arXiv:2408.02863 · Materials for Quantum Technology
Enhanced superconducting qubit performance through ammonium fluoride etch
Cameron Kopas, Dominic P. Goronzy, Thang Pham, Carlos G. Torres‐Castanedo, Matthew Cheng, Rory Cochrane, Patrick Nast, Ella Lachman, Nikolay Zhelev, André Vallières, Akshay A. Murthy, Jin‐Su Oh, L.W. Zhou, Matthew Joseph Kramer, Hilal Cansizoglu, Michael J. Bedzyk, Vinayak P. Dravid, Alexander Romanenko, Anna Grassellino, J. Mutus, Mark C. Hersam, Kameshwar K. Yadavalli
Abstract The performance of superconducting qubits is often limited by dissipation and two-level systems (TLS) losses. The dominant sources of these losses are believed to originate from amorphous materials and defects at interfaces and surfaces, likely as a result of fabrication processes or ambient exposure. Here, we explore a novel wet chemical surface treatment at the Josephson junction-substrate and the substrate-air interfaces by replacing a buffered oxide etch (BOE) cleaning process with one that uses hydrofluoric acid followed by aqueous ammonium fluoride. We show that the ammonium fluoride etch process results in a statistically significant improvement in median T 1 by ∼ 22 % (p = 0.002), and a reduction in the number of strongly-coupled TLS in the tunable frequency range. Microwave resonator measurements on samples treated with the ammonium fluoride etch after niobium deposition and etching also show ∼ 33 % lower TLS-induced loss tangent compared to the BOE treated samples. As the chemical treatment primarily modifies the Josephson junction-substrate interface and substrate-air interface, we perform targeted chemical and structural characterizations to examine materials differences at these interfaces and identify multiple microscopic changes that could contribute to decreased TLS losses.
Abstract The performance of superconducting qubits is often limited by dissipation and two-level systems (TLS) losses. The dominant sources of these losses are believed to originate from amorphous materials and defects at interfaces and surfaces, likely as a result of fabrication processes or ambient exposure. Here, we explore a novel wet chemical surface treatment at the Josephson junction-substrate and the substrate-air interfaces by replacing a buffered oxide etch (BOE) cleaning process with one that uses hydrofluoric acid followed by aqueous ammonium fluoride. We show that the ammonium fluoride etch process results in a statistically significant improvement in median T 1 by ∼ 22 % (p = 0.002), and a reduction in the number of strongly-coupled TLS in the tunable frequency range. Microwave resonator measurements on samples treated with the ammonium fluoride etch after niobium deposition and etching also show ∼ 33 % lower TLS-induced loss tangent compared to the BOE treated samples. As the chemical treatment primarily modifies the Josephson junction-substrate interface and substrate-air interface, we perform targeted chemical and structural characterizations to examine materials differences at these interfaces and identify multiple microscopic changes that could contribute to decreased TLS losses.
Aluminum (Al) remains the central material for superconducting qubits, and considerable effort has been devoted to optimizing its deposition and patterning for quantum devices. However, post-processing strategies focused on oxide removal of niobium (Nb) and tantalum (Ta) -based resonators using buffered oxide etch (BOE), which can not be used for Al. This challenge becomes particularly relevant for industry-scale fabrication with multi-chip bonding, where delays between sample preparation and cooldown require surface treatments that preserve low dielectric loss during extended exposure to ambient conditions. In this work, we investigate surface modification approaches for Al resonators subjected to a 24-hour delay prior to cryogenic measurement. Passivation using self-limiting oxygen and fluorine chemistries was evaluated utilizing different plasma processes. Remote oxygen plasma treatment reduced dielectric losses, in contrast to direct oxygen plasma. A fluorine-based plasma process was developed that passivated the Al surface for subsequent BOE treatment. However, the fluorine content in the surface resulted in higher loss, identifying fluorine as an unsuitable passivation material for Al resonators. Above all, selective oxide removal using HF (hydrogen fluoride) vapor and phosphoric acid yielded median dielectric losses as low as δ~LP=5.7×10−7 (QLP≈1.7M) with δ~TLS=3.6×10−7 (QTLS≈2.8M) in the single photon regime. Selective oxide removal provides a promising pathway for robust Al-based qubit fabrication, as it preserves low dielectric losses for a 24-hour delay before cooldown.
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.
While significant strides have been made to increase the coherence time of superconducting qubits, further advancements are essential for realizing scalable quantum computing. Decoherence is often a result of loss and noise stemming from two-level systems and excess quasiparticles, arising due to material defects, fabrication processes, and ambient exposure, particularly at surfaces and interfaces. Our recent efforts to mitigate these decoherence mechanisms have employed a variety of strategies, including low-loss surface encapsulation materials, advanced substrate preparation techniques, modifications to metal film growth, and the development of novel fabrication processes. The structural and chemical properties of materials, surfaces, and interfaces are studied using scanning probe microscopy, electron microscopy, photoelectron spectroscopy, mass spectrometry, and X-ray diffraction, which is correlated to device performance metrics, including superconducting resonator internal quality factor and qubit T1 time. This information is used to identify and understand material sources of loss and their origins in the device fabrication process. Through multi-institution efforts within SQMS we have identified the loss mechanism of interstitial hydrogen in niobium-based devices and shown how standard fabrication processes introduce these hydrides, developing strategies to mitigate their formation.1 Furthermore, we have characterized the metal-substrate interface, including the loss of niobium-silicides formed at that interface, and developed silicon surface treatments that reduce atomic scale roughness and oxygen content at the metal-substrate and Josephson junction interfaces.2-4 By developing the connection between materials properties and the overall performance of superconducting quantum circuitry, we can develop fabrication strategies to mitigate material losses, thus supporting the ongoing efforts to enhance coherence time in superconducting quantum devices. 1. Torres-Castanedo, C. G.*, Goronzy, D. P.*, et al., Adv. Funct. Mater., 2401365 (2024) 2. Lu, X., et al., Phys. Rev. Materials 6, 064402 (2022) 3. Berti, G., Appl. Phys. Lett. 122, 192605 (2023) 4. Kopas, C. J., Goronzy, D. P., et al., arXiv:2408.02863 (2024)
The fabrication of superconducting circuits requires multiple deposition, etching, and cleaning steps, each possibly introducing material property changes and microscopic defects. In this work, we specifically investigate the process of argon milling, a potentially coherence-limiting step, using niobium and aluminum superconducting resonators as a proxy for the surface-limited behavior of qubits. We find that niobium microwave resonators exhibit an order of magnitude decrease in quality factors after surface argon milling, while aluminum resonators are resilient to the same process. Extensive analysis of the niobium surface shows no change in the suboxide composition due to argon milling, while two-tone spectroscopy measurements reveal an increase in two-level system electrical dipole moments, indicating a structurally altered niobium oxide. However, a short dry etch can fully recover the argon-milling-induced losses on niobium, offering a potential route towards state-of-the-art overlap Josephson junction qubits with niobium circuitry.
The collaboration between the Superconducting Quantum Materials and Systems Center (SQMS) and Rigetti Computing produced several advancements in our understanding of the role of materials characteristics in quantum processor performance. This partnership leverages SQMS's extensive characterization infrastructure and cutting-edge research in materials, and Rigetti's expertise in quantum hardware and robust nanofabrication to improve precision and performance of Rigetti's test QPUs. Qubit frequency is determined in large part by the properties of Josephson junctions (JJs) made of amorphous oxide tunnel barriers; the Alternating-Bias Assisted Annealing (ABAA) process allows us to tune JJs to their desired frequency [1]. Work by SQMS researchers in characterizing high-precision JJs post-processed (using ABAA) have yielded crucial information on the nature of the structure and chemical bonding uniformity of the ABAA processed amorphous oxides. Performance has also been improved through a comprehensive series of experiments that tested encapsulation and surface treatment. Encapsulation of the niobium metal layer with tantalum resulted in an T1 improvement of 80%, experimentally confirming the role of Nb surface losses in qubit performance [2]. Pre-treatment of the underlying silicon surface prior to JJ fabrication by replacing a buffered oxide etch (BOE) with hydrofluoric acid (HF) followed by aqueous ammonium fluoride (NH4F) has shown a statistically significant improvement of T1 by 22%, and reduction in the number of strongly-coupled TLS [3]. These examples, as well as many other published and ongoing investigations, demonstrate the mutual benefits that come from Rigetti's involvement in the SQMS collaboration. [1] - Pappas, D.P., et al. (2024). https://doi.org/10.1038/s43246-024-00596-z [2] - Bal, M., et al. (2024). https://doi.org/10.1038/s41534-024-00840-x [3] Kopas, C. J. et al. Preprint at https://doi.org/10.48550/arXiv.2408.02863 (2024).
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.