Nanometer-thick molecular beam epitaxy Al films capped with in situ deposited Al2O3—High-crystallinity, morphology, and superconductivity
Y.H. Lin, C. K. Cheng, L. B. Young, Li-Hung Chiang, Wan-Sin Chen, Kuan-Hui Lai, Shao-Pin Chiu, Chien‐Ting Wu, Chi‐Te Liang, Juhn‐Jong Lin, Chia‐Hung Hsu, Yen‐Hsiang Lin, J. Kwo, Minghwei Hong
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.
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.
We have reproducibly grown near-single-domain superconducting aluminum (Al) films on GaAs(111)A wafers using molecular beam epitaxy. Synchrotron X-ray diffraction revealed twin-domain ratios of 0.00005 and 0.0003 for 19.4-nm- and 9.6-nm-thick films, respectively-the lowest reported for Al on any substrate and long considered unattainable for practical device platforms. Azimuthal scans across off-normal Al{111ˉ} reflections exhibit narrow full width at half maximum (FWHM) values down to 0.55∘, unmatched by epi-Al grown by any other method. Normal scans showed a well-defined (111) orientation with pronounced Pendellösung fringes, and θ-rocking-curve FWHM values down to 0.018∘; the former indicates abrupt film-substrate and oxide-film interfaces. Electron backscatter diffraction mapping confirms macroscopic in-plane uniformity and the absence of $Σ$3 twin domains. Atomic force microscopy and scanning transmission electron microscopy confirmed atomically smooth surfaces and abrupt heterointerfaces. The films exhibit critical temperatures approaching bulk values, establishing a materials platform for scalable, high-coherence superconducting qubits.
Abstract The quest for a universal quantum computer has renewed interest in the growth of superconducting materials on semiconductor substrates. High-quality superconducting thin films will make it possible to improve the coherence time of superconducting quantum bits (qubits), i.e., to extend the time a qubit can store the amplitude and phase of a quantum state. The electrical losses in superconducting qubits highly depend on the quality of the metal layers the qubits are made from. Here, we report on the epitaxy of single-crystal Al (011) layers on GaAs (001) substrates. Layers with 110 nm thickness were deposited by means of molecular beam epitaxy at low temperature and monitored by in situ reflection high-energy electron diffraction performed simultaneously at four azimuths. The single-crystal nature of the layers was confirmed by ex situ high-resolution x-ray diffraction. Differential interference contrast and atomic force microscopy analysis of the sample’s surface revealed a featureless surface with root mean square roughness of 0.55 nm. A detailed in situ study allowed us to gain insight into the nucleation mechanisms of Al layers on GaAs, highlighting the importance of GaAs surface reconstruction in determining the final Al layer crystallographic orientation and quality. A highly uniform and stable GaAs (001)- ( 2 × 4 ) reconstruction reproducibly led to a pure Al (011) phase, while an arsenic-rich GaAs (001)- ( 4 × 4 ) reconstruction yielded polycrystalline films with an Al (111) dominant orientation. The near-atomic smoothness and single-crystal character of Al films on GaAs, in combination with the ability to trench GaAs substrates, could set a new standard for the fabrication of superconducting qubits.
The realization of highly coherent and scalable superconducting quantum circuits relies critically on the structural perfection of epitaxial aluminium (Al) films. However, the presence of twin boundaries in these materials introduces prominent decoherence channels that severely limit device performance. Here, we have reproducibly grown near-single-domain superconducting Al films on GaAs(111)A wafers using molecular beam epitaxy. Synchrotron X-ray diffraction revealed twin-domain ratios of 0.00005 and 0.0003 for 19.4-nm- and 9.6-nm-thick films, respectively—the lowest reported for Al on any substrate and long considered unattainable for practical device platforms. Azimuthal scans across off-normal Al{111ˉ} reflections exhibit narrow full width at half maximum (FWHM) values down to 0.55°, unmatched by epi-Al grown by any other method. Normal scans showed a well-defined (111) orientation with pronounced Pendellösung fringes, and θ-rocking-curve FWHM values down to 0.018°; the former indicates abrupt film–substrate and oxide–film interfaces. Electron backscatter diffraction mapping confirms macroscopic in-plane uniformity and the absence of Σ3 twin domains. Atomic force microscopy and scanning transmission electron microscopy confirmed atomically smooth surfaces and abrupt heterointerfaces. The films exhibit critical temperatures approaching bulk values, establishing a materials platform for scalable, high-coherence superconducting qubits. The structural perfection of epitaxial aluminium films is crucial for advancing superconducting quantum circuits, yet twin boundaries hinder device performance. Here, the authors achieve near-single-domain superconducting Al films on Ga-terminated GaAs(111) wafers, demonstrating ultralow twin-domain ratios, atomically smooth surfaces, and abrupt heterointerfaces, paving the way for scalable, high-performance quantum devices.
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.
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.
Ultra-thin epitaxial NbN layers are a key component of Superconducting Single Photon infrared Detectors. Efforts devoted to the layer growth aim at improving their critical temperature and critical current density, while keeping their thickness close to 5 nm and Tc above 10 K, which insure a large bandwidth, large SNR detection at 4K. Choice of substrate is critical: for both applications, MgO wafers and R-plane sapphire are usually considered as best substrates to grown onto. However, growing NbN on M-plane orientation of sapphire wafer, 3 inch in diameter, can help improving the film quality and fabrication yield. NbN thin films were grown by reactive DC magnetron sputtering at about 600°C and passivated by an AlN layer 1.5nm thick deposited in-situ at room temperature. Growth on M-plane is shown to be better than on other sapphire orientations, including R-plane: NbN layer critical temperature reaches 13.3 K, uniform on the wafer, for a film thickness of 4.4nm measured by X-ray reflectivity. Transport properties of NbN grown on those various substrates have been correlated to their crystallographic microstructure, examined by both symmetric and asymmetric X ray diffraction. Observation of diffraction peaks has given insight on the disorientation of the NbN film.