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arXiv:2506.17474 · ACS Nano

Improving the Lifetime of Aluminum-Based Superconducting Qubits through Atomic Layer Etching and Deposition

Neha Mahuli, Joaquín Minguzzi, Jiansong Gao, Rachel Resnick, Sandra Díez, R. Cosmic, Guillaume Marcaud, Matthew Hunt, Loren J. Swenson, Jefferson Rose, Oskar J. Painter, Ignace Jarrige

Published Nov 20, 2025• 6 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1021/acsnano.5c14022

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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.
Material losses in superconducting circuits fundamentally limit qubit coherence times and resonator quality factors. Most research efforts focus on mitigating losses at circuit interfaces, including metal--substrate, substrate--air, and metal--air interfaces. However, the correlation between TLS and non-TLS losses with the intrinsic properties of the superconducting metal and the dielectric edge smoothness is not well studied. In this work, we link the aluminum film grain size to non-TLS losses and the dielectric trimming profile and roughness to TLS loss; both loss mechanisms are subsequently mitigated. To reduce metal-related losses, we engineer the aluminum microstructure by heating during deposition, increasing grain size and reducing grain boundary density. Beyond mitigating metal losses, we introduce a two-step etching technique, Tropic etching, to suppress dielectric TLS loss by producing an ultra-smooth silicon surface with minimal defects and redeposition. These results lay out the fabrication pathway for aluminum resonators with lower loss, demonstrating two-orders-of-magnitude improvement in quality factor from 6×1046\times10^{4}6×104 to 2.3×1062.3\times10^{6}2.3×106. Since aluminum is the basis for most high-coherence Josephson junctions and dielectric edges are inherent to all common device geometries, the improvements in aluminum microstructure and edge profiling, presented here, can enhance the performance of superconducting quantum devices.
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.
The recent realization of millisecond-scale coherence with tantalum-on-silicon transmon qubits showed that depositing the Al/AlOx/Al Josephson junction in a high purity, ultrahigh vacuum environment was critical for achieving lifetime-limited coherence, motivating careful examination of the aluminum surface two-level system (TLS) bath. Here, we measure the microwave absorption arising from surface TLSs in superconducting aluminum resonators, following methodology developed for tantalum resonators. We vary film and surface properties and correlate microwave measurements with materials characterization. We find that the lifetimes of superconducting aluminum resonators are primarily limited by surface losses associated with TLSs in the 2.7 nm-thick native AlOx. Treatment with 49% HF removes surface AlOx completely; however, rapid oxide regrowth limits improvements in surface loss and long term device stability. Using these measurements we estimate that TLSs in aluminum interfaces contribute around 27% of the relaxation rate of state-of-the-art tantalum-on-silicon qubits that incorporate aluminum-based Josephson junctions.
Abstract We demonstrate aluminum-on-silicon planar transmon qubits with time-averaged T 1 energy relaxation times of up to 270 μs, corresponding to Q = 5 million, and a highest observed value of 501 μs. Through materials analysis techniques and numerical simulations we investigate the dominant source of energy loss, and devise and demonstrate a strategy toward its mitigation. Growing aluminum films thicker than 300 nm reduces the presence of oxide, a known host of defects, near the substrate-metal interface, as confirmed by time-of-flight secondary ion mass spectrometry. A loss analysis of coplanar waveguide resonators shows that this results in a reduction of dielectric loss due to two-level system defects. The correlation between the enhanced performance of our devices and the film thickness is due to the aluminum growth in columnar structures of parallel grain boundaries: transmission electron microscopy shows larger grains in the thicker film, and consequently fewer grain boundaries containing oxide near the substrate-metal interface.
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.