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Material and Interface Engineering Strategies to Mitigate Decoherence in Superconducting Qubits

Dominic P. Goronzy, Anthony McFadden, David A. Garcia Wetten, Mitchell J. Walker, André Vallières, Megan E. Russell, Carlos G. Torres‐Castanedo, Thang Pham, Nicholas Materise, Cameron Kopas, Jayss Marshall, Ella Lachman, Nikolay Zhelev, James A. Sauls, J. Mutus, Corey Rae McRae, Vinayak P. Dravid, Michael J. Bedzyk, Mark C. Hersam

Published Sep 23, 2024• 0 citations
Publisher

Abstract

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)

DOI
10.2172/2448589

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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)
With massive improvements in device coherence times and gate fidelity over the past two decades, superconducting quantum devices have emerged as a leading technology platform for next generation quantum computing. While many of these improvements have been driven through optimized device designs and geometries, the presence of defects, impurities, interfaces, and surfaces in the constituent materials continue to limit performance and present a critical barrier in achieving scalable quantum systems with long coherence times. As part of the Superconducting Quantum Materials and Systems (SQMS) center, we have applied state-of-the-art materials characterization techniques, such as scanning/transmission electron microscopy, secondary ion mass spectrometry, and atom probe tomography, to identify structural defects and chemical inhomogeneities in superconducting qubits. In this review, we discuss the findings of these efforts as they relate to the inherent surfaces, interfaces, impurities, and defects in superconducting qubits. Through this comprehensive investigation, we provide insight into possible sources of dissipation in these systems. Further, we supplement these findings with potential strategies for mitigating these undesired features in an effort to systematically and intelligently improve the coherence times of superconducting qubits.
Improving qubit lifetime is essential for fault-tolerant quantum computing. It is widely acknowledged that intricate processing techniques introduce defects at the interfaces and surfaces of superconducting quantum circuits, which can create sources of decoherence. Therefore, a precise understanding of how a material's structure contributes to decoherence is critical for enhancing the performance of superconducting qubits. This talk highlights our recent advancements in understanding surface oxides in resonators and ultrathin aluminum oxide barriers in Josephson junctions (JJs) using transmission electron microscopy and spectroscopy techniques [1-4]. The Superconducting Quantum Materials & Systems Center (SQMS) demonstrated that encapsulating niobium surfaces with a ∼10nm tantalum layer results in 2-5x longer T1​ than bare niobium [2]. Our collaborative investigation shows that this improvement is attributed to tantalum's less lossy surface oxide, which contains fewer sub-oxides than niobium oxide. Moreover, the amorphous Ta2O5 shows a bonding nature closer to crystalline form than amorphous Nb2O5, potentially reducing hydrogen diffusion toward the oxide/metal interface [1, 2]. Moreover, we will briefly discuss our preliminary study of the thin film structure under cryogenic conditions down to 20K, conducted using a liquid helium TEM holder in a Thermo Cs-corrected Titan. We also explored the effect of aluminum deposition rates on aluminum oxide microstructure and qubit lifetime. Although increasing the deposition rate from 0.5 Å/s to 5 Å/s significantly improved oxide layer roughness and thickness variation, the qubits’ coherence remained unchanged. This is likely due to Cooper pairs only tunneling through the thinnest parts of the barrier, making them less affected by the grain boundaries in the thin aluminum films. Additionally, we uncovered a stress-induced grain boundary sliding mechanism, which contributes to short-circuit failures in JJs [4]. Our discovery provides vital insight into oxide microstructure and superconducting qubits’ functionality [5].
Superconducting qubits have emerged as a potentially foundational platform technology for addressing complex computational problems deemed intractable with classical computing. Despite recent advances enabling multiqubit designs that exhibit coherence lifetimes on the order of hundreds of μs, material quality and interfacial structures continue to curb device performance. Two-level system defects in the thin superconducting film and adjacent dielectric regions introduce stochastic noise and dissipate electromagnetic energy at the cryogenic operating temperatures. In this study, we utilize time-of-flight secondary ion mass spectrometry to understand the role specific fabrication procedures play in introducing such dissipation mechanisms in these complex systems. We interrogated Nb thin films and transmon qubit structures fabricated through slight modifications in the processing and vacuum conditions. We find that when the Nb film is sputtered onto the Si substrate, oxide and silicide regions are generated at various interfaces. We also observe that impurity species, such as niobium hydrides and carbides, are incorporated within the niobium layer during the subsequent lithographic patterning steps. The formation of these resistive compounds likely impacts the superconducting properties of the Nb thin film. Additionally, we observe the presence of halogen species distributed throughout the patterned thin films. We conclude by hypothesizing the source of such impurities in these structures in an effort to intelligently fabricate superconducting qubits and extend coherence times moving forward.
The development of quantum computers, capable of surpassing classical computing in solving specific complex problems, hinges on breakthroughs in materials science, precision device fabrication, and the optimization of quantum architectures [1]. Among the leading candidates for quantum computation, superconducting qubits, particularly those based on transmon designs, have shown promising advances with coherence times reaching hundreds of microseconds [2]. However, to fully unlock the potential of scalable quantum computing, further enhancements in coherence are necessary. The intricate structure-coherence relationship within these devices, especially at critical interfaces such as metal-air, metal-dielectric, and metal-substrate in Josephson junctions (JJs), poses a significant challenge due to the potential for two-level-system loss channels. Here, we detail our pioneering efforts to understand these structure-coherence relationships utilizing advanced electron microscopy techniques. Focusing on the Al-AlOx and Al-Si substrate interfaces in Josephson Junctions, we employ a combination of low-loss and core-loss electron energy loss spectroscopy (EELS) and four-dimensional scanning transmission electron microscopy (4D-STEM) conducted at room and ultra-low temperatures (sub-6 K). This approach allows for an unprecedented examination of the chemical composition, bonding environments, and nanoscale structures of key surfaces and interfaces critical to the quantum coherence. Figure 1 presents a typical superconducting architecture at the chip level; each superconducting qubit consists of a Josephson Junction in parallel with an ultra-low-loss capacitor to create a resonant structure in the 3-6GHz range. JJs are highlighted in the area boxed in Fig. 1A and can be observed in detail in Fig. 1B. Lamella cross-sections (as shown in Fig. 1C) were prepared using a dual-beam focused ion beam (FIB) FEI-SEM Helios Nanolab. The lift-off was performed using 30 kV Ga+ ions, and the final cleaning step was carried out at 2 kV to remove surface damage on the area of interest, resulting in a final sample thickness of 50-100 nm. Transmission electron microscopy (TEM) and scanning transmission electron microscopy (STEM) data were collected on a probe-corrected JEOL ARM200 S/TEM operating at 200 kV. The convergent angle for ADF-STEM imaging was 25 mrad. Electron energy loss spectra (EELS) were acquired at 200 kV using a Gatan GIF Quantum on a K2 pixelated detector. Data processing (background subtraction, plural scattering removal, and signal mapping) was conducted using Gatan GMS software. Four-dimensional STEM (4D-STEM) data were collected by a K3 and STELA cameras. The convergent angles were 0.5-1.5 mrad, and the camera length was 6-10 cm. The step size was 5-10 Å. Merging microscopic insights with electrical data and theoretical frameworks, we aim to reveal how atomic-scale irregularities affect coherence times. Our results highlight key decoherence mechanisms in superconducting qubits and suggest specific improvements for qubit design and manufacturing. By linking electron microscopy findings to device performance, we outline strategies to reduce decoherence, essential for achieving reliable quantum computing. This work bridges materials science and quantum engineering, driving efforts in making scalable quantum computers forward [3]. A) Microscopic view of a superconducting transmon qubit, highlighting its symmetric design with central island and capacitor pads. B) SEM image of a JJ displaying their Al top and bottom contacts. C) STEM image of a JJ showing its key components and interfaces: Al top and bottom contact, AlOx tunnel barrier, Si substrate and Al-Si interface. A) EELS chemical maps of two interfaces, Al/Al and Al/Si using K-edges of oxygen, aluminum and silicon of a Josephson junction. It is possible to detect a formation of oxides at both interfaces. Plots showing Al and Si K-edge at 1560 eV and 1839 eV, respectively, and the ELNES are shown on the right side (Scale bar in A – 20 nm). B) Analysis of the disordered Al phases at the interfaces utilizing ePDF.
Quantum computation is a fascinating field that combines novel physics with improvements in computation times and has been rapidly growing in the past few years. Using superconductors to form the qubits has the potential for large-scale computing, if the decoherence inherent in these devices can be understood and reduced. Two-level fluctuators due to defects in the materials are thought to cause changes to the Josephson critical current or the flux through the superconducting loop of a flux qubit, which leads to decoherence in the qubit. Alternatively, defects in the crystal lattice give rise to electron localization which in turn traps spins with random orientations at the substrate/metal interface, again producing decoherence. My work studied the proposed noise mechanisms by using Molecular Beam Epitaxy to fabricate single-crystal niobium-based Josephson junctions. Using RHEED, AFM, and TEM/STEM, I studied the epitaxy of the niobium film at the substrate interface to reduce noise due to crystal defects. I then measured flux noise in these films; the noise in the epitaxial films is lower than the comparative polycrystalline films. Further measurements using ex-situ Josephson junctions and epitaxial niobium loops resulted in the lowest reported flux noise measurements to date. Additionally, EELS measurements made in the course of the STEM analysis of the crystal structure reveal oxygen depletion from the substrate at elevated growth temperatures. This depletion leads to oxygen vacancies in the aluminum oxide substrate, which can in turn lead to charge traps at the substrate/metal interface and hence to decoherence in the qubit. Critical current noise was investigated by changing the oxidation dose of the alumina barrier in more than 50 separate Josephson junctions. Films which were grown with lower oxidation doses have a non-ideal critical current temperature dependence as well as higher critical current noise values, suggesting that insufficient oxygen is being incorporated into these junctions. Finally, I studied the effect of surface cleaning after fabrication for resonators and transmons. Microscopy shows that an oxygen ash and BOE dip together removes all photoresist residue from the chip. Internal-Q measurements do not show a marked improvement due to this cleaning, but the coherence times do improve upon the cleaning step.
SQMS Nanofabrication Taskforce, which brings together experts in nanofabrication and materials science at the SQMS Center, has been launched to implement novel materials, substrates, and fabrication techniques for high coherence superconducting quantum devices. In a first coordinated effort, the Nanofabrication Taskforce developed fabrication processes to eliminate the lossy materials at surfaces and interfaces of superconducting qubits to enhance qubit coherence. The initial results of this study demonstrated T1 enhancement by almost an order of magnitude with best T1 s reaching ~ 600 μ\muμs. [1] We attribute this improvement to the replacement of lossy native Nb oxide layer with native Ta oxide, which is thinner and less disordered. we are now currently working on strategies with an aim towards moving qubit coherence times to millisecond timescales and beyond. The results of a systematic study will be presented to address substrate preparation, alternative materials as low loss platforms (Nb, Ta, and Re), novel non-oxide forming low loss capping layers such as proximitized Au, optimized qubit designs, and optimized Josephson junction materials, processing, and design.