Identifying the microscopic origins of decoherence sources prevalent in Josephson junction (JJ) based circuits is central to their use as functional quantum devices. Focussing on so called ‘strongly coupled’ two-level defects, we construct a theoretical model using the atomic position of the oxygen which is spatially delocalized in the oxide forming the JJ barrier. Using this model, we investigate which atomic configurations give rise to two-level behaviour of the type seen in experiments. We compute experimentally observable parameters for phase qubits and examine defect response under the effects of applied electric field and strain.
Superconducting quantum circuits are promising platforms for scalable quantum computing, where qubit coherence is critically determined by microscopic defects in the oxide tunneling barrier of Josephson junctions. Amorphous Al
2O
3 is widely used as a barrier material, but under irradiation, oxygen vacancy (V
O) defects are readily generated, introducing noise sources that accelerate qubit decoherence. We systematically investigate the structural characteristics and electronic impact of V
O defects in amorphous Al
2O
3 using first-principles calculations and \textit{ab initio} molecular dynamics. Our results show that both the coordination environment and concentration of V
Os strongly influence electrical conductivity. In particular, two- and three-coordinated V
Os, unique to the amorphous structure, enhance conductivity more than conventional four-coordinated vacancies. Increasing V
O concentration amplifies conductivity fluctuations, which we link to critical current noise in Josephson junctions. Using a noise model, we estimate that higher V
O densities lead to shorter qubit coherence times. These findings provide insights for radiation-hard design of superconducting quantum devices.
Environmental two-level systems (TLS) have been identified as significant decoherence sources in Josephson junction (JJ) based circuits. For such quantum devices to be functional, the removal or control of the TLS is a necessity. Understanding the microscopic origins of the 'strongly coupled' TLS type is one current path of investigation to that end. The delocalized oxygen model suggests the atomic position of an oxygen atom is spatially delocalized in the oxide forming the JJ barrier. In this report we extend this model from its previous 2+1D construction to a complete 3D description using a Wick-rotated time-dependent Schrodinger equation to solve for time-independent solutions in three dimensions. We compute experimentally observable parameters for phase qubits and compare the results to the 2+1D framework. We devise a Voronoi classification scheme to investigate oxygen atoms delocalizing within strained and non-strained crystalline lattices, as well as realistic atomic positions a JJ amorphous tunnel barrier constructed in previous density functional studies.
Constructing circuits which invoke the tunnelling effect of Josephson junctions in the superconducting regime manifest controllable, quantum properties. The development of a quantum computer employing these phenomena is just one of the many advantages to be gained from building such devices. However, the use of quantum bits for computation is dependent on the ability to operate them in an essentially isolated environment. The phenomenon of decoherence refers to the instability of a quantum state of a system when it interacts with the surrounding environment. Superconducting qubits are sensitive to decoherence mechanisms within the readout leads connecting to the device, and more importantly from the materials from which they are manufactured. Removal or control of these imperfections is required before quantum computers using superconducting circuit architecture can be realised. One identifiable noise source is the so called 'strongly coupled' two-level system (TLS). Comparable resonance frequencies to the qubit; strong coupling strengths and decoherence times long enough to allow coherent oscillations between the qubit and TLS have been experimentally measured. The premise of this thesis is that positional anharmonicity of oxygen atoms arises within the AlOx barrier of the Josephson junction solely due to its amorphous construction. This ansatz allows the existence of various spatial configurations throughout the layer, causing unique TLS properties based solely on atomic positions and rotation in relation to the external electric field. To validate this conjecture, Josepson junction models are constructed using a hybrid ab initio and molecular mechanics approach, with various stoichiometry and density properties to reflect experimental observations of the barrier. The resultant atomic positions provide input conditions through a Voronoi classification scheme to a framework describing an oxygen atom that has the capacity to become spatially delocalised as bonds perturb away from a crystalline structure. A direct digitalisation method is developed for low dimensional descriptions and a Wick-rotated time-dependent Schrödinger equation implementation is used for three dimensional investigations. Calculated properties are compared to many current experimental strongly coupled TLS measurements in phase qubits, which shows the models' capacity to explain how an oxygen atom can generate a large dipole and appropriate ground to first excited state splitting values expected of a TLS by merely migrating from its preferred lattice position.
Al/AlOx/Al Josephson junctions are the building blocks of a wide range of superconducting quantum devices that are key elements for quantum computers, extremely sensitive magnetometers and radiation detectors. The properties of the junctions and the superconducting quantum devices are determined by the atomic structure of the tunnel barrier. The nanoscale dimension and disordered nature of the barrier oxide have been challenges for the direct experimental investigation of the atomic structure of the tunnel barrier. Here we show that the miniaturized dimension of the barrier and the interfacial interaction between crystalline Al and amorphous AlOx give rise to oxygen deficiency at the metal/oxide interfaces. In the interior of the barrier, the oxide resembles the atomic structure of bulk aluminium oxide. Atomic defects such as oxygen vacancies at the interfaces can be the origin of the two-level systems and contribute to decoherence and noise in superconducting quantum circuits.
Quantum computation is a fascinating field that combines novel physics with improvements in computation times and has been rapidly growing in the past few years. Using superconductors to form the qubits has the potential for large-scale computing, if the decoherence inherent in these devices can be understood and reduced. Two-level fluctuators due to defects in the materials are thought to cause changes to the Josephson critical current or the flux through the superconducting loop of a flux qubit, which leads to decoherence in the qubit. Alternatively, defects in the crystal lattice give rise to electron localization which in turn traps spins with random orientations at the substrate/metal interface, again producing decoherence. My work studied the proposed noise mechanisms by using Molecular Beam Epitaxy to fabricate single-crystal niobium-based Josephson junctions. Using RHEED, AFM, and TEM/STEM, I studied the epitaxy of the niobium film at the substrate interface to reduce noise due to crystal defects. I then measured flux noise in these films; the noise in the epitaxial films is lower than the comparative polycrystalline films. Further measurements using ex-situ Josephson junctions and epitaxial niobium loops resulted in the lowest reported flux noise measurements to date. Additionally, EELS measurements made in the course of the STEM analysis of the crystal structure reveal oxygen depletion from the substrate at elevated growth temperatures. This depletion leads to oxygen vacancies in the aluminum oxide substrate, which can in turn lead to charge traps at the substrate/metal interface and hence to decoherence in the qubit. Critical current noise was investigated by changing the oxidation dose of the alumina barrier in more than 50 separate Josephson junctions. Films which were grown with lower oxidation doses have a non-ideal critical current temperature dependence as well as higher critical current noise values, suggesting that insufficient oxygen is being incorporated into these junctions. Finally, I studied the effect of surface cleaning after fabrication for resonators and transmons. Microscopy shows that an oxygen ash and BOE dip together removes all photoresist residue from the chip. Internal-Q measurements do not show a marked improvement due to this cleaning, but the coherence times do improve upon the cleaning step.