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arXiv:2405.12417 · Physical Review Applied

Cryogenic growth of tantalum thin films for low-loss superconducting circuits

Teun A. J. van Schijndel, Anthony McFadden, Aaron N. Engel, Jason T. Dong, Wilson Yanez, M. Parthasarathy, Raymond W. Simmonds, C. J. Palmstrøm

Published Mar 12, 2025• 15 citations
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Abstract

Motivated by recent advancements highlighting $\mathrm{Ta}$ as a promising material in low-loss superconducting circuits and showing long coherence times in superconducting qubits, we have explored the effect of cryogenic temperatures on the growth of $\mathrm{Ta}$ and its integration in superconducting circuits. Cryogenic growth of $\mathrm{Ta}$ using a low-temperature molecular beam epitaxy (MBE) system is found to stabilize single-phase $\ensuremath{\alpha}$-$\mathrm{Ta}$ on several different substrates, which include ${\mathrm{Al}}_{2}{\mathrm{O}}_{3}(0001)$, $\mathrm{Si}$(001), $\mathrm{Si}$(111), ${\mathrm{Si}\mathrm{N}}_{x}$, and $\mathrm{Ga}\mathrm{As}$(001). The substrates are actively cooled down to cryogenic temperatures and remain 20 K during the $\mathrm{Ta}$ deposition. X-ray $\ensuremath{\theta}$-$2\ensuremath{\theta}$ diffraction (XRD) after warming to room temperature indicates the formation of polycrystalline $\ensuremath{\alpha}$-$\mathrm{Ta}$. The 50-nm $\ensuremath{\alpha}$-$\mathrm{Ta}$ films grown on ${\mathrm{Al}}_{2}{\mathrm{O}}_{3}(0001)$ at a substrate manipulator temperature of 7 K have a room temperature resistivity (${\ensuremath{\rho}}_{300\phantom{\rule{0.1em}{0ex}}\mathrm{K}}$) of $13.4\phantom{\rule{0.1em}{0ex}}\text{\ensuremath{\mu}}\mathrm{\ensuremath{\Omega}}\phantom{\rule{0.2em}{0ex}}\mathrm{cm}$, a residual resistivity ratio (RRR) of 17.3 and a superconducting transition temperature (${T}_{C}$) of 4.14 K, which are comparable to bulk values. In addition, atomic force microscopy (AFM) indicates that the film grown at 7 K with an rms roughness of 0.45 nm was significantly smoother than the one grown at room temperature. Similar properties are found for films grown on other substrates. Results for films grown at higher substrate manipulator temperatures show higher ${\ensuremath{\rho}}_{300\phantom{\rule{0.1em}{0ex}}\mathrm{K}}$, lower RRR and $\mathrm{Tc}$, and increased $\ensuremath{\beta}$-$\mathrm{Ta}$ content. Coplanar waveguide resonators with a gap width of $3\phantom{\rule{0.1em}{0ex}}\text{\ensuremath{\mu}}\mathrm{m}$ fabricated from cryogenically grown $\mathrm{Ta}$ on $\mathrm{Si}$(111) and ${\mathrm{Al}}_{2}{\mathrm{O}}_{3}(0001)$ show low-power ${Q}_{i}$ of 1.9 million and 0.7 million, respectively, indicating polycrystalline $\ensuremath{\alpha}$-$\mathrm{Ta}$ films may be promising for superconducting qubit applications even though they are not fully epitaxial.

DOI
10.1103/physrevapplied.23.034025

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Tantalum films incorporated into superconducting circuits have exhibited low surface losses, resulting in long-lived qubit states. The remaining loss pathways originate in microscopic defects that manifest as two level systems (TLSs) at low temperatures. These defects limit performance, so careful attention to tantalum film structures is critical for optimal use in quantum devices. In this work, we investigate the growth of tantalum using magnetron sputtering on sapphire, Si, and photoresist substrates. In the case of sapphire, we present procedures for the growth of fully-oriented films with α-Ta [1 1 1]//Al2O3 [0 0 0 1] and α-Ta [1 −1 0]//Al2O3 [1 0 −1 0] orientational relationships and having residual resistivity ratio (RRR) ∼ 60 for 220 nm thick films. On Si, we find a complex grain texturing with Ta [1 1 0] normal to the substrate and RRR ∼ 30. We further demonstrate airbridge fabrication using Nb to nucleate α-Ta on photoresist surfaces. For the films on sapphire, resonators show TLS-limited quality factors of 1.3 ± 0.3 × 106 at 10 mK (for a waveguide gap and conductor width of 3 and 6 μm, respectively). Structural characterization using scanning electron microscopy, x-ray diffraction, low temperature transport, secondary ion mass spectrometry, and transmission electron microscopy reveal the dependence of residual impurities and screw dislocation density on processing conditions. The results provide practical insights into the fabrication of advanced superconducting devices including qubit arrays and guide future works on crystallographically deterministic qubit fabrication.
Developing alternative material platforms for use in superconductor–semiconductor hybrid structures is desirable due to limitations caused by intrinsic microwave losses present in commonly used III/V material systems. With the recent reports on tantalum superconducting qubits that show improvements over the Nb and Al counterparts, exploring Ta the superconductor in hybrid material systems is promising. Here, we study the growth of Ta on semiconducting Ge (001) substrates grown via molecular beam epitaxy. We show that at a growth temperature of 400 °C, the Ta diffuses into the Ge matrix in a self-limiting nature resulting in smooth and abrupt surfaces and interfaces with roughness on the order of 3–7 Å as measured by atomic force microscopy and x-ray reflectivity. The films are found to be a mixture of Ta5Ge3 and TaGe2 binary alloys and form a native oxide that seems to form a sharp interface with the underlying film. These films are superconducting with a TC∼1.8−2 K and HC⊥∼1.88 T, HC∥∼5.1 T. These results show this tantalum germanide film to be promising for future superconducting quantum information platforms.
Abstract The use of α -tantalum in superconducting circuits has enabled a considerable improvement in the coherence time of transmon qubits. The standard approach to grow α -tantalum thin films on silicon involves heating the substrate, which takes several hours per deposition and prevents the integration of this material with wafers containing temperature-sensitive components. We report a detailed experimental study of an alternative growth method of α -tantalum on silicon, which is achieved at room temperature through the use of a niobium seed layer. Despite a substantially higher density of oxygen-rich grain boundaries in the films sputtered at room temperature, resonators made from these films are found to have state-of-the-art quality factors, comparable to resonators fabricated from tantalum grown at high temperature. This finding challenges previous assumptions about correlations between material properties and microwave loss of superconducting thin films, and opens a new avenue for the integration of tantalum into fabrication flows with limited thermal budget.
This is a study of the growth of titanium-nitride (TiN) by plasma assisted molecular beam epitaxy (MBE) for applications in low loss quantum circuits. Titanium nitride is a material known to have low loss at microwave frequencies which sees practical use in many emerging quantum device architectures. The goal of this research is to investigate improvements in TiN thin films utilizing MBE to produce highly pure, highly crystalline films. A review of the theory of superconducting qubits is given and recent developments in superconducting qubit research are summarized to elucidate how loss has been reduced historically and the importance of materials improvements to the future of scalable quantum computation. The dynamics of epitaxial film growth are discussed, focusing on the formation of a minimum energy surface, the thermally driven kinetics of atoms deposited on the surface, and how these lead to the formation of large scale crystalline domains in the film. An overview of the MBE growth chamber is given and the growth procedure for TiN is discussed. Transport and morphology measurement results are discussed for MBE TiN where, for optimized growth conditions, films are highly crystalline with superconducting transition temperatures(Tc) as high as Tc = 6.1K, matching the value for bulk crystals and exceeding all reported thin film values. Microwave loss measurements of transmission line resonators fabricated from these films are shown to have low-power quality factors(Q) as high as 200,000 and an increase to Q = 400,000 at high power, consistent with the saturation of two-level-systems (TLS) at high power. These results confirm a connection between the high quality crystalline materials produced in this work and low loss in quantum circuits.
Abstract Building usefully coherent superconducting quantum processors depends on reducing losses in their constituent materials.1 Tantalum, like niobium, has proven utility as the primary superconducting layer within highly coherent qubits.2,3 But, unlike Nb, high temperatures are typically used to stabilize the desirable body-centered-cubic phase, α-Ta, during thin film deposition. It has long been known that a thin Nb layer permits the room-temperature nucleation of α-Ta,4-6 although neither an epitaxial process nor few-photon microwave loss measurements have been reported for Nb-nucleated Ta films prior to this study. We compare resonators patterned from Ta films grown at high temperature (500 °C) and films nucleated at room temperature, in order to understand the impact of crystalline order on quantum coherence. In both cases, films grew with Al2O3 (001) || Ta (110) indicating that the epitaxial orientation is independent of temperature and is preserved across the Nb/Ta interface. We use conventional low-power spectroscopy to measure two level system (TLS) loss, as well as an electric-field bias technique to measure the effective dipole moments of TLS in the surfaces of resonators. In our measurements, Nb-nucleated Ta resonators had greater loss tangent (1.5 ± 0.1 × 10-5) than nonnucleated (5 ± 1 × 10-6) in approximate proportion to defect densities as characterized by X-ray diffraction (0.27 ° vs 0.18 ° [110] reflection width) and electron microscopy (30 nm vs 70 nm domain size). The dependence of the loss tangent on domain size indicates that the development of more ordered Ta films is likely to lead to improvements in qubit coherence times.1,7 Moreover, lowtemperature α-Ta epitaxy may enable the growth of new, microstate-free heterostructures which would not withstand high temperature processing.8
Quantum coherence in superconducting circuits has increased steadily over the last decades as a result of a growing understanding of the various loss mechanisms. Recently, tantalum (Ta) emerged as a promising material to address microscopic sources of loss found on niobium (Nb) or aluminum (Al) surfaces. However, the effects of film and interface microstructure on low-temperature microwave loss are still not well understood. Here we present a systematic study of the structural and electrical properties of Ta and Nb films sputtered on c-plane sapphire at varying growth temperatures. As growth temperature is increased, our results show that the onset of epitaxial growth of alpha-phase Ta correlates with lower Ta surface roughness, higher critical temperature, and higher residual resistivity ratio, but surprisingly also correlates with a significant increase in loss at microwave frequency. Notably, this high level of loss is not observed in Nb films prepared in the same way and having very similar structure. By experimentally controlling the surface on which the Ta film is nucleated, we determine that the source of loss is only present in samples having an epitaxial Ta/sapphire interface and show that it is apparently mitigated by either growing a thin, epitaxial Nb inter-layer between the Ta film and the substrate or by intentionally treating, and effectively damaging, the sapphire surface with an in-situ argon plasma before Ta growth. In addition to elucidating this interfacial microwave loss, this work provides adequate process details to aid reproducible growth of low-loss Ta films across fabrication facilities.