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arXiv:2410.06805 · Physical Review Applied

Crystallinity in niobium oxides: A pathway to mitigate two-level-system defects in niobium three-dimensional resonators for quantum applications

Yasmine Kalboussi, I. Curci, F. Miserque, David Troadec, Nathalie Brun B, Michael G. Walls, GRAHAM A. JULLIEN, Fabien Éozénou, Matthieu Baudrier, Luc Maurice, Q. Bertrand, Patrick Sahuquet, Thomas Proslier

Published Apr 9, 2025• 10 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physrevapplied.23.044023

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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.
Superconducting qubits have arisen as a leading technology platform for quantum computing which is on the verge of revolutionizing the world's calculation capacities. Nonetheless, the fabrication of computationally reliable qubit circuits requires increasing the quantum coherence lifetimes, which are predominantly limited by the dissipations of two-level system (TLS) defects present in the thin superconducting film and the adjacent dielectric regions. In this paper, we demonstrate the reduction of two-level system losses in three-dimensional superconducting radio frequency (SRF) niobium resonators by atomic layer deposition (ALD) of a 10 nm aluminum oxide Al2O3 thin films followed by a high vacuum (HV) heat treatment at 650 °C for few hours. By probing the effect of several heat treatments on Al2O3-coated niobium samples by X-ray photoelectron spectroscopy (XPS) plus scanning and conventional high resolution transmission electron microscopy (STEM/HRTEM) coupled with electron energy loss spectroscopy (EELS) and (EDX) , we witness a dissolution of niobium native oxides and the modification of the Al2O3-Nb interface, which correlates with the enhancement of the quality factor at low fields of two 1.3 GHz niobium cavities coated with 10 nm of Al2O3.
Superconducting qubits have arisen as a leading technology platform for quantum computing, which is on the verge of revolutionizing the world's calculation capacities. Nonetheless, the fabrication of computationally reliable qubit circuits requires increasing the quantum coherence lifetimes, which are predominantly limited by the dissipations of two-level system defects present in the thin superconducting film and the adjacent dielectric regions. In this paper, we demonstrate the reduction of two-level system losses in three-dimensional superconducting radio frequency niobium resonators by atomic layer deposition of a 10 nm aluminum oxide Al2O3 thin films, followed by a high vacuum heat treatment at 650 °C for few hours. By probing the effect of several heat treatments on Al2O3-coated niobium samples by x-ray photoelectron spectroscopy plus scanning and conventional high resolution transmission electron microscopy coupled with electron energy loss spectroscopy and energy dispersive spectroscopy, we witness a dissolution of niobium native oxides and the modification of the Al2O3-Nb interface, which correlates with the enhancement of the quality factor at low fields of two 1.3 GHz niobium cavities coated with 10 nm of Al2O3.
We identify a major source of quantum decoherence in three-dimensional superconducting radio-frequency (SRF) resonators and two-dimensional transmon qubits composed of oxidized niobium: oxygen vacancies in the niobium pentoxide, which drive two-level system (TLS) losses. By probing the effect of sequential in situ vacuum-baking treatments on the rf performance of bulk Nb\mathrm{Nb}Nb SRF resonators and on the oxide structure of a representative Nb\mathrm{Nb}Nb sample using TOF SIMS, we find a nonmonotonic evolution of cavity quality factor Q0{Q}_{0}Q0​, which correlates with the interplay of Nb2O5{\mathrm{Nb}}_{2}{\mathrm{O}}_{5}Nb2​O5​ vacancy generation and oxide-thickness reduction. We localize this effect to the oxide itself and present the insignificant role of diffused interstitial oxygen in the underlying Nb\mathrm{Nb}Nb by regrowing the oxide via wet oxidation, which reveals a mitigation of aggravated TLS losses. We hypothesize that such vacancies in the pentoxide serve as magnetic impurities and are a source of TLS-driven rf loss.
To improve the performance of state-of-the-art superconducting quantum devices, microwave loss due to defects at amorphous interfacial layers must be reduced, via proper surface treatment. The authors study niobium resonators after removing native oxides by HF etching, which reduces losses about tenfold and yields a quality factor of $7\ifmmode\times\else\texttimes\fi{}{10}^{6}$ in the single-photon limit. Losses reappear as oxides form upon exposure to air; Nb2{}_{2}2​O5{}_{5}5​ is the only surface oxide that grows significantly in the first week. These findings are of interest for a panoply of devices, inluding superconducting qubits, quantum-limited amplifiers, microwave kinetic-inductance detectors, and single-photon detectors.
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.
Superconducting coplanar waveguide resonators are essential components in quantum processors, where their internal quality factor (Qi) constrains qubit coherence and readout fidelity. In niobium devices, microwave losses at millikelvin temperatures are strongly influenced by two-level systems (TLS) associated with the complex NbOx surface oxide. To mitigate these losses, we investigate a surface-engineering approach in which Nb films are capped in situ with a thin tantalum layer to suppress Nb2O5 formation and replace the native NbOx interface with a Ta-based oxide. We fabricate Nb/Ta bilayer and reference Nb resonators on high-resistivity silicon using identical DC sputtering and wet etching conditions, and characterize their performance at millikelvin temperatures. Fresh Ta-encapsulated devices exhibit internal quality factors up to 2.4 x 10^6 in the near-single-photon regime, with power dependence consistent with reduced TLS-related loss at the metal-air interface. A control Nb device fabricated under the same process shows comparatively lower Q_TLS, consistent with the beneficial effect of the Ta capping layer. Furthermore, ageing tests performed on Nb/Ta resonators after six months reveal a moderate reduction in Q_TLS relative to their initial values, yet the performance remains superior to newly fabricated Nb-only devices. These results suggest that thin Ta encapsulation enhances interface quality and contributes to improved temporal stability while remaining compatible with Nb-based fabrication workflows.