Tantalum Films Research Articles

Comparative S/TEM study of superconducting Ta quantum resonators by wet and dry etching types

Superconducting resonators play a pivotal role in various quantum technology applications, such as quantum computing and high-frequency communication systems. The performance of these resonators is closely tied to the properties of the superconducting films used in their fabrication. In this study, we investigated the impact of wet and dry etching on tantalum (Ta) films leveraging advanced scanning transmission electron microscopy-based characterization methods and examined the morphological, chemical, and strain changes caused by the etching processes. Consequently, we report the significant differences between the two etching methods, with dry etching resulting in straight slanted sidewalls and a thinner oxidized layer, while wet etching produced curved sidewalls and undercuts. Both methods led to the formation of a residual Ta wedge at the lower part of the sidewall, causing lattice deformation, which could adversely influence the homogeneous operations of superconducting devices. These insights enhance our understanding of how etching influences superconducting films, offering valuable guidance for optimizing resonators and related devices. Our findings mark a significant stride in advancing quantum technologies and high-frequency communication by enhancing our practical understanding of superconducting material fabrication.

Metal hydride hydrogen sensing materials from 28 °C to 270 °C

Metal hydrides have been widely studied as hydrogen sensing materials and applied to various optical sensor configurations. With the increasing interest in using hydrogen as an energy source across sectors involving combustion processes, there is a growing demand for reliable hydrogen sensors operating at temperatures above 100 °C. Therefore, it is necessary to evaluate the performance of potential hydrogen sensing materials at elevated temperatures. We conducted experiments to observe the optical response and structural characteristics of palladium, palladium–gold, tantalum, and tantalum-alloy thin films with respect to varying hydrogen concentrations from 28 °C to 270 °C. Our results demonstrate that the optical response of palladium and palladium–gold diminish at 270 °C. However, tantalum provides a remarkable optical response to hydrogen concentrations below 1% for all the observed temperatures and a stable response at 270 °C for 350 cycles. Our measurement results show that tantalum is the most suitable material for detecting hydrogen within the range of 0.01% to 100% at temperatures ranging from 28 °C to 270 °C.

Electrolytic Micro‐Capacitors Based on Tantalum Films for High Voltage Applications

AbstractElectrolytic capacitors are known to be fast devices with very low time constant and able to deliver high power. This class of capacitors is then an interesting technology to power miniaturized embedded electronics for Internet of Things applications. However, the current electrolytic capacitor suffers from its bulky size that does not fit with the miniaturization. To solve this issue, a proof‐of‐concept consisting of miniaturizing an electrolytic capacitor based on tantalum materials to give rise to a new class of electrolytic micro‐capacitors is proposed. To reach this ambitious objective, thin films (<100 nm) of tantalum metal (Ta), tantalum nitride (TaN), and tantalum oxide (Ta2O5) are deposited on a Si substrate by sputtering deposition method. After a careful optimization of the deposition parameters, Ta/Ta2O5 and TaN/Ta2O5 electrodes (Ta and TaN ≈45 nm and Ta2O5 ≈25 nm) and study their behaviors when biased at high voltage (>20 Volts) in aqueous electrolyte are produced. The Ta/Ta2O5 and TaN/Ta2O5 interfaces when the electrode is polarized near and beyond the breakdown voltage of the dielectric layer are carefully investigated. Polarizing the electrodes beyond the breakdown voltage are shown to result in anodization‐like mechanisms. In the case of the TaN/Ta2O5 electrode, an N‐rich porous layer grew within the Ta2O5 layer as polarization increased. A comparative study on the 2 stacked layers electrodes with different compositions (Ta/Ta2O5 and TaN/Ta2O5) but similar thicknesses (45/25 nm) is carried out: both electrodes show excellent capacitance retention of over 90% over 300 000 cycles. The frequency behavior of Ta/Ta2O5 and TaN/Ta2O5 electrodes shows that both are potential candidates in electrolytic micro‐capacitors for powering miniaturized electronics.

Molecular Layering of an Additive Layer of Silicon Dioxide on Anodized Tantalum and Niobium Oxides

The results of studying the processes of formation of nanolayers of silicon oxide by the method of molecular layering (atomic layer deposition) on the surface of films of tantalum and niobium oxides obtained by electrochemical oxidation of the corresponding metals are presented. A study of the electrical strength of metal-dielectric-metal (MDM) structures based on tantalum and niobium oxides showed that the introduction of an additive dielectric layer (SiO2) can significantly increase the electrical strength of these structures.

Microwave characterization of tantalum superconducting resonators on silicon substrate with niobium buffer layer

Tantalum thin films sputtered on unheated silicon substrates are characterized with microwaves at around 10 GHz in a 10 mK environment. We show that the phase of tantalum with a body-centered cubic lattice (α-Ta) can be grown selectively by depositing a niobium buffer layer prior to a tantalum film. The physical properties of the films, such as superconducting transition temperature and crystallinity, change markedly with the addition of the buffer layer. Coplanar waveguide resonators based on the composite film exhibit significantly enhanced internal quality factors compared with a film without the buffer layer. The internal quality factor approaches 2 × 107 at a large-photon-number limit. While the quality factor decreases at the single-photon level owing to two-level system (TLS) loss, we have deduced that one of the causes of TLS loss is the amorphous silicon layer at the film–substrate interface, which originates from the substrate cleaning before the film deposition rather than the film itself. The temperature dependence of the internal quality factors shows a marked rise below 200 mK, suggesting the presence of TLS–TLS interactions. The present low-loss tantalum films can be deposited without substrate heating and thus have various potential applications in superconducting quantum electronics.

Enhanced Electrical and Optical Properties of Bismuth Tantalum Oxide Thin Films through Graphene Oxide Doping.

In this study, a hybrid thin film was fabricated by doping graphene oxide in a bismuth tantalum oxide solution in the sol-gel state. The thin film was produced by a brush-coating process. The graphene oxide doping ratios used were 0, 5, and 15 wt %. In the process of producing the thin film, the prepared sol-gel solution generates contraction forces, owing to the shear stress from the bristles of the brush, forming a microgroove structure. This structure was confirmed through atomic force microscopy, transmission electron microscopy, and energy-dispersive spectroscopy analyses. As a result of line profile analysis in atomic force microscopy, the groove heights of the thin film surface at 0, 5, and 15 wt % doping were 110, 130, and 160 nm, respectively, and the width of all grooves was 1 μm. The width of all thin films was approximately 1 μm, and microgrooves were confirmed. Moreover, the hybrid thin-film formation was confirmed by X-ray photoelectron spectroscopy. By comparing the electrical properties of the bismuth tantalum oxide thin film without graphene oxide doping and the thin film doped with 15 wt % graphene oxide, it was demonstrated that the electro-optical properties increased excellently with graphene oxide doping. Typically, the threshold voltage was reduced by approximately 0.26 V. Based on these observations, graphene oxide doped bismuth tantalum oxide hybrid thin films can be considered as promising candidates for thin-film applications in next-generation displays.

Plasma‐Enhanced Atomic Layer Deposition of Amorphous Tantalum Thin Films for Copper Interconnects Using an Organometallic Precursor

AbstractAs integrated circuits continue to shrink in size, the demand for high‐quality adhesive layers in copper Damascene interconnects has increased. However, tantalum (Ta) films, used as liners, prepared by atomic layer deposition (ALD) from metal halide precursors, are prone to corrosion and exhibit issues such as low film density and unstable performance. In this study, Ta films are successfully fabricated using a plasma‐enhanced ALD (PEALD) process with an organometallic precursor of Ta(NtBu)(NEt2)3 (TBTDET). The study of the growth conditions reveals that introducing 10% Ar in Ar‐H2 mixed gas leads to continuous high‐quality Ta films. The deposited Ta films are free of halogen impurities, which can avoid the detrimental impact on the stability of the Cu interconnects. Although the films contain some carbon and nitrogen impurities, they do not affect the film adhesive properties. Transmission electron microscopy shows that the Ta films are amorphous, and the amorphous Ta films exhibit superior barrier properties. Moreover, highly uniform Ta films can be conformally deposited into narrow interconnect structures using this PEALD process. These findings suggest that the Ta films prepared by the organometallic precursor can offer a promising solution to address the issues related to the halogen elements in the adhesive layer preparation.

Magnetic ac susceptibility of superconducting Ta films for quantum computing

Recently, breakthroughs were reported in the long coherence time (>0.5 ms) transmon qubit using tantalum films (Ta). Identifying the loss mechanism in Ta films will help further improve the performance of Ta-based superconducting qubits. Here, we report a study of superconducting properties in two sets of Ta films grown on c-cut and a-cut sapphires respectively using contact transport and noncontact magnetic ac susceptibility measurements. Although the resistive transition appears to be similar in both films, we found strikingly different responses in their complex magnetic susceptibilities . in the c-cut films exhibits a sharp peak at superconducting transition T c and becomes featureless below T c indicating a strongly coupled superconducting state. In contrast, in the a-cut films exhibits a broad peak near T c and a second peak appears below T c, indicating granular superconductivity behavior. This second peak in is associated with the hysteresis loss at weak-link-type grain boundaries, which is believed to be a leading source of decoherence in the a-cut Ta films. The derived magnetic loss tangent in the a-cut films is about one order of magnitude higher than in the c-cut films. This study demonstrates that ac susceptibility is an excellent probe for characterizing bulk superconducting properties of the constituent superconducting materials used in qubits.

Effect of an oxide layer on high velocity impact of tantalum particles characterized using molecular dynamics

Micro-cold spray, also commonly referred to as the aerosol deposition method or vacuum kinetic spraying, is a process for depositing nanostructured films of metals and ceramics by impacting solid nanoparticles at high velocity onto a substrate at room temperature and at low pressures. Tantalum films deposited by micro-cold spray are desirable because tantalum is non-reactive to certain molten metals and can therefore serve as a non-reactive barrier coating. However, unlike most other metals deposited by micro-cold spray, tantalum quickly forms an oxide layer when exposed to air. In the deposition of films using traditional cold spray with much larger particles, native oxides must fracture for particle–substrate bonding to occur. The fraction of the particle that is oxidized in micro-cold spray and the strain rates experienced by the particles upon impact are both much larger than in cold spray, suggesting that the role of the oxide on film deposition may be distinct. The effect of this oxide layer on particle deformation and adherence to a substrate under high strain rates is studied using molecular dynamics simulations. The effect of oxide layer thickness, particle diameter, and impact velocity are examined.

Shock state distributions in porous tantalum and characterization with multipoint velocimetry

Heterogenous materials under shock compression can be expected to reach different shock states throughout the material according to local differences in microstructure and the history of wave propagation. Here, a compact, multiple-beam focusing optic assembly is used with high-speed velocimetry to interrogate the shock response of porous tantalum films prepared through thermal-spray deposition. The distribution of particle velocities across a shocked interface is compared to results obtained using a set of defocused interferometric beams that sampled the shock response over larger areas. The two methods produced velocity distributions along the shock plateau with the same mean, while a larger variance was measured with narrower beams. The finding was replicated using three-dimensional, mesoscopically resolved hydrodynamics simulations of solid tantalum with a pore structure mimicking statistical attributes of the material and accounting for radial divergence of the beams, with agreement across several impact velocities. Accounting for pore morphology in the simulations was found to be necessary for replicating the rise time of the shock plateau. The validated simulations were then used to show that while the average velocity along the shock plateau could be determined accurately with only a few interferometric beams, accurately determining the width of the velocity distribution, which here was approximately Gaussian, required a beam dimension much smaller than the spatial correlation lengthscale of the velocity field, here by a factor of ∼30×, with implications for the study of other porous materials.

STEM Study on the Native Amorphous Surface Axides of Tantalum Film for a Superconducting Qubit.

STEM Study on the Native Amorphous Surface Axides of Tantalum Film for a Superconducting Qubit.

Efficient ultrafast photoacoustic transduction on Tantalum thin films

Nano-acoustic strain generation in thin metallic films via ultrafast laser excitation is widely used in material science, imaging and medical applications. Recently, it was shown that transition metals, such as titanium, exhibit enhanced photoacoustic transduction properties compared to noble metals, such as silver. This work presents experimental results and simulations that demonstrate that among transition metals tantalum exhibits superior photoacoustic properties. Experiments of nano-acoustic strain generation by femtosecond laser pulses focused on thin tantalum films deposited on Silicon substrates are presented. The nano-acoustic strains are measured via pump-probe transient reflectivity that captures the Brillouin oscillations produced by photon–phonon interactions. The observed Brillouin oscillations are correlated to the photoacoustic transduction efficiency of the tantalum thin film and compared to the performance of titanium thin films, clearly demonstrating the superior photoacoustic transduction efficiency of tantalum. The findings are supported by computational results on the laser-induced strains and their propagation in these thin metal film/substrate systems using a two-temperature model in combination with thermo-mechanical finite element analysis. Finally, the role of the metal transducer-substrate acoustic impedance matching is discussed and the possibility to generate appropriately modulated acoustic pulse trains inside the crystalline substrate structures for the development of crystalline undulators used for γ-ray generation is presented.

Effect of tantalum and Ni[sbnd]Ta barriers on inter-diffusion between nickel coating and GH3535 alloy at 700 °C

Nickel-coated GH3535 alloy is suitable used for molten salt reactor at elevated temperature. However, coating failure caused by inter-diffusion is still problematic. In this study, tantalum and NiTa films were deposited as barriers between nickel coating and GH3535 alloy by magnetron sputtering, respectively. The diffusion behaviors of the coatings were investigated by micro-structure analysis and calculation of diffusion coefficient. The results indicate that a Ta barrier can inhibit the diffusion of Cr and Fe due to the formation of Ni3Ta phases, but Ni diffusion from the substrate to the barrier is promoted causing the formation of Kirkendall voids. However, a novel NiTa barrier exhibits excellent diffusion resistance for Cr, Fe, and Ni in the Ni/GH3535 system at 700 °C.

Near-Field Localization of the Boson Peak on Tantalum Films for Superconducting Quantum Devices.

Superconducting circuits are among the most advanced quantum computing technologies; however, their performance is limited by losses found in surface oxides and disordered materials. In this work, we demonstrate the identification and spatial localization of a near-field signature of loss centers on tantalum films using terahertz scattering-type scanning near-field optical microscopy. By utilizing terahertz nanospectroscopy, we observe a localized excess vibrational mode around 0.5 THz and identify this resonance as the boson peak, a signature of amorphous materials. Grazing-incidence wide-angle X-ray scattering reveals that oxides on freshly solvent-cleaned samples are amorphous, whereas crystalline phases emerge after aging in air. Through nanoscale localization of defect centers, our findings provide valuable insights for the optimization of fabrication procedures for new low-loss superconducting circuits.

Chemical Profiles of the Oxides on Tantalum in State of the Art Superconducting Circuits.

Over the past decades, superconducting qubits have emerged as one of the leading hardware platforms for realizing a quantum processor. Consequently, researchers have made significant effort to understand the loss channels that limit the coherence times of superconducting qubits. A major source of loss has been attributed to two level systems that are present at the material interfaces. It is recently shown that replacing the metal in the capacitor of a transmon with tantalum yields record relaxation and coherence times for superconducting qubits, motivating a detailed study of the tantalum surface. In this work, the chemical profile of the surface of tantalum films grown on c-plane sapphire using variable energy X-ray photoelectron spectroscopy (VEXPS) is studied. The different oxidation states of tantalum that are present in the native oxide resulting from exposure to air are identified, and their distribution through the depth of the film is measured. Furthermore, it is shown how the volume and depth distribution of these tantalum oxidation states can be altered by various chemical treatments. Correlating these measurements with detailed measurements of quantum devices may elucidate the underlying microscopic sources of loss.

A-phase tantalum film deposition using bipolar high-power impulse magnetron sputtering technique

In this study, a method for forming a highly adhesive and ductile α-phase tantalum film on 304 stainless steel using the bipolar high-power impulse magnetron sputtering (bipolar HiPIMS) technique was investigated. The growth of brittle β-phase tantalum, which is commonly formed when using conventional direct current magnetron sputtering methods (DCMS) at room temperature, was prevented by the high-energy ions directed toward the growing films. The results showed the formation of an extremely thin (<70 nm) α-phase tantalum film without any additional processes, such as substrate biasing or heating. In addition, a high adhesion strength exceeding 45 MPa, broadened intermixed layer, and nanocrystalline microstructure were achieved by the effect of positive voltage. These results indicate that the bipolar HiPIMS technique is a facile deposition method for modifying the substrate surface and forming high-quality crystalline films. Our tantalum films are optimized to protect substrates against corrosion in severely harsh mechanical, chemical, and thermal environments. To confirm the superiority of the bipolar HiPIMS technique over HiPIMS and DCMS, the properties of the films formed using the three methods were analyzed via X-ray diffraction, Auger electron spectroscopy, atomic force microscopy, scanning electron microscopy, and pull-off adhesion testing.

Synergetic effect of thickness and oxygen addition on the electrochemical behaviour of tantalum oxide coatings deposited by HiPIMS in DOMS mode

The HiPIMS technique in DOMS mode was used to deposit tantalum (Ta) and Ta1-xOx films. After depositing pure metallic Ta and Ta1-xOx films with two different thicknesses, their structure, morphology and chemical composition were investigated. Nano-indentation was used to evaluate the hardness of the films. OCP, potentiodynamic and EIS in artificial saliva at T = 37 °C were used to investigate the corrosion behaviour of the coatings. The results showed that, in the case of metallic coatings, increasing the film thickness, the β-phase becomes dominant over the α-phase, which compromised both the mechanical and electrochemical behaviours. Tantalum oxide films raised the polarisation resistance of the non-reactive coatings (metallic ones), exhibiting values 2–3 orders of magnitude higher.

On the chemistry, photocatalytical, and corrosion behavior of co-sputtered tantalum and titanium oxynitride thin films

Direct current magnetron co-sputtered titanium and tantalum based oxynitride coatings (TaTiON) were analyzed in terms of their chemistry, surface morphology, surface energy, photocatalytic activity, and corrosion resistance. The variable parameter for the deposition was the applied current on each target, changing between 0.75A and 0.25A for the Ta target, and from 0.25A to 0.75 A for the Ti target, to obtain a total current of 1A. Reference single-sputtered samples (TaON and TiON) were deposited under identical conditions. It was observed that a higher degree of oxidation occurred in the samples deposited with higher current on the Ti target, while nitriding and oxynitriding processes occurred only on the surfaces of the films containing Ta. In terms of surface roughness, the co-sputtered coatings exhibited significantly smaller values, compared to the single-sputtered coatings. The highest photodegradation efficiency was registered for the co-sputtered sample which contains the highest N concentration. The corrosion rate, obtained from electrochemical tests, varies in a rather large domain, as function of the chemical species in the coatings.

Reactive ion etching of tantalum in silicon tetrachloride

A precise patterning of metal structures plays an essential role in the development of feasible metal-based devices. By examining the etching conditions under which a layer of material is properly etched, the etching process can be further optimised and hence controlled. This work reports on the reactive ion etching (RIE) of micrometric films of tantalum (Ta) using silicon tetrachloride (SiCl4)/Argon (Ar) plasmas. The etching characteristics have been studied with respect to SiCl4/Ar ratio, plasma power and chamber pressure. It has been found that increasing the flow rate of SiCl4 or plasma power leads to an increase in the etching rate. Moreover, the observations suggest that it is ineffective to increase the flow rate of Ar to more than 30 sccm and the plasma pressure to more than 100 mTorr. The work implemented here represents an important step for the development of tantalum-based structures that can be used in a wide range of devices.

A study of the phase transformation of low temperature deposited tantalum thin films using high power impulse magnetron sputtering and pulsed DC magnetron sputtering

In this study, tantalum thin films were deposited on silicon substrates using high power impulse magnetron sputtering (HiPIMS) and pulsed DC magnetron sputtering (pulsed DC), investigating the texture transformation behavior of α-Ta and β-Ta tantalum films by changing the duty cycle of tantalum targets from 5% to 88% at the power of 150 W and 50 W. The surface, microstructure, and texture of sputtered tantalum films were measured by scanning electron microscopy (SEM), atomic force microscope (AFM) and X-ray diffraction spectroscopy (XRD). The hardness and resistivity were measured by nanoindentation and a four-point probe. The results reveal that the impulse power and voltage of the Ta target were increased because of the lower duty cycle. The higher the ion energy, resulting in a more efficient atomic mobility, the texture phase of tantalum film gradually changes from β-Ta-dominated to α-Ta-dominated, hardness and resistivity shift from β-Ta to the α-Ta property with the decreasing duty cycle. By adjusting the duty cycle and controlling the power, the texture transformation of tantalum film occurs. Different from the previously complicated transformation process, the tantalum thin film structure with high density and high quality deposited using this approach provides a broader range of applications.