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arXiv:2606.10144

Synthesis and Characterization of Atomically-Sharp Superconductor-Dielectric Interface

Nathan Sitaraman, Zhaslan Baraissov, Alexis Grassl, Hongbin Yang, Daniel Tong, David Anthony Muller, Matthias Liepe

Published Jun 8, 2026• 0 citations
arXivHTMLPDF

Abstract

Modification of superconductor-dielectric interfaces is known to strongly impact coherence times of superconducting quantum devices. This relationship is thought to arise from differences in the concentration of "two-level system" defects in the disordered dielectrics and superconductor-dielectric interfaces; these defects couple to electromagnetic modes in the device and cause dissipation. Zirconium oxide barrier layers on niobium have emerged as a promising pathway to low-loss interfaces in recent years, evidently due to the crystalline nature of these layers in comparison to the amorphous niobium native oxide. We explain the unique ability of zirconium oxide to form a crystalline layer, to maintain a sharp interface with metallic niobium, and to prevent niobium oxide re-growth in terms of the chemical properties of ZrO$_2$ and the Nb-Zr-O ternary system. We demonstrate a new method to grow air-stable zirconium oxide layers on niobium with a higher level of crystallinity and a sharper oxide-metal interface than previously shown, and provide the first comprehensive microscopic analysis of ZrO$_2$ capping layer properties. These developments pave the way toward vital performance advances in superconducting quantum devices.

DOI
10.48550/arxiv.2606.10144

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Modification of superconductor-dielectric interfaces is known to strongly impact coherence times of superconducting quantum devices. This relationship is thought to arise from differences in the concentration of "two-level system" defects in the disordered dielectrics and superconductor-dielectric interfaces; these defects couple to electromagnetic modes in the device and cause dissipation. Zirconium oxide barrier layers on niobium have emerged as a promising pathway to low-loss interfaces in recent years, evidently due to the crystalline nature of these layers in comparison to the amorphous niobium native oxide. We explain the unique ability of zirconium oxide to form a crystalline layer, to maintain a sharp interface with metallic niobium, and to prevent niobium oxide re-growth in terms of the chemical properties of ZrO2_22​ and the Nb-Zr-O ternary system. We demonstrate a new method to grow air-stable zirconium oxide layers on niobium with a higher level of crystallinity and a sharper oxide-metal interface than previously shown, and provide the first comprehensive microscopic analysis of ZrO2_22​ capping layer properties. These developments pave the way toward vital performance advances in superconducting quantum devices.
Niobium is commonly used for superconducting quantum systems as readout resonators, capacitors, and interconnects. The coherence time of the superconducting qubits is mainly limited by microwave dissipation attributed to two-level system defects at interfaces, such as the Nb/Si and Nb/air interface. One way to improve the Nb/air interface quality is by thermal annealing, as shown by extensive studies in 3D superconducting radio frequency (SRF) cavities. However, it is unclear how the microstructure and chemistry of the interface structures change during heat treatment. To address this knowledge gap, we comprehensively characterized Nb films deposited on Si wafers by physical vapor deposition, including (1) an Nb film from a transmon and (2) an Nb film without any patterning step, using an aberration-corrected transmission electron microscope. Both Nb films exhibit columnar growth with strong [110] textures. There is a double layer between the Nb film and Si substrate, which are amorphous niobium silicides with different Nb and Si concentrations. After in-situ heating of the heterostructure at 360°C inside the microscope, the composition of the double layers at the Nb-Si interface remains almost the same despite different thickness changes. The initial amorphous niobium oxide layer on Nb surface decomposes into face-centered cubic Nb nanograins in the amorphous Nb-O matrix upon heating.
Materials imperfections in Nb -based superconducting quantum circuits—in particular, two-level-system (TLS) defects—are a major source of decoherence, ultimately limiting the performance of quantum computation and sensing. Thus, identifying and understanding the microscopic origin of possible TLS defects in these devices will help develop strategies that eliminate them, which are key to superconducting qubit performance improvement. In this paper, we demonstrate an order-of-magnitude reduction in two-level system losses in three-dimensional superconducting radio frequency (SRF) niobium resonators by a 10-h high vacuum (HV) heat treatment at 650 °C, even after exposure to air and high-pressure rinsing (HPR). X-ray photoelectron spectroscopy (XPS) and high-resolution scanning transmission electron microscopy (STEM) reveal an alteration of the native oxide composition regrown after air exposure and HPR and the creation of nanoscale crystalline oxide regions, which correlates with the measured tenfold quality factor enhancement at low fields of the 1.3 GHz niobium resonator. Tunneling spectroscopy measurements show a pronounced proximity effect that further confirms the presence of metallic layers on the niobium surface.
The Josephson junction is a crucial element in superconducting devices, and niobium is a promising candidate for the superconducting material due to its large energy gap relative to aluminum. AlOx has long been regarded as the highest quality oxide tunnel barrier and is often used in niobium-based junctions. Here, we propose ZrOx as an alternative tunnel barrier material for Nb electrodes. We theoretically estimate that zirconium oxide has excellent oxygen retention properties and experimentally verify that there is no significant oxygen diffusion leading to NbOx formation in the adjacent Nb electrode. We develop a top–down, subtractive fabrication process for Nb/Zr–ZrOx/Nb Josephson junctions, which enables scalability and large-scale production of superconducting electronics. Using cross-sectional scanning transmission electron microscopy, we experimentally find that depending on the Zr thickness, ZrOx tunnel barriers can be fully crystalline with chemically abrupt interfaces with niobium. Further analysis using electron energy loss spectroscopy reveals that ZrOx corresponds to tetragonal ZrO2. Room temperature characterization of fabricated junctions using Simmons’ model shows that ZrO2 exhibits a low tunnel barrier height, which is promising in merged-element transmon applications. Low temperature transport measurements reveal sub-gap structure, while the low-voltage sub-gap resistance remains in the megaohm range.
While several experiments claim that two-level system (TLS) defects in amorphous surfaces and interfaces are responsible for energy relaxation in superconducting resonators and qubits, none can provide quantitative explanation of their data in terms of the conventional noninteracting TLS model. Here a model that interpolates between the interacting and noninteracting TLS loss tangent is proposed to perform numerical analysis of experimental data and extract information about TLS parameters and their distribution. As a proof of principle, the model is applied to TESLA cavities that contain only a single lossy material in their interior, the niobium-niobium oxide interface. The best fits show interacting TLSs with a sharp modulus of electric dipole moment for both thin (5nm5\phantom{\rule{0.2em}{0ex}}\mathrm{nm}5nm) and thick (100nm100\phantom{\rule{0.2em}{0ex}}\mathrm{nm}100nm) oxides, indicating that the TLSs are ``atomic'' instead of ``glassy.'' The proposed method can be applied to other devices with multiple material interfaces and substrates, with the goal of elucidating the nature of TLSs causing energy loss in resonators and qubits.
times 2 to 5 times longer than baseline niobium qubit devices with native niobium oxides. When capping niobium with tantalum, we obtain median qubit lifetimes above 200 microseconds. Our comparative structural and chemical analysis suggests that amorphous niobium oxides may induce higher losses compared to other amorphous oxides. These results are in line with high-accuracy measurements of the niobium oxide loss tangent obtained with ultra-high Q superconducting radiofrequency (SRF) cavities. This new surface encapsulation strategy enables even further reduction of dielectric losses via passivation with ambient-stable materials, while preserving fabrication and scalable manufacturability thanks to the compatibility with silicon processes.
The current performance of superconducting circuit-based quantum processors is limited by the poor understanding of interface physics, including native surface oxide formation on the superconducting metal, which causes two-level system (TLS) loss. Niobium (Nb), a superconducting metal with a high energy gap, is an ideal choice for superconducting processors, but unfortunately, it is marred by TLS. Several methods have been proposed to minimize surface oxide on the Nb film, and considerable improvement in TLS loss has been demonstrated. These methods include surface passivation through metal capping, self-assembly of organic molecules, and post-cleaning processes. Among these, metal capping is a suitable choice despite forming a 3–5 nm thick oxide, as self-assembly and post-treatment do not protect the Nb film surface during further fabrication. Here, we have proposed ruthenium (Ru) as a capping layer, forming a self-limiting oxidation with a 0.6 nm oxide thickness and predominantly producing fewer oxide compositions while being chemically resistant for further wafer fabrication processes, thus fulfilling all the criteria of an ideal capping layer. Our investigation suggests that Nb/Ru resonators have great potential as versatile and promising tools for advancing superconducting quantum technologies and integrating quantum interconnects into qubits with minimized TLS loss.