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].
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].
An ultra-thin aluminum oxide layer is a key component for Josephson junctions (JJ) in superconducting quantum bits (qubits). This layer serves as a barrier layer for Cooper pairs tunneling between the superconducting electrodes and significantly influences the overall performance of the junction. In this study, we investigate the impact of aluminum deposition rates on the microstructure and chemical variation of the aluminum oxide layer, as well as the device’s yields and qubits’ lifetimes. Surprisingly, although the oxide layer roughness and thickness variation improve noticeably with an increasing Al deposition rate from 0.5 Å/s to 5 Å/s, the qubit’s coherence time is almost unchanged. We attribute this to the fact that Cooper pairs tunnel only through the thinnest region of the barrier. Additionally, we revealed a stress-induced grain boundary sliding short-circuit failure mechanism in the JJ. Our discovery provides a vital understanding of oxide microstructure and JJ functionality, which are critical for improving the coherence time of superconducting qubits.
High Resolution Image Download MS PowerPoint Slide Improving the qubit’s lifetime (T 1 ) is crucial for fault-tolerant quantum computing. Recent advancements have shown that replacing niobium (Nb) with tantalum (Ta) as the base metal significantly increases T 1, likely due to a less lossy native surface oxide. However, understanding the formation mechanism and nature of both surface oxides is still limited. Using aberration-corrected transmission electron microscopy and electron energy loss spectroscopy, we found that Ta surface oxide has fewer suboxides than Nb oxide. We observed an abrupt oxidation state transition from Ta 2 O 5 to Ta, as opposed to the gradual shift from Nb 2 O 5, NbO 2, and NbO to Nb, consistent with thermodynamic modeling. Additionally, amorphous Ta 2 O 5 exhibits a closer-to-crystalline bonding nature than Nb 2 O 5, potentially hindering H atomic diffusion toward the oxide/metal interface. Finally, we propose a loss mechanism arising from the transition between two states within the distorted octahedron in an amorphous structure, potentially causing two-level system loss. Our findings offer a deeper understanding of the differences between native amorphous Ta and Nb oxides, providing valuable insights for advancing superconducting qubits through surface oxide engineering.
Abstract We present a transmon qubit fabrication technique that yields systematic improvements in T 1 relaxation times. We encapsulate the surface of niobium and prevent the formation of its lossy surface oxide. By maintaining the same superconducting metal and only varying the surface, this comparative investigation examining different capping materials, such as tantalum, aluminum, titanium nitride, and gold, as well as substrates across different qubit foundries demonstrates the detrimental impact that niobium oxides have on coherence times of superconducting qubits, compared to native oxides of tantalum, aluminum or titanium nitride. Our surface-encapsulated niobium qubit devices exhibit T 1 relaxation times 2–5 times longer than baseline qubit devices with native niobium oxides. When capping niobium with tantalum, we obtain median qubit lifetimes above 300 μs, with maximum values up to 600 μs. Our comparative structural and chemical analysis provides insight into why amorphous niobium oxides may induce higher losses compared to other amorphous oxides.
Superconducting qubits are among the most advanced platforms for quantum information, offering potential scalability and compatibility with standard device fabrication techniques [1-5]. Among the materials investigated for superconducting qubits, Tantalum (Ta) has emerged as a compelling candidate due to its self-terminating stoichiometric surface oxide and chemical resistance to harsh post-fabrication processes. Efforts to mitigate surface loss by treating the surface oxides and utilizing high-resistivity silicon substrates have led to Ta-based qubits with lifetime and coherence times exceeding 1 ms [3]. Guided by these successes in reducing dielectric loss in Ta-based devices, we are interested in exploring material engineering approaches that enhance the superconducting gap. Alloying Ta with another element to enhance the superconducting performance expands the range of viable material candidates available to tackle different loss channels in superconducting circuits [1]. Recently, we explore superconducting gap engineering in Ta-based devices as a powerful strategy for expanding the range of suitable host materials. By alloying 20 at.% hafnium (Hf) into Ta thin films, we achieve a superconducting transition temperature (Tc) of 6.09 K as observed in direct current (DC) transport measurements, reflecting an increase in the superconducting gap. Here we demonstrate an approach for controlling varying deposition conditions to control film orientation and transport properties of Ta and Ta-Hf alloy thin films. We investigate the microstructure and composition distribution of the thin films by using high-resolution scanning transmission electron microscopy (STEM) with super-X EDS system (no serious beam damage issue [6-8]). Our structural analysis using TEM diffraction and STEM verifies the BCC structure across all the films (Figure 1), and direct current (DC) transport measurements reveal a 40% enhancement in Tc relative to undoped Ta (Tc=4.3 K). We monitored oxide growth over an 18-day period following film deposition to better understand how Hf incorporation influences surface oxides. In both Ta and Hf spectra, the fraction of fully oxidized (Ta2O5 and HfO2) states gradually increased during the 18-day exposure, indicating progressive surface oxidation. To estimate the surface oxide thickness, we use cross-sectional TEM/EDS mapping (Figure 1c). The analysis reveals that the oxide thickness for the 1 ks Ta-Hf alloy film is approximately 3 nm in thickness, comparable to the 3 nm oxide observed on native Ta [2]. For the 2 ks Ta-Hf film, the oxide thickness increases slightly to about 4 nm (Figure 1). The measured surface loss tangent of the Ta-Hf alloy remains comparable to that of native Ta. This result suggests that the surface oxide of the Ta-Hf alloy, which contains a measurable fraction of HfOx, does not introduce additional dielectric loss. By engineering the alloy composition and film deposition, this study achieves both improved superconducting properties and compatibility with fabrication processes. These findings show that material doping and alloying can strategically expand the suite of viable materials for superconducting quantum devices. This approach provides a pathway for tailoring material properties to support the next generation of quantum technologies and offers broad relevance to researchers in materials science, quantum information, and device engineering [9]. STEM images on cross sections of 1 ks (a) and 2 ks (b) Ta-Hf thin films, both films were sputtered at 750 ◦C. (c) Cross-sectional EDS elemental mapping on Ta-Hf. Cross-sectional EDS mapping Ta (blue) and Hf (orange) confirmed a uniform Ta-Hf alloy with the Ta to Hf atomic ratios for the bulk to be (83% : 17%). The oxygen (red) map reveals a surface oxide layer with the estimated surface oxide thickness of around 4 nm. The 1 ks Ta-Hf film exhibits an oxide thickness of approximately 3 nm, similar to that of native Ta. The EDS resolution limit is 0.5 atomic percent.
Superconducting thin films of niobium have been extensively employed in transmon qubit architectures. Although these architectures have demonstrated improvements in recent years, further improvements in performance through materials engineering will aid in large-scale deployment. Here, we use information retrieved from secondary ion mass spectrometry and electron microscopy to conduct a detailed assessment of the surface oxide that forms in ambient conditions for transmon test qubit devices patterned from a niobium film. We observe that this oxide exhibits a varying stoichiometry with NbO and NbO 2 found closer to the niobium film/oxide interface and Nb 2 O 5 found closer to the surface. In terms of structural analysis, we find that the Nb 2 O 5 region is semicrystalline in nature and exhibits randomly oriented grains on the order of 1–3 nm corresponding to monoclinic N–Nb 2 O 5 that are dispersed throughout an amorphous matrix. Using fluctuation electron microscopy, we are able to map the relative crystallinity in the Nb 2 O 5 region with nanometer spatial resolution. Through this correlative method, we observe that the highly disordered regions are more likely to contain oxygen vacancies and exhibit weaker bonds between the niobium and oxygen atoms. Based on these findings, we expect that oxygen vacancies likely serve as a decoherence mechanism in quantum systems.
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)