Achieving high-quality superconducting thin films at low temperatures is a central challenge for scalable quantum device integration and Complementary Metal-Oxide-Semiconductor (CMOS)-compatible fabrication. Here, we demonstrate a room-temperature magnetron sputtering approach for synthesizing niobium nitride (NbN) thin films using a novel energy-selective ion source that enables independent control of ion energy and ion flux. This capability provides a powerful route to precisely tailor surface kinetics and crystallization pathways, overcoming longstanding limitations in stabilizing high-quality NbN at reduced temperatures. The resulting films were characterized by superconducting transport measurements, X-ray diffraction, X-ray photoelectron spectroscopy, and transmission electron microscopy. Compared with conventional reactive sputtering, ion beam-assisted growth yields a substantial narrowing of the transition width at the superconducting temperature, indicating improved phase purity and electronic homogeneity. Furthermore, this work introduces energy-selective ion control as a general, non-equilibrium route to stabilize metastable superconducting phases at low temperatures, offering a new design paradigm for thin-film quantum materials.
Low-Temperature Stabilization of δ-NbN Superconducting Thin Films through Energy-Selective Ion Beam Sputtering
Achieving high-quality superconducting thin films at low temperatures is a central challenge for scalable quantum device integration and Complementary Metal-Oxide-Semiconductor (CMOS)-compatible fabrication. Here, we demonstrate a room-temperature magnetron sputtering approach for synthesizing niobium nitride (NbN) thin films using a novel energy-selective ion source that enables independent control of ion energy and ion flux. This capability provides a powerful route to precisely tailor surface kinetics and crystallization pathways, overcoming longstanding limitations in stabilizing high-quality NbN at reduced temperatures. The resulting films were characterized by superconducting transport measurements, X-ray diffraction, X-ray photoelectron spectroscopy, and transmission electron microscopy. Compared with conventional reactive sputtering, ion beam-assisted growth yields a substantial narrowing of the transition width at the superconducting temperature, indicating improved phase purity and electronic homogeneity. Furthermore, this work introduces energy-selective ion control as a general, non-equilibrium route to stabilize metastable superconducting phases at low temperatures, offering a new design paradigm for thin-film quantum materials.
Superconducting thin-film microstructures are promising for generating local magnetic-field gradients for individual ion addressing in trapped-ion quantum processors while minimizing Joule heating at cryogenic temperatures. In this work, sputtered niobium (Nb) thin films on Si were patterned into coil and meander structures as candidate components for cryogenic 3D microsystem integration. The films were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Raman spectroscopy, and electrical resistance at cryogenic temperature. XRD confirms textured bcc Nb with a dominant Nb (110) reflection and an apparent out-of-plane coherence length of ~20 nm. SEM reveals a porous, needle-like nanograin morphology, while Raman spectroscopy indicates a disordered mixed niobium-oxide surface layer. Electrical measurements show clear superconducting transitions, with midpoint critical temperatures of about 7.5 K for the coil and 7.8 K for the meander, both below bulk Nb. The normal-state behavior is characterized by low residual-resistivity ratios (RRR), indicating significant disorder and grain-boundary scattering. Based on the measured Tc values and geometry-derived effective current densities (Jc), a phenomenological J-B-T critical-surface model was constructed to estimate the superconducting operating window under simultaneous temperature and magnetic-field loading. The results establish a process-structure-property correlation for sputtered Nb on Si and provide guidance for integrating superconducting thin-film coils into future trapped-ion cryogenic microsystems.
We report a milestone in achieving large-scale, ultrathin (~5 nm) superconducting NbN thin films on 300 mm Si wafers using a high-volume manufacturing (HVM) industrial physical vapor deposition (PVD) system. The NbN thin films possess remarkable structural uniformity and consistently high superconducting quality across the entire 300 mm Si wafer, by incorporating an AlN buffer layer. High-resolution X-ray diffraction and transmission electron microscopy analyses unveiled enhanced crystallinity of (111)-oriented δ-phase NbN with the AlN buffer layer. Notably, NbN films deposited on AlN-buffered Si substrates exhibited a significantly elevated superconducting critical temperature (~2 K higher for the 10 nm NbN) and a higher upper critical magnetic field or Hc2 (34.06 T boost in Hc2 for the 50 nm NbN) in comparison with those without AlN. These findings present a promising pathway for the integration of quantum-grade superconducting NbN films with the existing 300 mm CMOS Si platform for quantum information applications.
High energy gap Nb-based superconducting alloys with low normal state resistivity are fundamentally important for realization of low-loss high frequency circuits operating above the typical ~670 GHz gap frequency of elemental Nb. NbTiN has been shown to have a superconducting energy gap nearly twice that of elemental Nb, and is emerging as an important material for various detector and superconducting computing technologies. In this paper, we report on the growth of high-quality face-centered cubic (FCC) NbTiN films through the use of an alternative materials deposition technology-reactive bias target ion beam deposition. This novel technique offers more degrees of freedom compared to conventional sputtering, notably through decoupling the plasma generation and target bias, through use of a hollow-cathode ion source and independently pulse biased sputtering targets. The reported films are of high quality, with increased transition temperatures, reduced normal state resistivity, and surface roughness, compared to our previously reported reactive magnetron sputtered NbTiN films. In particular, at UVA, we are investigating these NbTiN films for wide-bandgap all-NbTiN superconducting-insulating-superconducting mixers, kinetic inductance detectors, and traveling-wave kinetic inductance parametric amplifier devices.
Nb-based superconducting alloys, such as NbN and NbTiN, can have a superconducting energy gap near twice that of elemental Nb, thus, being ideal candidates for low-loss superconducting circuits operating above the gap frequency of Nb. We are particularly interested in these materials for THz-frequency superconducting-insulating-superconducting (SIS) mixers, kinetic inductance detectors, and traveling wave kinetic inductance parametric amplifier devices. We recently reported the use of an alternative synthesis technique, reactive bias target ion beam deposition (RBTIBD), used to realize high-quality NbTiN films and high-energy gap NbTiN/AlN/NbTiN SIS heterostructures. In this paper, the effect of post-deposition annealing on the electrical and structural properties of room temperature deposited RBTIBD NbTiN was investigated. Our room temperature RBTIBD NbTiN films were annealed using rapid thermal annealing from 200 to 1000 °C. The change in structural and electrical properties was characterized by X-ray diffraction, atomic force microscopy, and four-point probe measurements. The annealed films demonstrated an enhancement in transition temperature (Tc), increased crystallinity, larger grain size, and significantly reduced intrinsic stress.
The rising interest in increased manufacturing maturity of quantum processing units is pushing the development of alternative superconducting materials for semiconductor fab process technology. However, these are often facing CMOS process incompatibility. In contrast to common CMOS materials, such as Al, TiN, and TaN, reports on the superconductivity of other suitable transition-metal nitrides are scarce, despite potential superiority. Here, we demonstrate fully CMOS-compatible fabrication of HfN and ZrN thin films on state-of-the-art 300 mm semiconductor process equipment, utilizing reactive DC magnetron sputtering on silicon wafers. Measurement of mechanical stress and surface roughness of the thin films demonstrates process compatibility. We investigated the materials phase and stoichiometry by structural analysis. The HfN and ZrN samples exhibit superconducting phase transitions with critical temperatures up to 5.84 and 7.32 K, critical fields of 1.73 and 6.40 T, and coherence lengths of 14 and 7 nm, respectively. A decrease in the critical temperature with decreasing film thickness indicates mesoscopic behavior due to geometric and grain-size limitations. The results promise a scalable application of HfN and ZrN in quantum computing and related fields.
The performance and coherence of superconducting quantum systems are fundamentally tied to the quality of the materials from which they are built. In superconducting transmon qubits, many loss mechanisms and sources of decoherence originate from material imperfections or unwanted oxide formation. Likewise, semiconductor–superconductor hybrid systems depend on high-quality interfaces to ensure strong coupling between electronic states in the two materials. In such hybrid devices, the accessible operating regime is often dictated by the intrinsic material properties of either the semiconductor or the superconductor. Advancing quantum device performance therefore requires exploring new material systems and optimizing their physical characteristics. In this thesis, we present the development of several superconducting material platforms for quantum technologies, including superconducting qubits, single-photon detectors, and semiconductor superconductor hybrid devices. We focus on the growth and characterization of superconducting films and heterostructures, and we establish clear connections between their material properties and the resulting device performance. First, we will present a novel semiconductor-superconductor hybrid material based on in-situ deposited epitaxial layers of Nb and Al on a shallow InAs quantum well. In this structure, the Al interlayer provides an epitaxial connection between an in-situ magnetron sputtered Nb or NbTi thin film and a shallow InAs two dimensional electron gas. This metal-to-metal epitaxy is achieved by optimization of the material stack and results in an induced superconducting gap of approximately 1 meV, determined from transport measurements of superconductor semiconductor Josephson junctions. This induced gap is approximately five times larger than the values reported for Al-based hybrid materials and indicates the formation of highly-transparent interfaces that are required in high-quality hybrid material platforms. Then, we discuss a different approach in the next chapter where we develop a hybrid material based on a molecular beam epitaxy grown InAsSb surface quantum well with an in-situ deposited Nb layer directly on top of the quantum well. Relative to conventional Al-InAs based systems, the InAsSb surface quantum well offers a lower effective mass and stronger spin-orbit interaction, while the Nb layer has a higher critical temperature and a larger critical magnetic field. The in-situ deposition of the Nb layer directly on top of the quantum well results in a high-quality interface that enables strong coupling to the InAsSb quantum well. Transport measurements on Josephson junctions reveal an induced superconducting gap of 1.3 meV and a critical current density of 3.75 × 10³A/cm². Furthermore, a planar asymmetric SQUID is realized, exhibiting gate-tunable superimposed oscillations originating from both the individual Josephson junction and the full SQUID loop. The large induced superconducting gap combined with strong spin-orbit interaction position this material as an attractive platform for experiments exploring gate-tunable superconductivity and topological superconducting devices. In the next chapter, we will focus on establishing a link between Nb film crystal properties and their performance in superconducting circuits. In this study, we investigate the microwave properties of niobium resonators with different crystalline properties and related surface topographies. We analyze a series of magnetron sputtered films in which the Nb crystal orientation and surface topography are changed by varying the substrate temperatures between room temperature and 975 K. The lowest-loss resonators that we measure have quality factors of over 10⁶ at single-photon powers, among the best ever recorded using the Nb on sapphire platform. We observe the highest quality factors in films grown at an intermediate temperature regime of the growth series (550 K) where the films display both preferential ordering of the crystal domains and low surface roughness. Furthermore, we analyze the temperature-dependent behavior of our resonators to learn about how the quasi-particle density in the Nb film is affected by the niobium crystal structure and the presence of grain boundaries. Then, we explore yet a different material platform by attempting to realize onchip NbTiN single photon detectors on LiNbO₃, an emerging photonic platform with high potential for scalable quantum information processing. We use DC reactive magnetron sputtering to grow high-quality NbTiN thin films and investigate the impact of substrate temperature during NbTiN growth. We achieve four nm thick superconducting films with a critical temperature (𝑇𝑐) of 12.3 K grown at a substrate temperature of 825 K. We demonstrate that the increased substrate temperature reduces the oxygen concentration in our films and improves the overall stoichiometry. In addition, we integrate these films with the LiNbO3 platform and investigate the obtained interface quality. Finally, we fabricate superconducting nanowire single photon detectors from the NbTiN film on LiNbO₃ and characterize the detector performance. Lastly, we report a gate-tunable Josephson diode effect in hybrid nanowire junctions consisting of a spin-orbit-coupled semiconductor core coated with epitaxial ferromagnetic insulator and superconductor shells. The wires display a hysteretic superconducting window as a function of axial magnetic field. In the superconducting regime, the devices exhibit nonreciprocal current transport, with the diode efficiency showing a strong dependence on back-gate voltage. The effect persists in a remanent magnetization state following a controlled demagnetization procedure, establishing zero-field operation. The combination of results presented in this thesis stress the importance of a material-focused approach in advancing the performance of quantum hardware. The novel hybrid material platforms developed in this thesis expand the operating regime of devices, which could enable future experiments involving gate-tunable superconductivity or topological properties. Similarly, we demonstrate that optimizing superconductor crystal structure benefits quantum devices, such as single-photon detectors and superconducting resonators.