We report the dielectric functions of insulating tantalum nitride (TaN) films, deposited using atomic layer deposition (ALD) on 300 mm Si/SiO2 substrates, to demonstrate their suitabilityas tunnel barriers in tantalum-based Josephson junctions (JJ) for superconducting quantum circuits. The temperature-dependent ellipsometric angles were measured using ALD TaN films with nominal thicknesses of 13 nm and 25 nm at an incidence angle of 70 degrees, across photon energy ranges of 0.03 eV to 0.7 eV (80-300 K) and 0.5 eV to 6.5 eV (80-600 K). This data was used to develop a dispersion model for insulating ALD TaN films that incorporates a Tauc-Lorentz oscillator with a band gap of 1.5-1.8 eV to model the interband optical transitions. The extracted dielectric function of ALD TaN films shows an insulating behavior (mid-infrared transparency) at all temperatures and for both film thicknesses tested. ALD TaN does not exhibit infrared absorption due to free carriers, even at elevated temperatures, demonstrating its insulating nature, which is required for the tunnel barrier of the JJ in quantum applications. The results of transmission electron microscopy, including selected area electron diffraction, and X-ray diffraction are also discussed. Sputter depth-profile X-ray photoelectron spectroscopy (XPS) shows an N/Ta ratio of ~1.2 throughout the film. The lower band gap, low roughness, and thermal stability of ALD TaN compared to AlOx suggest the possibility of fabricating JJs with thicker barriers while achieving critical current densities required for qubits, better control of thickness and composition, reduced topography, and resistance to aging.
Despite constituting a smaller fraction of the qubits electromagnetic mode, surfaces and interfaces can exert significant influence as sources of high-loss tangents, which brings forwardthe need to reveal properties of these extended defects and identify routes to their control. Here, we examine the structure and composition of the metal-substrate interfacial layer that exists in Ta/sapphire-based superconducting films. Synchrotron-based X-ray reflectivity measurements of Ta films, commonly used in these qubits, reveal an unexplored interface layer at the metal-substrate interface. Scanning transmission electron microscopy and core-level electron energy loss spectroscopy identified an approximately 0.65 \ \text{nm} \pm 0.05 \ \text{nm} thick intermixing layer at the metal-substrate interface containing Al, O, and Ta atoms. Density functional theory (DFT) modeling reveals that the structure and properties of the Ta/sapphire heterojunctions are determined by the oxygen content on the sapphire surface prior to Ta deposition, as discussed for the limiting cases of Ta films on the O-rich versus Al-rich Al2O3 (0001) surface. By using a multimodal approach, integrating various material characterization techniques and DFT modeling, we have gained deeper insights into the interface layer between the metal and substrate. This intermixing at the metal-substrate interface influences their thermodynamic stability and electronic behavior, which may affect qubit performance.
The lifetime of superconducting qubits is limited by dielectric loss, and a major source of dielectric loss is the native oxide present at the surface of the superconducting metal.Specifically, tantalum-based superconducting qubits have been demonstrated with record lifetimes, but a major source of loss is the presence of two-level systems (TLSs) in the surface tantalum oxide. Here, we demonstrate a strategy for avoiding oxide formation by encapsulating the tantalum with noble metals that do not form native oxide. By depositing a few nanometers of Au or AuPd alloy before breaking vacuum, we completely suppress tantalum oxide formation. Microwave loss measurements of superconducting resonators reveal that the noble metal is proximitized, with a superconducting gap over 80% of the bare tantalum at thicknesses where the oxide is fully suppressed. We find that losses in resonators fabricated by subtractive etching are dominated by oxides on the sidewalls, suggesting total surface encapsulation by additive fabrication as a promising strategy for eliminating surface oxide TLS loss in superconducting qubits.