We report the first evidence of the formation of niobium hydrides within niobium films on silicon substrates in superconducting qubits fabricated at Rigetti Computing. We combine complementary techniques including room and cryogenic temperature atomic scale high-resolution and scanning transmission electron microscopy (HR-TEM and STEM), atomic force microscopy (AFM), and the time-of-flight secondary ion mass spectroscopy (TOF-SIMS) to reveal the existence of the niobium hydride precipitates directly in the Rigetti chip areas. Electron diffraction and high-resolution transmission electron microscopy (HR-TEM) analyses are performed at room and cryogenic temperatures (~106 K) on superconducting qubit niobium film areas, and reveal the formation of three types of Nb hydride domains with different crystalline orientations and atomic structures. There is also variation in their size and morphology from small (~5 nm) irregular shape domains within the Nb grains to large (~10-100 nm) Nb grains fully converted to niobium hydride. As niobium hydrides are non-superconducting and can easily change in size and location upon different cooldowns to cryogenic temperatures, our findings highlight a new previously unknown source of decoherence in superconducting qubits, contributing to both quasiparticle and two-level system (TLS) losses, and offering a potential explanation for qubit performance changes upon cooldowns. A pathway to mitigate the formation of the Nb hydrides for superconducting qubit applications is also discussed.
We report the first evidence of the formation of niobium hydrides within niobium films on silicon substrates in superconducting qubits fabricated at Rigetti Computing. We combine complementary techniques including room and cryogenic temperature atomic scale high-resolution and scanning transmission electron microscopy (HR-TEM and STEM), atomic force microscopy (AFM), and the time-of-flight secondary ion mass spectroscopy (TOF-SIMS) to reveal the existence of the niobium hydride precipitates directly in the Rigetti chip areas. Electron diffraction and high-resolution transmission electron microscopy (HR-TEM) analyses are performed at room and cryogenic temperatures (~106 K) on superconducting qubit niobium film areas, and reveal the formation of three types of Nb hydride domains with different crystalline orientations and atomic structures. There is also variation in their size and morphology from small (~5 nm) irregular shape domains within the Nb grains to large (~10-100 nm) Nb grains fully converted to niobium hydride. As niobium hydrides are non-superconducting and can easily change in size and location upon different cooldowns to cryogenic temperatures, our findings highlight a new previously unknown source of decoherence in superconducting qubits, contributing to both quasiparticle and two-level system (TLS) losses, and offering a potential explanation for qubit performance changes upon cooldowns. A pathway to mitigate the formation of the Nb hydrides for superconducting qubit applications is also discussed.
We report evidence for the formation of niobium hydride phase within niobium films on silicon substrates in superconducting qubits fabricated at Rigetti Computing. For this study, we combined complementary techniques—including room-temperature and cryogenic atomic force microscopy (AFM), synchrotron x-ray diffraction, and time-of-flight secondary ion mass spectroscopy (ToF-SIMS)—to directly reveal the existence of niobium hydride precipitates on the surface of superconducting qubits. Upon cryogenic cooling, we observed variation in the size and morphology of the hydrides, ranging from small (∼5 nm) irregular shapes to large (∼10–100 nm) domains within the Nb grains, which were fully converted to niobium hydrides. Since niobium hydrides are nonsuperconducting and can easily change in size and location upon different cooldowns to cryogenic temperature, our finding highlights a previously unknown source of decoherence in superconducting qubits. This contributes to quasiparticle losses, offering a potential explanation for changes in qubit performance upon cooldowns. Finally, by leveraging the RF performance of a 3D bulk Nb resonator, we quantify RF dissipation in a superconducting qubit caused by hydrogen concentration variation, and propose a practical engineering pathway to mitigate the formation of Nb hydrides for superconducting qubit applications.
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.
Continued advances in superconducting qubit performance require more detailed understandings of the many sources of decoherence. Within these devices, two-level systems arise due to defects, interfaces, and grain boundaries and are thought to be a major source of qubit decoherence at millikelvin temperatures. In addition to Al, Nb is a commonly used metallization layer in superconducting qubits. Consequently, a significant effort is required to develop and qualify processes that mitigate defects in Nb films. As the fabrication of complete superconducting qubits and their characterization at millikelvin temperatures is a time and resource intensive process, it is desirable to have measurement tools that can rapidly characterize the properties of films and evaluate different treatments. Here, we show that measurements of the variation of the superconducting critical temperature Tc with an applied external magnetic field H (of the phase boundary Tc−H) performed with very high-resolution show features that are directly correlated with the structure of the Nb films. In combination with x-ray diffraction measurements, we show that one can even distinguish variations in the size and crystal orientation of the grains in a Nb film by small but reproducible changes in the measured superconducting phase boundary.
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)
Niobium thin films on silicon substrate used in the fabrication of superconducting qubits have been characterized using scanning and transmission electron microscopy, electrical transport, magnetization, the London penetration depth - based quasiparticle spectroscopy, and real-space real-time magneto-optical imaging. We study niobium films to provide an example of a comprehensive analytical set that may benefit superconducting circuits such as those used in quantum computers. The films have a superconducting transition temperature of Tc=9.35 K and a fairly clean superconducting gap. The estimated superfluid density is enhanced at intermediate temperatures. These observations are consistent with the recent theory of anisotropic strong-coupling superconductivity in Nb and indicate outstanding quality. However, the response to the magnetic field is complicated, exhibiting significantly irreversible behavior and insufficient heat dissipation (to a substrate), leading to thermomagnetic instabilities. This may present a challenge for further improvement of transmon quantum coherence. Possible mitigation strategies are discussed.
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.