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arXiv:1712.01581 · Scientific Reports

Correlating the nanostructure of Al-oxide with deposition conditions and dielectric contributions of two-level systems in perspective of superconducting quantum circuits

Stefan Fritz, Arnold Seiler, Lucas Radtke, Reinhard Schneider, Martin P. Weides, G. Weiß, Dagmar Gerthsen

Published May 15, 2018• 35 citations
arXivHTMLPDF

Abstract

Abstract This work is concerned with Al/Al-oxide(AlOx)/Al-layer systems which are important for Josephson-junction-based superconducting devices such as quantum bits. The device performance is limited by noise, which has been to a large degree assigned to the presence and properties of two-level tunneling systems in the amorphous AlOx tunnel barrier. The study is focused on the correlation of the fabrication conditions, nanostructural and nanochemical properties and the occurrence of two-level tunneling systems with particular emphasis on the AlOx-layer. Electron-beam evaporation with two different processes and sputter deposition were used for structure fabrication, and the effect of illumination by ultraviolet light during Al-oxide formation is elucidated. Characterization was performed by analytical transmission electron microscopy and low-temperature dielectric measurements. We show that the fabrication conditions have a strong impact on the nanostructural and nanochemical properties of the layer systems and the properties of two-level tunneling systems. Based on the understanding of the observed structural characteristics, routes are suggested towards the fabrication of Al/AlOx/Al-layers systems with improved properties.

DOI
10.1038/s41598-018-26066-4

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Progettazione e sviluppo di un processo bridge-free per la realizzazione di giunzioni Josephson per applicazioni di quantum computing

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The present thesis focuses on the laboratory fabrication of Al/AlOₓ/Al Josephson junctions using a bridge-free shadow evaporation technique, developed within the broader context of superconducting technologies for quantum computing. The interest in such devices arises from the central role played by the Josephson junction in superconducting qubits: unlike a purely harmonic LC oscillator, characterized by equally spaced energy levels, the presence of the junction introduces a nonlinearity that leads to an anharmonic energy spectrum. This allows for the selective addressing of the fundamental transition, which is a necessary condition for implementing a circuit-based qubit. In this framework, the quality of the AlOₓ tunnel barrier and of the metal interfaces is of crucial importance, as it directly affects not only the static electrical parameters of the junction but also dielectric losses and, more generally, the performance of the device in quantum applications. Following a theoretical overview of superconducting qubits and the physics of Al/AlOₓ/Al Josephson junctions, the work focuses on the experimental implementation and optimization of a bridge-free fabrication approach, adopted as an alternative to conventional suspended-bridge techniques. This method preserves the advantages of in-situ shadow evaporation for barrier formation while replacing the mechanical fragility of the suspended bridge with a geometrical control of the resist undercut. The operating principle relies on engineering an asymmetric profile in a bilayer resist system such that, during the two angled evaporations, only one deposition reaches the substrate along the connection lines, while the other is deposited on the resist sidewalls and subsequently removed during lift-off. In the central region, the overlap of the two evaporated aluminum layers, separated by an intermediate oxidation step, defines the Al/AlOₓ/Al superconductor–insulator–superconductor structure. This approach results in a more robust masking scheme compared to suspended-bridge processes, albeit at the cost of increased sensitivity to the precise definition and reproducibility of the undercut. The experimental activity was structured in several stages. First, the positive resists PMMA and MMA, used to form the bilayer lithographic stack, were characterized in order to determine their response as a function of electron-beam exposure dose and development conditions. A calibration mask consisting of an array of square patterns exposed at varying doses was employed to extract contrast curves and identify suitable exposure parameters. The development depth was quantitatively measured using atomic force microscopy (AFM), enabling a direct correlation between exposure dose and resulting resist profile. This step proved essential for selecting the most appropriate resist configuration capable of producing a controlled undercut compatible with the requirements of the bridge-free process. Subsequently, the lithographic process and evaporation geometry were calibrated through iterative refinement of the mask design, exposure parameters, and development conditions. Cross-sectional analysis, obtained via controlled sample cleaving followed by scanning electron microscopy (SEM), played a key role in assessing the three-dimensional profile of the resist, verifying the presence and quality of the undercut, and identifying potential structural instabilities such as resist collapse. At the same time, modifications were introduced to the evaporation system to enable deposition at the desired angles. This required the design of a new sample holder and a complete recalibration of the quartz crystal microbalance, as the altered geometry significantly affected the relationship between the nominal thickness reading and the actual film thickness deposited on the sample. A further important aspect of the work involved the progressive design and optimization of the full device mask, including contact pads, alignment markers, and the active junction region. The evolution of the layout, from initial test structures to the final configuration, was guided by experimental observations of pattern distortions and dose non-uniformities. It was found that the writing order of the electron-beam lithography pattern generator could significantly influence the final pattern quality, introducing systematic variations in feature definition. To mitigate this effect, a constrained writing sequence was implemented, ensuring improved reproducibility of the exposure process. Once all process parameters were stabilized, a comprehensive Standard Operating Procedure (SOP) was established, covering both the fabrication of Cr/Au contact structures and the subsequent lithography, angled evaporation, oxidation, and lift-off steps required for the realization of the Josephson junction. Finally, prior to fabricating fully oxidized junctions, a preliminary electrical validation of the process was carried out by producing test structures without the intermediate oxidation step. This allowed for the verification of electrical continuity in the aluminum structures. Measurements performed using a probe station confirmed ohmic behavior and the absence of macroscopic discontinuities in the conduction path. 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The main contribution of the thesis lies in transforming a conceptual fabrication approach into a structured and reproducible experimental procedure, based on resist characterization, cross-sectional analysis, instrumental recalibration, and preliminary electrical validation. The results obtained provide a solid foundation for further optimization of the tunnel barrier, cryogenic characterization, and integration of these junctions into superconducting circuits for quantum computing applications.

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Abstract This work is concerned with Al/Al-oxide(AlOx)/Al-layer systems which are important for Josephson-junction-based superconducting devices such as quantum bits. The device performance is limited by noise, which has been to a large degree assigned to the presence and properties of two-level tunneling systems in the amorphous AlOx tunnel barrier. The study is focused on the correlation of the fabrication conditions, nanostructural and nanochemical properties and the occurrence of two-level tunneling systems with particular emphasis on the AlOx-layer. Electron-beam evaporation with two different processes and sputter deposition were used for structure fabrication, and the effect of illumination by ultraviolet light during Al-oxide formation is elucidated. Characterization was performed by analytical transmission electron microscopy and low-temperature dielectric measurements. We show that the fabrication conditions have a strong impact on the nanostructural and nanochemical properties of the layer systems and the properties of two-level tunneling systems. Based on the understanding of the observed structural characteristics, routes are suggested towards the fabrication of Al/AlOx/Al-layers systems with improved properties.
As one of the candidates for realizing quantum bits, superconducting quantum bits, based on Josephson junction, have the advantages of easy integrating, coupling with the outside environment and so on. Double-layer photoresist was used to prepare suspended shadow mask by deep ultra-violet (DUV) lithography. We fabricated the sample of superconducting flux quantum bits by electron beam evaporation and static oxidization with aluminum as superconducting material. According to the dependence of the flatness on the thickness of aluminum film, we select 60 nm as the thickness of the bottom electrode of tunnel junction. By increasing the distance between the evaporation source and the substrate, we have improved the smoothness of film and thus reduced the leakage current of tunnel junction. The tri-layer structure of aluminum tunnel junction was observed by transmission electron microscopy (TEM), and the relationship between the thickness of barrier layer and the oxidation pressure was obtained.
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.
Superconducting qubits based on Al/AlOx/Al Josephson junction are one of the most promising candidates for the physical implementation of universal quantum computers. Due to scalability and compatibility with the state-of-the-art nanoelectronic processes one can fabricate hundreds of qubits on a single silicon chip. However, decoherence in these systems caused by two-level-systems in amorphous dielectrics, including a tunneling barrier AlOx, is one of the major problems. We report on a Josephson junction thermal annealing process development to crystallize an amorphous barrier oxide (AlOx). The dependences of the thermal annealing parameters on the room temperature resistance are obtained. The developed method allows not only to increase the Josephson junction resistance by 175%, but also to decrease by 60% with precisions of 10% in Rn. Finally, theoretical assumptions about the structure modification in tunnel barrier are proposed. The suggested thermal annealing approach can be used to form a stable and reproducible tunneling barriers and scalable frequency trimming for a widely used fixed-frequency transmon qubits.
An ultra-thin aluminum oxide layer is a key component for Josephson junctions (JJ) in superconducting quantum bits (qubits). This layer serves as a barrier layer for Cooper pairs tunneling between the superconducting electrodes and significantly influences the overall performance of the junction. In this study, we investigate the impact of aluminum deposition rates on the microstructure and chemical variation of the aluminum oxide layer, as well as the device’s yields and qubits’ lifetimes. Surprisingly, although the oxide layer roughness and thickness variation improve noticeably with an increasing Al deposition rate from 0.5 Å/s to 5 Å/s, the qubit’s coherence time is almost unchanged. We attribute this to the fact that Cooper pairs tunnel only through the thinnest region of the barrier. Additionally, we revealed a stress-induced grain boundary sliding short-circuit failure mechanism in the JJ. Our discovery provides a vital understanding of oxide microstructure and JJ functionality, which are critical for improving the coherence time of superconducting qubits.
Abstract Tunneling defects in disordered materials form spurious two-level systems which are a major source of decoherence for micro-fabricated quantum devices. For superconducting qubits, defects in tunnel barriers of submicrometer-sized Josephson junctions couple strongest to the qubit, which necessitates optimization of the junction fabrication to mitigate defect formation. Here, we investigate whether defects appear predominantly at the edges or deep within the amorphous tunnel barrier of a junction. For this, we compare defect densities in differently shaped Al/AlO x /Al Josephson junctions that are part of a Transmon qubit. We observe that the number of detectable junction-defects is proportional to the junction area, and does not significantly scale with the junction’s circumference, which proposes that defects are evenly distributed inside the tunnel barrier. Moreover, we find very similar defect densities in thermally grown tunnel barriers that were formed either directly after the base electrode was deposited, or in a separate deposition step after removal of native oxide by Argon ion milling.
The present thesis focuses on the laboratory fabrication of Al/AlOₓ/Al Josephson junctions using a bridge-free shadow evaporation technique, developed within the broader context of superconducting technologies for quantum computing. The interest in such devices arises from the central role played by the Josephson junction in superconducting qubits: unlike a purely harmonic LC oscillator, characterized by equally spaced energy levels, the presence of the junction introduces a nonlinearity that leads to an anharmonic energy spectrum. This allows for the selective addressing of the fundamental transition, which is a necessary condition for implementing a circuit-based qubit. In this framework, the quality of the AlOₓ tunnel barrier and of the metal interfaces is of crucial importance, as it directly affects not only the static electrical parameters of the junction but also dielectric losses and, more generally, the performance of the device in quantum applications. Following a theoretical overview of superconducting qubits and the physics of Al/AlOₓ/Al Josephson junctions, the work focuses on the experimental implementation and optimization of a bridge-free fabrication approach, adopted as an alternative to conventional suspended-bridge techniques. This method preserves the advantages of in-situ shadow evaporation for barrier formation while replacing the mechanical fragility of the suspended bridge with a geometrical control of the resist undercut. The operating principle relies on engineering an asymmetric profile in a bilayer resist system such that, during the two angled evaporations, only one deposition reaches the substrate along the connection lines, while the other is deposited on the resist sidewalls and subsequently removed during lift-off. In the central region, the overlap of the two evaporated aluminum layers, separated by an intermediate oxidation step, defines the Al/AlOₓ/Al superconductor–insulator–superconductor structure. This approach results in a more robust masking scheme compared to suspended-bridge processes, albeit at the cost of increased sensitivity to the precise definition and reproducibility of the undercut. The experimental activity was structured in several stages. First, the positive resists PMMA and MMA, used to form the bilayer lithographic stack, were characterized in order to determine their response as a function of electron-beam exposure dose and development conditions. A calibration mask consisting of an array of square patterns exposed at varying doses was employed to extract contrast curves and identify suitable exposure parameters. The development depth was quantitatively measured using atomic force microscopy (AFM), enabling a direct correlation between exposure dose and resulting resist profile. This step proved essential for selecting the most appropriate resist configuration capable of producing a controlled undercut compatible with the requirements of the bridge-free process. Subsequently, the lithographic process and evaporation geometry were calibrated through iterative refinement of the mask design, exposure parameters, and development conditions. Cross-sectional analysis, obtained via controlled sample cleaving followed by scanning electron microscopy (SEM), played a key role in assessing the three-dimensional profile of the resist, verifying the presence and quality of the undercut, and identifying potential structural instabilities such as resist collapse. At the same time, modifications were introduced to the evaporation system to enable deposition at the desired angles. This required the design of a new sample holder and a complete recalibration of the quartz crystal microbalance, as the altered geometry significantly affected the relationship between the nominal thickness reading and the actual film thickness deposited on the sample. A further important aspect of the work involved the progressive design and optimization of the full device mask, including contact pads, alignment markers, and the active junction region. The evolution of the layout, from initial test structures to the final configuration, was guided by experimental observations of pattern distortions and dose non-uniformities. It was found that the writing order of the electron-beam lithography pattern generator could significantly influence the final pattern quality, introducing systematic variations in feature definition. To mitigate this effect, a constrained writing sequence was implemented, ensuring improved reproducibility of the exposure process. Once all process parameters were stabilized, a comprehensive Standard Operating Procedure (SOP) was established, covering both the fabrication of Cr/Au contact structures and the subsequent lithography, angled evaporation, oxidation, and lift-off steps required for the realization of the Josephson junction. Finally, prior to fabricating fully oxidized junctions, a preliminary electrical validation of the process was carried out by producing test structures without the intermediate oxidation step. This allowed for the verification of electrical continuity in the aluminum structures. Measurements performed using a probe station confirmed ohmic behavior and the absence of macroscopic discontinuities in the conduction path. The measured resistance values were higher than those predicted using bulk aluminum resistivity; however, this discrepancy is consistent with the well-known behavior of thin evaporated films, in which surface scattering, grain boundaries, and interface effects lead to an increased effective resistivity. Although these measurements do not yet constitute a full characterization of the Josephson junction in the quantum regime, they provide an essential validation of the fabrication process and the structural integrity of the devices. In conclusion, this work enabled the development and calibration of a bridge-free fabrication process for Al/AlOₓ/Al Josephson junctions, highlighting the strong interplay between lithographic control, evaporation geometry, barrier formation, and electrical response. The main contribution of the thesis lies in transforming a conceptual fabrication approach into a structured and reproducible experimental procedure, based on resist characterization, cross-sectional analysis, instrumental recalibration, and preliminary electrical validation. The results obtained provide a solid foundation for further optimization of the tunnel barrier, cryogenic characterization, and integration of these junctions into superconducting circuits for quantum computing applications.