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Oxide heterostructures exhibit a vast variety of unique physical properties. Examples are unconventional superconductivity in layered nickelates and topological polar order in (PbTiO₃)_n/(SrTiO₃)_nsuperlattices. Although it is clear that variations in oxygen content are crucial for the electronic correlation phenomena in oxides, it remains a major challenge to quantify their impact. Here, we measure the chemical composition in multiferroic (LuFeO₃)₉/(LuFe₂O₄)₁superlattices, mapping correlations between the distribution of oxygen vacancies and the electric and magnetic properties. Using atom probe tomography, we observe oxygen vacancies arranging in a layered three-dimensional structure with a local density on the order of 10¹⁴cm⁻², congruent with the formula-unit-thick ferrimagnetic LuFe₂O₄layers. The vacancy order is promoted by the locally reduced formation energy and plays a key role in stabilizing the ferroelectric domains and ferrimagnetism in the LuFeO₃and LuFe₂O₄layers, respectively. The results demonstrate pronounced interactions between oxygen vacancies and the multiferroic order in this system and establish an approach for quantifying the oxygen defects with atomic-scale precision in 3D, giving new opportunities for deterministic defect-enabled property control in oxide heterostructures.

Transparent oxide thin film transistors (TFTs) are an important ingredient of transparent electronics. Their fabrication at the back‐end‐of‐line (BEOL) opens the door to novel strategies to more closely integrate logic with memory for data‐intensive computing architectures that overcome the scaling challenges of today's integrated circuits. A recently developed variant of molecular‐beam epitaxy (MBE) called suboxide MBE (S‐MBE) is demonstrated to be capable of growing epitaxial In₂O₃at BEOL temperatures with unmatched crystal quality. The fullwidth at halfmaximum of the rocking curve is 0.015° and, thus, ≈5x narrower than any reports at any temperature to date and limited by the substrate quality. The key to achieving these results is the provision of an In₂O beam by S‐MBE, which enables growth in adsorption control and is kinetically favorable. To benchmark this deposition method for TFTs, rudimentary devices were fabricated.

In bulk${\mathrm{Sr}}_2{\mathrm{RuO}}_4$, the strong sensitivity of the superconducting transition temperature$T_{\text{c}}$to nonmagnetic impurities provides robust evidence for a superconducting order parameter that changes sign around the Fermi surface. In superconducting epitaxial thin-film${\mathrm{Sr}}_2{\mathrm{RuO}}_4$, the relationship between$T_{\text{c}}$and the residual resistivity${\rho }_0$, which in bulk samples is taken to be a proxy for the low-temperature elastic scattering rate, is far less clear. Using high-energy electron irradiation to controllably introduce point disorder into bulk single-crystal and thin-film${\mathrm{Sr}}_2{\mathrm{RuO}}_4$, we show that$T_{\text{c}}$is suppressed in both systems at nearly identical rates. This suggests that part of${\rho }_0$in films comes from defects that do not contribute to superconducting pairbreaking and establishes a quantitative link between the superconductivity of bulk and thin-film samples.

Mott metal–insulator transitions possess electronic, magnetic, and structural degrees of freedom promising next‐generation energy‐efficient electronics. A previously unknown, hierarchically ordered, and anisotropic supercrystal state is reported and its intrinsic formation characterized in‐situ during a Mott transition in a Ca₂RuO₄thin film. Machine learning‐assisted X‐ray nanodiffraction together with cryogenic electron microscopy reveal multi‐scale periodic domain formation at and below the film transition temperature (T_Film ≈ 200–250 K) and a separate anisotropic spatial structure at and aboveT_Film. Local resistivity measurements imply an intrinsic coupling of the supercrystal orientation to the material's anisotropic conductivity. These findings add a new degree of complexity to the physical understanding of Mott transitions, opening opportunities for designing materials with tunable electronic properties.

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.

Low resistance non-alloyed ohmic contacts are realized by a metal-first process on homoepitaxial, heavily n+ doped (010) β-Ga2O3. The resulting contacts have a contact resistance (Rc) as low as 0.23 Ω-mm on an as-grown sample and exhibit nearly linear ohmic behavior even without a post-metallization anneal. The metal-first process was applied to form non-alloyed contacts on n+ (010) β-Ga2O3 grown by metal-organic chemical vapor deposition (MOCVD) as well as suboxide molecular beam epitaxy. Identical contacts fabricated on similar MOCVD samples by conventional liftoff processing exhibit highly rectifying Schottky behavior. Re-processing using the metal-first process after removal of the poor contacts by conventional methods does not improve the contacts; however, addition of a Ga-flux polishing step followed by re-processing using a metal-first process again results in low resistance, nearly linear ohmic contacts. The liftoff process, therefore, does not reliably render nearly linear ohmic behavior in non-alloyed contacts. Furthermore, no interface contamination was detected by x-ray photoelectron spectroscopy. This suggests that during the initial liftoff processing, a detrimental layer may form at the interface, likely modification of the Ga2O3 surface, that is not removable during the contact removal process but that can be removed by Ga-flux polishing.