Hafnium oxide (HfO x )-based memristive devices have tremendous potential as nonvolatile resistive random access memory (RRAM) and in neuromorphic electronics. Despite its seemingly simple two-terminal structure, a myriad of RRAM devices reported in the rapidly growing literature exhibit rather complex resistive switching behaviors. Using Pt/HfO x /TiN-based metal-insulator-metal structures as model systems, it is shown that a well-controlled oxygen stoichiometry governs the filament formation and the occurrence of multiple switching modes. The oxygen vacancy concentration is found to be the key factor in manipulating the balance between electric field and Joule heating during formation, rupture (reset), and reformation (set) of the conductive filaments in the dielectric. In addition, the engineering of oxygen vacancies stabilizes atomic size filament constrictions exhibiting integer and half-integer conductance quantization at room temperature during set and reset. Identifying the materials conditions of different switching modes and conductance quantization contributes to a unified switching model correlating structural and functional properties of RRAM materials. The possibility to engineer the oxygen stoichiometry in HfO x will allow creating quantum point contacts with multiple conductance quanta as a first step toward multilevel memristive quantum devices.
We have investigated the resistive switching behavior in stoichiometric HfO2 and oxygen-deficient HfO2−x thin films grown on TiN electrodes using reactive molecular beam epitaxy. Oxygen defect states were controlled by the flow of oxygen radicals during thin film growth. Hard X-ray photoelectron spectroscopy confirmed the presence of sub-stoichiometric hafnium oxide and defect states near the Fermi level. The oxygen deficient HfO2−x thin films show bipolar switching with an electroforming occurring at low voltages and low operating currents, paving the way for almost forming-free devices for low-power applications.
We have synthesized highly oxygen deficient HfO2−x thin films by controlled oxygen engineering using reactive molecular beam epitaxy. Above a threshold value of oxygen vacancies, p-type conductivity sets in with up to 6 times 10 21 charge carriers per cm 3 . At the same time, the band-gap is reduced continuously by more than 1 eV. We suggest an oxygen vacancy induced p-type defect band as origin of the observed behavior.
The superconductivity phase diagrams of electron doped cuprates of the form R2−xCexCuO4 (with R = La, Pr, Nd, Sm, and Eu) have been determined for cerium compositions 0 < x < 0.36 in a consistent series of epitaxial thin films grown by reactive molecular beam epitaxy (MBE). The use of epitaxial thin films allows the growth of materials away from thermodynamical equilibrium expanding the accessible phase space beyond the availability of bulk material. The superconducting phase space systematically increases with the rare earth ionic size. The doping concentration where the maximal transition temperature occurs in La2−xCexCuO4 is considerably shifted to lower doping (x ∼ 0.09) compared to La2−xSrxCuO4 (x ∼ 0.15). At the same time, the width of the superconducting region is broadened.
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We have investigated the material and electrical properties of tantalum oxide thin films (TaOx) with engineered oxygen contents grown by RF-plasma assisted molecular beam epitaxy. The optical bandgap and the density of the TaOx films change consistently with oxygen contents in the range of 3.63 to 4.66 eV and 12.4 to 9.0 g/cm3, respectively. When exposed to atmosphere, an oxidized Ta2O5-y surface layer forms with a maximal thickness of 1.2 nm depending on the initial oxygen deficiency of the film. X-ray photoelectron spectroscopy studies show that multiple sub-stoichiometric compositions occur in oxygen deficient TaOx thin films, where all valence states of Ta including metallic Ta are possible. Devices of the form Pt/Ta2O5-y/TaOx/TiN exhibit highly tunable forming voltages of 10.5 V to 1.5 V with decreasing oxygen contents in TaOx. While a stable bipolar resistive switching (BRS) occurs in all devices irrespective of oxygen content, unipolar switching was found to coexist with BRS only at higher oxygen contents, which transforms to a threshold switching behaviour in the devices grown under highest oxidation.
We have conducted a detailed thin film growth structure of oxygen engineered monoclinic HfO 2±x grown by reactive molecular beam epitaxy (MBE). The oxidation conditions induce a switching between (111) and (002)
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