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arXiv:2402.04137

Reducing two-level system dissipations in 3D superconducting Niobium resonators by atomic layer deposition and high temperature heat treatment

Yasmine Kalboussi, Baptiste Delatte, Sarra Bira, Kassiogé Dembélé, Xiaoyan Li, F. Miserque, Nathalie Brun B, Michael G. Walls, Jean-Luc Maurice, Diana Dragoé, Jocelyne Leroy, David Longuevergne, A. Gentils, S. Jublot-Leclerc, Grégoire Julien, Fabien Éozénou, Matthieu Baudrier, Luc Maurice, Thomas Proslier

Published Feb 6, 2024• 0 citations
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Abstract

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.

DOI
10.48550/arxiv.2402.04137

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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.
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.
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.
We present a dry surface treatment combining atomic layer etching and deposition (ALE and ALD) to mitigate dielectric loss in fully fabricated superconducting quantum devices formed from aluminum thin films on silicon. The treatment, performed as a final processing step prior to device packaging, starts by conformally removing the native metal oxide and fabrication residues from the exposed surfaces through ALE, before in situ encapsulating the metal surfaces with a thin dielectric layer using ALD. We measure a 2-fold reduction in loss attributed to two-level system (TLS) absorption in treated aluminum-based resonators and planar transmon qubits. Treated transmons with compact capacitor plates and gaps achieve median transmon quality factor ( Q ) and transmon qubit energy relaxation time ( T 1 ) values of 3.69 ± 0.42 × 10 6 and 196 ± 22 μs, respectively. These improvements were found to be sustained over several months. We discuss how the combination of ALE and ALD reverses fabrication-induced surface damage to significantly and durably improve device performance via a reduction of the TLS defect density in the capacitive elements.
Abstract Quantum bits (qubits) with long coherence times are an important element for the implementation of medium- and large-scale quantum computers. In the case of superconducting planar qubits, understanding and improving qubits’ quality can be achieved by studying superconducting planar resonators. In this paper, we fabricate and characterize coplanar waveguide resonators made from aluminum thin films deposited on silicon substrates. We perform three different substrate surface treatments prior to aluminum deposition: one chemical treatment based on a hydrofluoric acid clean; one physical treatment consisting of a thermal annealing at 880 °C in high vacuum; and one combined treatment comprising both the chemical and the physical treatments. The aim of these treatments is to remove the two-level state (TLS) defects hosted by the native oxides residing at the various samples’ interfaces. We first characterize the fabricated samples through cross-sectional tunneling electron microscopy, acquiring electron energy loss spectroscopy maps of the samples’ cross sections. These measurements show that both the chemical and the physical treatments almost entirely remove native silicon oxide from the substrate surface and that their combination results in the cleanest interface. Additionally, we analyze the effects of the various substrate treatments on the roughness of the silicon surface by means of atomic force microscopy surface morphology mapping. We then study the quality of the resonators by means of microwave measurements in the ‘quantum regime’, i.e., at a temperature T ∼ 10 mK and at a mean microwave photon number 〈 n ph 〉 ∼ 1 . In this regime, we find that both surface treatments independently improve the resonator’s intrinsic quality factor by ≈172%. The highest quality factor is obtained for the combined treatment, Q i ≈ 0.82 million, corresponding to an improvement by ≈256%. Finally, we find that the TLS quality factor averaged over a time period of 3 h is ∼3 million at 〈 n ph 〉 ∼ 10 , indicating that substrate surface engineering can potentially reduce the TLS loss below other losses such as quasiparticle loss and flux noise.
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.