE) that produces Si-doped α-Ga2O3 with record transport properties. The method involves growing a relaxed α-(AlxGa1−x)2O3 buffer layer on m-plane sapphire at a relatively high substrate temperature (Tsub), ∼750 °C, followed by an Si-doped α-Ga2O3 overlayer grown at lower Tsub, ∼500 °C. The high Tsub allows the ∼3.6% lattice-mismatched α-(AlxGa1−x)2O3 buffer with x = 0.08 ± 0.02 to remain epitaxial and phase pure during relaxation to form a pseudosubstrate for the overgrowth of α-Ga2O3. The optimal conditions for the subsequent growth of Si-doped α-Ga2O3 by S-MBE are 425 °C ≤ Tsub ≤ 500 °C and P80% O3 = 5 × 10−6 Torr. Si-doped α-Ga2O3 films grown with this method at Tsub > 550 °C are always insulating. Secondary-ion mass spectrometry confirms that both the insulating and conductive films have uniform silicon incorporation. In conductive films with 1019 ≤ NSi ≤ 1020 cm−3, the incorporated silicon is ∼100% electrically active. At NSi ≤ 1019 cm−3, the carrier concentration (n) plummets. A maximum Hall mobility (μ) = 90 cm2V·s at room-temperature is measured in a film with n = 2.9 × 1019 cm−3 and a maximum conductivity (σ) = 650 S/cm at room-temperature in a film with n = 4.8 × 1019 cm−3. A threading dislocation density of (5.6 ± 0.6) × 1010 cm−2 is revealed by scanning transmission electron microscopy, showing that there is still enormous room to improve the electrical properties of doped α-Ga2O3 thin films. 
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  3. Development of a high-performance, p-type oxide channel is crucial to realize all-oxide complementary metal–oxide semiconductor technology that is amenable to 3D integration. Among p-type oxides, α-SnO is one of the most promising owing to its relatively high hole mobility {as high as 21 cm2 V−1 s−1 has been reported [M. Minohara et al., J. Phys. Chem. C 124, 1755–1760 (2020)]}, back-end-of-line compatible processing temperature (≤400 °C), and good optical transparency for visible light. Unfortunately, doping control has only been demonstrated over a limited range of hole concentrations in such films. Here, we demonstrate systematic control of the hole concentration of α-SnO thin films via potassium doping. First-principles calculations identify potassium substitution on the tin site (KSn) of α-SnO to be a promising acceptor that is not (self)-compensated by native vacancies or potassium interstitials (Ki). We synthesize epitaxial K-doped α-SnO thin films with controlled doping concentration using suboxide molecular-beam epitaxy. The concentration of potassium is measured by secondary ion mass spectrometry, and its incorporation into the α-SnO structure is corroborated by x-ray diffraction. The effect of potassium doping on the optical response of α-SnO is measured by spectroscopic ellipsometry. Potassium doping provides systematic control of hole doping in α-SnO thin films over the 4.8 × 1017 to 1.5 × 1019 cm−3 range without significant degradation of hole mobility or the introduction of states that absorb visible light. Temperature-dependent Hall measurements reveal that the potassium is a shallow acceptor in α-SnO with an ionization energy in the 10–20 meV range. 
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  4. 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. 
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  5. Strain-engineering is a powerful means to tune the polar, structural, and electronic instabilities of incipient ferroelectrics. KTaO 3 is near a polar instability and shows anisotropic superconductivity in electron-doped samples. Here, we demonstrate growth of high-quality KTaO 3 thin films by molecular-beam epitaxy. Tantalum was provided by either a suboxide source emanating a TaO 2 flux from Ta 2 O 5 contained in a conventional effusion cell or an electron-beam-heated tantalum source. Excess potassium and a combination of ozone and oxygen (10% O 3 + 90% O 2 ) were simultaneously supplied with the TaO 2 (or tantalum) molecular beams to grow the KTaO 3 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 SrTiO 3 (001) and GdScO 3 (110) substrates. 
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  6. We report the use of suboxide molecular-beam epitaxy ( S-MBE) to grow β-Ga 2 O 3 at a growth rate of ∼1 µm/h with control of the silicon doping concentration from 5 × 10 16 to 10 19  cm −3 . In S-MBE, pre-oxidized gallium in the form of a molecular beam that is 99.98% Ga 2 O, i.e., gallium suboxide, is supplied. Directly supplying Ga 2 O to the growth surface bypasses the rate-limiting first step of the two-step reaction mechanism involved in the growth of β-Ga 2 O 3 by conventional MBE. As a result, a growth rate of ∼1 µm/h is readily achieved at a relatively low growth temperature ( T sub ≈ 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 SiO 2 ) producing an SiO suboxide molecular beam are used to dope the β-Ga 2 O 3 layers. Temperature-dependent Hall effect measurements on a 1 µm thick film with a mobile carrier concentration of 2.7 × 10 17  cm −3 reveal a room-temperature mobility of 124 cm 2  V −1  s −1 that increases to 627 cm 2  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-Ga 2 O 3 films grown by S-MBE at growth rates of ∼1 µm/h. 
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  7. 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 frst 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 flms with high structural perfection and smooth surfaces (rms roughness of <2 nm on ∼1 μm thick flms). 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 flm 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 feld-effect transistors made from these silicon-doped β-Ga2O3 flms grown by S-MBE at growth rates of ∼1 μm/h. 
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