Abstract Aluminum (Al) is the most critical material in the burgeoning field of superconducting quantum computing due to its self-limiting native oxide and reliable Josephson effect. However, material-induced decoherence remains a major bottleneck currently limits the scalability of quantum processors. As highlighted in seminal roadmaps, dielectric loss from amorphous interfaces and structural defects in standard evaporated Al films are the primary sources of noise. While current international efforts focus on engineering-level mitigation (e.g., circuit design), this review proposes a materials-level solution through the lens of research conducted in Taiwan. We will focus on the paradigm shift enabled by molecular beam epitaxy (MBE) growth of ultrahigh-quality Al nanofilms. Unlike traditional “dirty-limit” superconductors where transition temperature (Tc) increases are linked to disorder, researchers in Taiwan have demonstrated a doubling of Tc (reaching ≈ 2.4 K) in the ultraclean limit. We will discuss the underlying physics, such as surface phonon softening and quantum size effects, and why these clean-limit films are superior for practical applications. Notably, in situ Al2O3 passivation ensures long-term environmental stability, enabling MBE-grown-Al-based resonators to maintain internal quality factors exceeding 106 even after extended air exposure. Current literature frequently reviews atomic layer deposition (ALD) or disordered “granular aluminum” for high kinetic inductance. However, there is a significant gap in surveying epitaxial, wafer-scale Al for applied devices. Our review aims to provide a balanced global survey, showcasing how the synergy between MBE expertise and low-temperature physics in Taiwan provides a viable technological pathway to address the materials challenges of the quantum era.
Abstract Aluminum (Al) is the most critical material in the burgeoning field of superconducting quantum computing due to its self-limiting native oxide and reliable Josephson effect. However, material-induced decoherence remains a major bottleneck currently limits the scalability of quantum processors. As highlighted in seminal roadmaps, dielectric loss from amorphous interfaces and structural defects in standard evaporated Al films are the primary sources of noise. While current international efforts focus on engineering-level mitigation (e.g., circuit design), this review proposes a materials-level solution through the lens of research conducted in Taiwan. We will focus on the paradigm shift enabled by molecular beam epitaxy (MBE) growth of ultrahigh-quality Al nanofilms. Unlike traditional “dirty-limit” superconductors where transition temperature (Tc) increases are linked to disorder, researchers in Taiwan have demonstrated a doubling of Tc (reaching ≈ 2.4 K) in the ultraclean limit. We will discuss the underlying physics, such as surface phonon softening and quantum size effects, and why these clean-limit films are superior for practical applications. Notably, in situ Al2O3 passivation ensures long-term environmental stability, enabling MBE-grown-Al-based resonators to maintain internal quality factors exceeding 106 even after extended air exposure. Current literature frequently reviews atomic layer deposition (ALD) or disordered “granular aluminum” for high kinetic inductance. However, there is a significant gap in surveying epitaxial, wafer-scale Al for applied devices. Our review aims to provide a balanced global survey, showcasing how the synergy between MBE expertise and low-temperature physics in Taiwan provides a viable technological pathway to address the materials challenges of the quantum era.
Achieving high material perfection in aluminum (Al) films and their associated Al/AlOx heterostructures is essential for enhancing the coherence time in superconducting quantum circuits. We grew Al films with thicknesses ranging from 3 to 30 nanometers (nm) epitaxially on sapphire substrates using molecular beam epitaxy (MBE). An integral aspect of our work involved electron-beam (e-beam) evaporation to directly deposit aluminum oxide (Al2O3) films on the freshly grown ultrathin epitaxial Al films in an ultra-high-vacuum (UHV) environment. This in situ oxide deposition is critical for preventing the oxidation of parts of the Al films, avoiding the formation of undesired native oxides, and thereby preserving the nm-thick Al films in their pristine conditions. The thicknesses of our Al films in the study were accurately determined; for example, coherence lengths of 3.0 and 20.2 nm were measured in the nominal 3.0 and 20 nm thick Al films, respectively. These Al films were epitaxially grown on sapphire substrates, showing an orientational relationship, denoted as Al(111)⟨21¯1¯⟩∥sapphire(0001)[21¯1¯0]. The Al/sapphire interface was atomically ordered without any interfacial layers, as confirmed by in situ reflection high-energy electron diffraction (RHEED) and cross-sectional scanning transmission electron microscopy (STEM). All sample surfaces exhibited smoothness with a roughness in the range of 0.1–0.2 nm. The Al films are superconducting with critical temperatures ranging from 1.23 to around 2 K, depending on the film thickness.
The performance and coherence of superconducting quantum systems are fundamentally tied to the quality of the materials from which they are built. In superconducting transmon qubits, many loss mechanisms and sources of decoherence originate from material imperfections or unwanted oxide formation. Likewise, semiconductor–superconductor hybrid systems depend on high-quality interfaces to ensure strong coupling between electronic states in the two materials. In such hybrid devices, the accessible operating regime is often dictated by the intrinsic material properties of either the semiconductor or the superconductor. Advancing quantum device performance therefore requires exploring new material systems and optimizing their physical characteristics. In this thesis, we present the development of several superconducting material platforms for quantum technologies, including superconducting qubits, single-photon detectors, and semiconductor superconductor hybrid devices. We focus on the growth and characterization of superconducting films and heterostructures, and we establish clear connections between their material properties and the resulting device performance. First, we will present a novel semiconductor-superconductor hybrid material based on in-situ deposited epitaxial layers of Nb and Al on a shallow InAs quantum well. In this structure, the Al interlayer provides an epitaxial connection between an in-situ magnetron sputtered Nb or NbTi thin film and a shallow InAs two dimensional electron gas. This metal-to-metal epitaxy is achieved by optimization of the material stack and results in an induced superconducting gap of approximately 1 meV, determined from transport measurements of superconductor semiconductor Josephson junctions. This induced gap is approximately five times larger than the values reported for Al-based hybrid materials and indicates the formation of highly-transparent interfaces that are required in high-quality hybrid material platforms. Then, we discuss a different approach in the next chapter where we develop a hybrid material based on a molecular beam epitaxy grown InAsSb surface quantum well with an in-situ deposited Nb layer directly on top of the quantum well. Relative to conventional Al-InAs based systems, the InAsSb surface quantum well offers a lower effective mass and stronger spin-orbit interaction, while the Nb layer has a higher critical temperature and a larger critical magnetic field. The in-situ deposition of the Nb layer directly on top of the quantum well results in a high-quality interface that enables strong coupling to the InAsSb quantum well. Transport measurements on Josephson junctions reveal an induced superconducting gap of 1.3 meV and a critical current density of 3.75 × 10³A/cm². Furthermore, a planar asymmetric SQUID is realized, exhibiting gate-tunable superimposed oscillations originating from both the individual Josephson junction and the full SQUID loop. The large induced superconducting gap combined with strong spin-orbit interaction position this material as an attractive platform for experiments exploring gate-tunable superconductivity and topological superconducting devices. In the next chapter, we will focus on establishing a link between Nb film crystal properties and their performance in superconducting circuits. In this study, we investigate the microwave properties of niobium resonators with different crystalline properties and related surface topographies. We analyze a series of magnetron sputtered films in which the Nb crystal orientation and surface topography are changed by varying the substrate temperatures between room temperature and 975 K. The lowest-loss resonators that we measure have quality factors of over 10⁶ at single-photon powers, among the best ever recorded using the Nb on sapphire platform. We observe the highest quality factors in films grown at an intermediate temperature regime of the growth series (550 K) where the films display both preferential ordering of the crystal domains and low surface roughness. Furthermore, we analyze the temperature-dependent behavior of our resonators to learn about how the quasi-particle density in the Nb film is affected by the niobium crystal structure and the presence of grain boundaries. Then, we explore yet a different material platform by attempting to realize onchip NbTiN single photon detectors on LiNbO₃, an emerging photonic platform with high potential for scalable quantum information processing. We use DC reactive magnetron sputtering to grow high-quality NbTiN thin films and investigate the impact of substrate temperature during NbTiN growth. We achieve four nm thick superconducting films with a critical temperature (𝑇𝑐) of 12.3 K grown at a substrate temperature of 825 K. We demonstrate that the increased substrate temperature reduces the oxygen concentration in our films and improves the overall stoichiometry. In addition, we integrate these films with the LiNbO3 platform and investigate the obtained interface quality. Finally, we fabricate superconducting nanowire single photon detectors from the NbTiN film on LiNbO₃ and characterize the detector performance. Lastly, we report a gate-tunable Josephson diode effect in hybrid nanowire junctions consisting of a spin-orbit-coupled semiconductor core coated with epitaxial ferromagnetic insulator and superconductor shells. The wires display a hysteretic superconducting window as a function of axial magnetic field. In the superconducting regime, the devices exhibit nonreciprocal current transport, with the diode efficiency showing a strong dependence on back-gate voltage. The effect persists in a remanent magnetization state following a controlled demagnetization procedure, establishing zero-field operation. The combination of results presented in this thesis stress the importance of a material-focused approach in advancing the performance of quantum hardware. The novel hybrid material platforms developed in this thesis expand the operating regime of devices, which could enable future experiments involving gate-tunable superconductivity or topological properties. Similarly, we demonstrate that optimizing superconductor crystal structure benefits quantum devices, such as single-photon detectors and superconducting resonators.
I hereby declare that I am the sole author of this thesis. This is a true copy of the thesis, including any required final revisions, as accepted by my examiners. I understand that my thesis may be made electronically available to the public. ii The growth of Aluminum (Al) on semiconductors and dielectrics is a cornerstone in the quest for scalable quantum computing systems. Indeed the electrical properties of Al make it an exceptional candidate for the realization of superconducting resonators, pivotal tools for understanding and operating superconducting qubits. Such resonators have been fabricated recently on Sapphire substrates, using Molecular Beam Epitaxy (MBE), and displayed quality factors above a million. Complementary studies of these resonators have demonstrated that the metal-substrate interface was the primary source of decoherence and losses, highlighting the importance of pristine interfaces (free of contaminants), and high quality epitaxial growth in order to minimize the native defects level. In this work we investigate different substrate materials in order to yield equivalent or higher qual-
This is a study of the growth of titanium-nitride (TiN) by plasma assisted molecular beam epitaxy (MBE) for applications in low loss quantum circuits. Titanium nitride is a material known to have low loss at microwave frequencies which sees practical use in many emerging quantum device architectures. The goal of this research is to investigate improvements in TiN thin films utilizing MBE to produce highly pure, highly crystalline films. A review of the theory of superconducting qubits is given and recent developments in superconducting qubit research are summarized to elucidate how loss has been reduced historically and the importance of materials improvements to the future of scalable quantum computation. The dynamics of epitaxial film growth are discussed, focusing on the formation of a minimum energy surface, the thermally driven kinetics of atoms deposited on the surface, and how these lead to the formation of large scale crystalline domains in the film. An overview of the MBE growth chamber is given and the growth procedure for TiN is discussed. Transport and morphology measurement results are discussed for MBE TiN where, for optimized growth conditions, films are highly crystalline with superconducting transition temperatures(Tc) as high as Tc = 6.1K, matching the value for bulk crystals and exceeding all reported thin film values. Microwave loss measurements of transmission line resonators fabricated from these films are shown to have low-power quality factors(Q) as high as 200,000 and an increase to Q = 400,000 at high power, consistent with the saturation of two-level-systems (TLS) at high power. These results confirm a connection between the high quality crystalline materials produced in this work and low loss in quantum circuits.
Quantum computing is a very interesting field, due to the ability of quantum computers to solve many problems much faster than a classical computer. Superconducting qubits are electronic circuits composed of superconducting capacitors, inductors and Josephson junctions, which can implement a physical qubit. However they need improvements in their coherence time to create a viable quantum computing. In this work I study the effect on decoherence caused by two level systems in the native oxide that forms on the surface of qubit. To this end I fabricate 3D transmon qubits using materials grown my molecular beam epitaxy, to which a variety of different surface treatments had been applied. I began by fabricating qubits from niobium/aluminum oxide/niobium trilayers. To this end I developed a self-aligned process for fabricating sub-micron Josephson junctions. This process presented many challenges. During the development of this process, it became clear that niobium was an inferior material for fabricating qubits compared to aluminum. I then switched to making qubits from Aluminum. I began by studying the growth of aluminum on sapphire, and was able to achieve aluminum films with an RMS roughness of 0.2 nm by growing on c-plane sapphire that had been annealed in oxygen at 1100 °C and dipped in BOE. Next I fabricated 3D transmon qubits by adapting the standard shadowmask process for use with MBE. I fabricated qubits with a long in situ oxidation to fully passivate the surface before exposure to air. I also passivated the surface by means of growing co deposited aluminum oxide, and by grown aluminum nitride using a nitrogen plasma source. The coherence times of these qubits were compared to those a control sample that had been exposed to air immediately after growth. Overall it doesn’t appear that cladding the surface changes the coherence time much, however it is difficult to form conclusions with this small sample size. The coated samples appeared to have slightly longer coherence times than the untreated samples, with diffusive oxidation and coating with aluminum oxide providing the largest increase in T1 and diffusive oxidation providing the largest increase in T2.
Novel isotopically enriched and aluminum (Al) delta-doped silicon crystals with exceptional material properties are proposed and developed, in an effort to bridge superconducting quantum information with silicon-based quantum devices for a new generation of solid-state quantum computing. Quantum computing platforms based on semiconducting and superconducting qubits are two powerful candidates. For semiconductor spin qubits, long coherence times can be achieved when using isotopically enriched 28Si as a host material. However, qubit coupling in semiconductor qubits is difficult to achieve due to the nanometer scale of the devices. For superconductor qubit devices, millimeter scale with long spatial coherence length makes them relatively easy to couple multiple qubits, but losses at the material interface are limiting the device performance. Our ultimate objective is to create a hybrid system where both Si spin qubits and superconductor qubits are coupled in a nuclear spin-free and interface-free material. To achieve this, a superconducting semiconductor with monocrystalline structure is proposed. One possible candidate is through Al delta-doped 28Si, as highly Al doped Si is expected to have a 10× higher critical temperature (Tc) than highly boron (B) doped Si (Tc ≈ 0.6 K). The focus of this thesis is to attack two materials limitations for realizing a monocrystalline, super-semiconducting hybrid architecture: 1) substantially reducing 29Si that limits coherence of semiconducting spin qubits and 2) exploring supersaturated, Al-doped silicon as a system for localized superconductivity within silicon with a potential Tc > 1K.In the first part of this thesis, we demonstrate the advancements in isotopically enriched 28Si in terms of chemical purity, enrichment, and electrical properties. In this work, a new, compact UHV version of the hyperthermal Penning ion source was designed and built. An improvement in the chemical purity from 98.47 % to 99.97 %, while maintaining a 28Si enrichment of > 99.999987 % (0.832 ppm 29Si) has been achieved. We broaden the material variety of 28Si at different levels in the quantum information community by demonstrating the ability to grow isotopically enriched 28Si epitaxial films with precisely controlled (≈ 90 % accuracy) enrichment levels, ranging from natural abundance to < 1 ppm 29Si. In addition, to better assess the quality of our 28Si material, we have successfully fabricated and measured 28Si MOSFET devices, and compared to those from natural abundance Si on the same substrate. The charge carrier mobility on isotopically enriched 28Si is found to be approximately a factor of 3 lower compared to the natural abundance Si, a result of the short-range scattering (impurity scattering). In the second part of this thesis, we report on the material growth and characterization of super-saturated Al delta layers in Si and explore the possibility for superconductivity. To reach a critical density needed for superconducting transition, the first step is to study the saturation density of this dopant and a way to confine it in 3D. Using a combination of different characterization tools, the maximum 2D atom density of one atomic layer of Al on Si(100) surface before cluster formation is found to be 3.4 × 1014 cm-2. We also studied the effects of different material growth methods on electrical conduction and the possibility of reaching higher 3D density of Al in this Si-Al-Si heterostructure. We found that Al delta doping in Si behaves differently compared to other dopants: the incorporation anneal does not change the dopant activation efficiency. Standard molecular beam epitaxy (MBE) and locking layer (LL) growth on Al layer is not successful and Al dopant activation is found to be < 50 %, most likely due to the tendency of Al atoms to move toward the surface and the cluster states been developed from the thermal anneals. The electrical conduction of this delta layer at low temperature is also studied and modeled using a temperature dependent two-carrier type model, which is the first reported conducting Al delta layer in Si. We believe that reaching the superconducting transition using an Al delta layer as a dopant in Si is possible, but this requires further studies both experimentally and theoretically to minimize the Al segregation in order to achieve a high enough 3D dopant density.