Atomic-Scale Characterization and Electronic Properties of Gold-Capped Niobium Films for Superconducting Qubits
Junki Makita, Seth Rice, G. Berti, Francesco Crisa, Sabrina Garattoni, Mustafa Bal, Jaeyel Lee, Akshay A. Murthy, David A. Garcia Wetten, Dominic P. Goronzy, Thang Pham, Vinayak P. Dravid, Mark C. Hersam, Michael J. Bedzyk, Jin‐Su Oh, Lin Zhou, Alexander Romanenko, Anna Grassellino, John Francis Zasadzinski, M. Iavarone
Niobium thin films are central to superconducting qubits, but their complex native oxides contribute significantly to microwave losses. A promising mitigation strategy is to suppress oxide formation using engineered thin-film encapsulation layers. Recent experiments have shown that ∼10 nm metallic overlayers on Nb capacitor films can improve the energy relaxation time T 1 of transmon qubits. Here, we present a comparative study of Au-capped Nb films fabricated in situ by molecular beam epitaxy and ex situ by sequential deposition benchmarked against bare Nb films. Using complementary structural, chemical, and spectroscopic techniques, we correlate the interface quality with superconducting electronic properties of the Au surface. Low-temperature scanning tunneling spectroscopy (STS) provides spatially resolved quasiparticle density-of-states maps. While both Au-capped Nb samples exhibit large areas with uniform, fully gapped density of states, clear differences emerge between the two interfaces. Compared to in situ Nb–Au, ex situ Nb–Au exhibits a reduced induced superconducting gap, broadened coherence peak, and localized in-gap states, consistent with a residual Nb x O y layer at the interface. Supported by complementary structural and chemical analyses, these findings demonstrate that STS directly links nanoscale superconducting properties to interface preparation, highlighting the importance of controlled in situ encapsulation for minimizing dissipation and improving quantum coherence.
Niobium thin films are central to superconducting qubits, but their complex native oxides contribute significantly to microwave losses. A promising mitigation strategy is to suppress oxide formation using engineered thin-film encapsulation layers. Recent experiments have shown that ∼10 nm metallic overlayers on Nb capacitor films can improve the energy relaxation time T 1 of transmon qubits. Here, we present a comparative study of Au-capped Nb films fabricated in situ by molecular beam epitaxy and ex situ by sequential deposition benchmarked against bare Nb films. Using complementary structural, chemical, and spectroscopic techniques, we correlate the interface quality with superconducting electronic properties of the Au surface. Low-temperature scanning tunneling spectroscopy (STS) provides spatially resolved quasiparticle density-of-states maps. While both Au-capped Nb samples exhibit large areas with uniform, fully gapped density of states, clear differences emerge between the two interfaces. Compared to in situ Nb–Au, ex situ Nb–Au exhibits a reduced induced superconducting gap, broadened coherence peak, and localized in-gap states, consistent with a residual Nb x O y layer at the interface. Supported by complementary structural and chemical analyses, these findings demonstrate that STS directly links nanoscale superconducting properties to interface preparation, highlighting the importance of controlled in situ encapsulation for minimizing dissipation and improving quantum coherence.
Niobium metal occupies nearly 100\% of the volume of a typical 2D transmon device. While the aluminum Josephson junction is of utmost importance, maintaining quantum coherence across the entire device means that pair-breaking in Nb leads, capacitive pads, and readout resonators can be a major source of decoherence. The established contributors are surface oxides and hydroxides, as well as absorbed hydrogen and oxygen. Metal encapsulation of freshly grown surfaces with non-oxidizing metals, preferably without breaking the vacuum, is a successful strategy to mitigate these issues. While the positive effects of encapsulation are undeniable, it is important to understand its impact on the macroscopic behavior of niobium films. We present a comprehensive study of the bulk superconducting properties of Nb thin films encapsulated with gold and palladium/gold, and compare them to those of bare Nb films. Magneto-optical imaging, magnetization, resistivity, and London and Campbell penetration depth measurements reveal significant differences in encapsulated samples. Both sputtered, and epitaxial Au-capped films exhibit the highest residual resistivity ratio and superconducting transition temperature, as well as the lowest upper critical field, London penetration depth, and critical current. These results are in good agreement with the microscopic theory of anisotropic normal and superconducting states of Nb. We conclude that pair-breaking in the bulk of niobium films, driven by disorder throughout the film rather than just at the surface, is a significant source of quantum decoherence in transmons. We also conclude that gold capping not only passivates the surface but also affects the properties of the entire film, significantly reducing the scattering rate due to defects likely induced by surface diffusion if the film is not protected immediately after fabrication.
Abstract We present a transmon qubit fabrication technique that yields systematic improvements in T 1 relaxation times. We encapsulate the surface of niobium and prevent the formation of its lossy surface oxide. By maintaining the same superconducting metal and only varying the surface, this comparative investigation examining different capping materials, such as tantalum, aluminum, titanium nitride, and gold, as well as substrates across different qubit foundries demonstrates the detrimental impact that niobium oxides have on coherence times of superconducting qubits, compared to native oxides of tantalum, aluminum or titanium nitride. Our surface-encapsulated niobium qubit devices exhibit T 1 relaxation times 2–5 times longer than baseline qubit devices with native niobium oxides. When capping niobium with tantalum, we obtain median qubit lifetimes above 300 μs, with maximum values up to 600 μs. Our comparative structural and chemical analysis provides insight into why amorphous niobium oxides may induce higher losses compared to other amorphous oxides.
Dielectric losses at surfaces and interfaces remains a primary limitation to coherence in superconducting transmon qubits. Niobium (Nb), a widely used material in superconducting quantum circuits, readily forms native oxides under ambient conditions, leading to lossy dielectric interfaces that degrade device performance. Here, we demonstrate a novel fabrication strategy that chemically transforms the native dielectric oxide on Nb into a metallic Pt--Nb surface alloy through post-oxidation Pt deposition followed by thermal annealing, thereby stabilizing Nb surfaces against further oxidation, potentially including sidewall regions. High-purity Nb films were fabricated with bulk-like superconducting transition temperatures (Tc=9.30±0.10~K). Spectroscopic and microscopic analyses confirm the conversion of the native oxide into a chemically stable, metallic alloy-dominated layer that suppresses subsequent oxide growth. Ab initio simulations elucidate the atomic-scale rearrangement and electronic structure evolution associated with Pt incorporation into native niobium oxide, providing insight into the mechanism underlying the oxide-to-metal transformation and stabilization of the alloyed surface.
ABSTRACT Niobium (Nb) films have emerged as a crucial material in the development of superconducting qubits, which are key components in quantum computing technology. This review provides a comprehensive examination of Nb films from a materials perspective, focusing on their intrinsic properties, fabrication methods/techniques, and their influence on qubit performance, particularly through surface and interface driven loss mechanisms. We discuss the key material properties that are essential for qubit operation. Various deposition techniques for Nb thin films, such as sputtering, evaporation, molecular beam epitaxy, and atomic layer deposition, are explored, alongside their impact on film quality, uniformity, and qubit performance. Additionally, the influence of surface roughness, thin‐film thickness, and substrate materials on quantum coherence is analyzed. Challenges such as defects and material degradation in Nb films are reviewed, along with strategies to mitigate these issues. Finally, we present the latest advancements and future directions in Nb film research, including potential improvements to enhance qubit coherence and scalability for large‐scale quantum computing systems. Ultimately, a deeper understanding of surface and interface phenomena is essential for pushing the limits of qubit performance and realizing next‐generation quantum technologies.
Niobium thin films are key components of superconducting microwave resonators. Interest in these devices has increased dramatically because of their application in quantum systems. Despite tremendous effort to improve their performance, loss mechanisms are still not well understood. Nb/substrate and Nb/air interfaces are likely culprits in contributing to decoherence and ultimately limiting the performance of superconducting devices. Here, we investigate the Nb/substrate interface by studying the effect of hydrogen-passivated H:Si(111) substrates on the local superconducting properties of ∼40 nm thick Nb films compared to Nb films grown on typical Si(001) substrates. Specifically, low-temperature scanning tunneling microscopy and spectroscopy are employed to compare nanoscale material properties. The atomically flat monohydride H:Si(111) substrates are found to yield a smoother and less defective interface with the Nb film. Correspondingly, the Nb films grown on H:Si(111) substrates present more uniform superconducting properties and exhibit less quasiparticle broadening.
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.