Superconducting and structural properties of Nb films covered by plasma enhanced chemical vapor deposited a-Si:H layers for superconducting qubit application
Alessandro Bruno, P. Mengucci, Lucia Vittoria Mercaldo, Mikhail Lisitskiy
With a view to the fabrication of superconducting qubits with low decoherence time, we have investigated the influence of a-Si:H deposition by the plasma enhanced chemical vapor deposition method at 250◦C on the superconducting and structural properties of a 20 nm thick Nb film treated by two surface protection methods: plasma nitridation and deposition of a thin unhydrogenated Si layer. A suppression of theTc and an increase of the residual resistivity are observed due to hydrogen diffusion and decomposition of the native surface oxide, with subsequent oxygen diffusion caused by sample heating. The unhydrogenated Si layer is found to efficiently protect the Nb films against both diffusion processes.
With a view to the fabrication of superconducting qubits with low decoherence time, we have investigated the influence of a-Si:H deposition by the plasma enhanced chemical vapor deposition method at 250◦C on the superconducting and structural properties of a 20 nm thick Nb film treated by two surface protection methods: plasma nitridation and deposition of a thin unhydrogenated Si layer. A suppression of theTc and an increase of the residual resistivity are observed due to hydrogen diffusion and decomposition of the native surface oxide, with subsequent oxygen diffusion caused by sample heating. The unhydrogenated Si layer is found to efficiently protect the Nb films against both diffusion processes.
Hydrogenated amorphous silicon (a-Si:H) grown by PECVD has a lower loss tangent (tan _) among conventional dielectrics (such as SiO2 and SiNx) and hence is considered as the best amorphous dielectric material for superconducting qubit application. The incorporation of PECVD a-Si:H into the Nb technology requires attention due to the possible degradation of the superconductivity of the Nb films. Superconducting transition temperature (Tc) and residual resistivity (_0) of 20 nm, 50 nm and 100 nm thick Nb films were measured before and after a-Si:H deposition. The penetration of oxygen and hydrogen inside the Nb films was evaluated from the variation of the lattice parameter obtained by X-ray di_raction. The high process temperature (250_ C) and the presence of energetic hydrogen ions during the a-Si:H layer growth caused a decrease of Tc and increase of _0 through two physical processes: 1) oxygen di_usion from the surface Nb oxides and 2) hydrogen di_usion inside the Nb films. The degradation of Tc was reduced with the increase of the film thickness. Nitridation of Nb films and deposition of a sputtered thin amorphous silicon layer (a-Si) on the Nb films (in both cases made in situ after the Nb film deposition) were investigated a s surface treatments to protect the Nb filmsduring PECVD. It was demonstrated that both methods markedly reduce oxygen and hydrogen di_usion into Nb films during a-Si:H deposition, but the a-Si layer was more e_ective to protect the Nb films.
Amorphous hydrogenated silicon (a-Si:H) based lumped elements are one of the promising ways for large-scale integration of superconducting quantum devices. We present a detailed study devoted to the plasma-enhanced chemical vapor deposition process parameters' influence on the structure and morphology of a-Si:H dielectric thin films. We experimentally demonstrate a microcrystalline-to-amorphous growth transition by changing the H2/SiH4 ratio and establish a relationship between the film's structure, thickness, and dielectric loss tangent (tan δ). It is shown that the best dielectric loss tangents of tan δLP = 4.5 × 10−5 (average 9.2 × 10−5) and tan δHP = 1.0 × 10−6 (average 1.2 × 10−6) for superconducting lumped elements with 350 nm-thick amorphous films can be achieved in single- and multi-photon regimes at sub-20 mK, correspondingly. These values are extracted by characterizing superconducting resonators with integrated parallel-plate capacitors (C = 0.2…6.0 pF) for a frequency range from 4.0 to 7.0 GHz. The presented low-loss a-Si:H films can be useful for various superconducting quantum applications, which is illustrated by the fabrication of lumped-element bandpass filters with a well-predicted amplitude–frequency response characteristic.
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.
Similar to observations from other groups, we have observed degradation of the superconducting properties of Nb thin films that have been subjected to subsequent high temperature fabrication processes, such as curing of a passivating polyimide layer at 350°C. This degradation may be caused by interaction with material that diffuses into the Nb during the subsequent processes, and is the subject of ongoing research. To counteract these degradation effects, we have explored multiple materials as barrier layers to attempt to isolate and protect the Nb. The effectiveness of the barrier layer depends on the use of an appropriate layer stack that minimizes degradation in the superconducting thin film, is compatible with subsequent fabrication steps, and is stable and repeatable. We have investigated multiple material stack-ups to protect Nb-based superconducting thin film in flexible structures. We show that curing polymers above a certain temperature on top of a Nb layer can adversely affect the superconducting properties including critical transition temperature (Tc) and critical current (Ic). DC electrical characterization of patterned film test structures were carried out using a closed-cycle cryostat to determine Tc and Ic for the samples. Details of the fabrication processes, experimental procedures and performance results will be presented. Results of these experiments are expected to provide insight into possible materials stack-ups for packaging and interconnect structures for future cryogenic electronics systems.
Abstract Atomic layer deposition (ALD) has been identified as a promising growth method for high-uniformity superconducting thin films for superconducting quantum photonic applications, offering superior uniformity, thickness control and conformality to techniques such as reactive sputtering. The potential scalability of ALD makes this method especially appealing for fabrication of superconducting nanowires and resonators across large areas. We report on the growth of highly uniform superconducting NbN thin films via plasma-enhanced atomic layer deposition (PEALD) with radio frequency substrate biasing, on a 200 mm (8 inch) Si wafer, specifically for superconducting nanowire single-photon detector applications. Niobium nitride films were grown using (tert-butylimido)-tris(diethylamido)-niobium(V) precursor and an H 2 /Ar plasma. The superconducting properties of a variable thickness series of films (5.9–29.8 nm) show critical temperature ( T c ) of 13.5 K approaching bulk thickness (28.8 nm) with low suppression down to the ultrathin regime (5.9 nm), with T c = 10.2 K. T c across the 200 mm wafer with 8 nm thick NbN, measured in 15 mm intervals, exhibits minimal variation (<7%). Microbridge structures fabricated on 8 nm thick NbN films also exhibit high critical current densities ( J c ), > 10 MA cm −2 at 2.6 K. PEALD could therefore be a pivotal technique in enabling large-scale fabrication of integrated quantum photonic devices across a variety of applications.
Low-loss deposited dielectrics will benefit superconducting devices such as integrated superconducting spectrometers, superconducting qubits, and kinetic inductance parametric amplifiers. Compared with planar structures, multilayer structures such as microstrips are more compact and eliminate radiation loss at high frequencies. Multilayer structures are most easily fabricated with deposited dielectrics, which typically exhibit higher dielectric loss than crystalline dielectrics. We measure the subkelvin and low-power microwave and millimeter-submillimeter-wave dielectric loss of hydrogenated amorphous silicon carbide (a-SiC:H), using superconducting chips with Nb-Ti-N/a-SiC:H/Nb-Ti-N microstrip resonators. We deposit the a-SiC:H by plasma-enhanced chemical vapor deposition at a substrate temperature of $400{\phantom{\rule{0.1em}{0ex}}}^{\ensuremath{\circ}}\mathrm{C}$. The a-SiC:H has a millimeter-submillimeter loss tangent ranging from $0.9\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}4}$ at 270 GHz to $1.5\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}4}$ at 385 GHz. The microwave loss tangent is $3.1\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}5}$. These are the lowest low-power subkelvin loss tangents that have been reported for microstrip resonators at millimeter-submillimeter and microwave frequencies. The a-SiC:H films are free of blisters and have low stress: $\ensuremath{-}20$ MPa compressive at 200-nm thickness to 60 MPa tensile at 1000-nm thickness.