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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. 

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.