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{$$11\bar{1}$$} 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.
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.
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.
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.
Superconducting qubit technology is among the most promising hardware platform for quantum computing due to its fast gate operation, manufacturing scalability, and architectural flexibility [1]. A key figure of merit that dictates quantum computing functionality is the qubit’s coherence time, which needs to be maximized in order to bring quantum computing to the practical and scalable realm [2]. In particular, the T1 relaxation time—now on the order of milliseconds—can be enhanced with materials engineering, as amorphous dielectrics and crystallographic defects, among other factors, are known to induce decoherence [3-7]. Current state-of-the-art superconducting qubit devices use amorphous AlOx sandwiched between two superconducting Al electrodes as the Josephson junction (JJ), a key element in the transmon qubit, but amorphous dielectrics introduce two-level system (TLS) loss that underlie decoherence [8]. For this reason, numerous efforts have explored crystalline dielectrics as a replacement for amorphous AlOx, since single-crystal materials do not suffer from the lack of long-range order and sub-stoichiometry that comprise TLS defects [9-12]. However, none of these alternative materials choices have been able to surpass, let alone replicate, the performance of Al-AlOx-Al JJs. In this work, we fabricate superconducting quantum devices using a novel heteroepitaxial TiN/γ-Al2O3/TiN tri-layer stack grown on sapphire (Fig. 1a) and find that the measured microwave loss of the single-crystal γ-Al2O3 dielectric is lower than that of amorphous AlOx by two orders of magnitude. For qubits made with this tri-layer to transcend the coherence of incumbent Al-AlOx-Al, the structural, chemical, and electronic defects that induce TLS loss in these materials need to be well understood. Towards this end, we combine scanning transmission electron microscopy (STEM) and scanning electron microscopy (SEM) methods to highlight structural and interfacial complexity across length scales, ultimately identifying loss sources in the TiN/γ-Al2O3/TiN heteroepitaxial tri-layer. With atomic-resolution imaging and four-dimensional (4D-)STEM nanobeam electron diffraction (NBED), we find that the dielectric γ-Al2O3 layer, though single-crystalline (Fig. 1b), suffers from the formation of antiphase boundaries (Fig. 1c), which can host strong local electric fields and enhance lossy dielectric response [13]. Correlated with these nanoscale planar defects is uniformly distributed elastic strain, on the order of 6%, between the lattice-mismatched γ-Al2O3 and TiN (Fig. 1d). In other words, the dielectric layer is fully strained to match the underlying metal layer; such high strain can distort local bonding environments and thus create new TLSs or shift existing TLSs into resonance. Beyond imperfections within the bulk of the dielectric layer, there are noteworthy interfacial defects: roughening of both TiN/γ-Al2O3 interfaces deviate from atomically flat boundaries (Fig. 1c), while anion interdiffusion across both interfaces, as evident from core-loss electron energy-loss spectral (EELS) maps (Fig. 1e), leave behind vacancies and undercoordinated metal atoms, thereby creating 1.5 – 2 nm nonstoichiometric diffuse interfacial layers, both of which can cause TLS loss. In the superconducting TiN layers, we again use NBED to identify 180°-reflected specular twinned domains, indicating distinct heteroepitaxial relationships of [111]TiN//[0006]Al2O3 and [002¯]TiN//[22¯02¯]Al2O3 (Fig. 2a) [14]. Crystal twinning of the TiN epilayer is not only spatially distributed at the nanoscale, as shown using virtual dark-field (VDF) images (Fig. 2b), but is also widespread at the microscale, as shown using SEM electron backscatter diffraction (EBSD) (Fig. 2c). While microwave performance is not limited by a single factor, it is clear that defective quantum microstructure across length scales collectively contribute to dielectric loss, and in turn, TLS-related decoherence. By correlating nanoscale crystallographic and spectroscopic information with microscale diffraction measurements, our work can guide interface engineering during material growth, paving the way towards further improvements in quantum device performance. Cross-sectional samples were prepared by subsequent 30 kV, 8 kV and 5 kV Xe+ plasma focused ion beam (FIB) using the Thermo Scientific Helios 5 Hydra CX DualBeam Plasma FIB/SEM. Samples were then plasma cleaned using South Bay Technology PC-2000 Plasma Cleaner with a 3:1 mixture of Ar:O2 gas at 20∼40 W RF power for 15 s at 150 mTorr. High-angle annular dark-field (HAADF-) and annular bright-field (ABF-) STEM images were collected on a probe-corrected JEOL JEM-ARM200CF S/TEM operating at 200 kV using JEOL detectors. The STEM convergence angle, HAADF collection angle, and ABF collection angle were 27 mrad, 90 – 370 mrad, and 23 mrad, respectively. EELS data were collected on a JEOL JEM-ARM300F GrandARM S/TEM operating at 300 kV using the Gatan GIF Continuum K3 IS system. The data were collected using a 2.5 mm aperture and a 750 eV wide energy slit at a dispersion of 0.18 eV/Ch and a camera length of 2 cm. 4D-STEM data were collected on the same microscope and detector system using a 0.5 – 1.5 mrad convergence angle and a 20 eV wide energy slit at a camera length of 4 cm. All STEM data processing was performed using the Gatan Microscopy Suite software. Top-down EBSD measurements were performed in the Thermo Scientific Helios 5 CX DualBeam FIB/SEM at 25 kV using the Oxford Symmetry S3 detector. EBSD data processing was performed using the Oxford AZtecCrystal software [15]. Defects in γ-Al2O3. a) HAADF-STEM image of a TiN/γ-Al2O3/TiN tri-layer stack on a α-Al2O3 (0001) substrate. The thickness of γ-Al2O3 is approximately 13.5 nm. b) 4D-STEM NBED pattern of the γ-Al2O3 layer, confirming the {111} out-of-plane orientation. c) Fourier-filtered atomic-resolution ABF-STEM image of the γ-Al2O3 dielectric layer, taken from the cyan-colored square region in a), emphasizing the planar defects along both TiN/γ-Al2O3 interfaces and within the γ-Al2O3 layer itself–interfacial roughness (yellow lines) and antiphase boundaries (colored parallelograms), respectively. The scale bar is 2 nm. d) In-plane and out-of-plane strain maps of the heteroepitaxial tri-layer stack, with approximately 6.5∼6.8% strain in both directions. The units of the intensity bar are such that 100% strain would be equivalent to 1.0. e) STEM-EELS maps of Ti-L2,3, N-K, and O-K edges, along with a superimposed image of the three, taken from the same region as c). The scale bars are all 5 nm. Defects in TiN. a) 4D-STEM NBED patterns and b) VDF images of nanoscale TiN {111} and {002} twins. c) SEM EBSD pole figures in the three face-centered cubic crystallographic directions, revealing that the 60° rotation twinning behavior (with the [111] twin axis) is spread across the microscale.
Tantalum films incorporated into superconducting circuits have exhibited low surface losses, resulting in long-lived qubit states. The remaining loss pathways originate in microscopic defects that manifest as two level systems (TLSs) at low temperatures. These defects limit performance, so careful attention to tantalum film structures is critical for optimal use in quantum devices. In this work, we investigate the growth of tantalum using magnetron sputtering on sapphire, Si, and photoresist substrates. In the case of sapphire, we present procedures for the growth of fully-oriented films with α-Ta [1 1 1]//Al2O3 [0 0 0 1] and α-Ta [1 −1 0]//Al2O3 [1 0 −1 0] orientational relationships and having residual resistivity ratio (RRR) ∼ 60 for 220 nm thick films. On Si, we find a complex grain texturing with Ta [1 1 0] normal to the substrate and RRR ∼ 30. We further demonstrate airbridge fabrication using Nb to nucleate α-Ta on photoresist surfaces. For the films on sapphire, resonators show TLS-limited quality factors of 1.3 ± 0.3 × 106 at 10 mK (for a waveguide gap and conductor width of 3 and 6 μm, respectively). Structural characterization using scanning electron microscopy, x-ray diffraction, low temperature transport, secondary ion mass spectrometry, and transmission electron microscopy reveal the dependence of residual impurities and screw dislocation density on processing conditions. The results provide practical insights into the fabrication of advanced superconducting devices including qubit arrays and guide future works on crystallographically deterministic qubit fabrication.