Chemical profiles of the oxides on tantalum in state of the art superconducting circuits
Russell A. McLellan, Aveek Dutta, Chenyu Zhou, Yichen Jia, Conan Weiland, Xin Gui, Alexander P. M. Place, Kevin D. Crowley, Xuan Hoang Le, Trisha Madhavan, Youq… 展开作者
Russell A. McLellan, Aveek Dutta, Chenyu Zhou, Yichen Jia, Conan Weiland, Xin Gui, Alexander P. M. Place, Kevin D. Crowley, Xuan Hoang Le, Trisha Madhavan, Youqi Gang, Lukas Baker, Ashley R. Head, Iradwikanari Waluyo, Ruoshui Li, Kim Kisslinger, Adrian Hunt, Ignace Jarrige, Stephen A. Lyon, Andi M. Barbour, Robert J. Cava, Andrew A. Houck, Steven L. Hulbert, Mingzhao Liu, Andrew L. Walter, Nathalie P. de Leon
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. We recently showed 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, we study the chemical profile of the surface of tantalum films grown on c-plane sapphire using variable energy X-ray photoelectron spectroscopy (VEXPS). We identify the different oxidation states of tantalum that are present in the native oxide resulting from exposure to air, and we measure their distribution through the depth of the film. Furthermore, we show how the volume and depth distribution of these tantalum oxidation states can be altered by various chemical treatments. By correlating these measurements with detailed measurements of quantum devices, we can improve our understanding of the microscopic device losses.
Complementary resistive switches (CRS) are considered as a potential solution for the sneak path problem in large-scale integration of passive crossbar resistive memory arrays. A typical CRS is composed of two bipolar memory cells that are connected anti-serially. Here we report a tantalum-oxide based resistive memory that achieves the complementary switching functionality within a single memory cell. The complementary switching effect is accompanied by switching polarity reversal in different voltage bias regimes. These effects were explained by the redistribution of oxygen vacancies inside t…
Tantalum Damascene Coplanar Waveguide Resonators Fabricated Using 300 mm Scale Processes
NY Creates（纽约创造）；Pacific Northwest National Laboratory（太平洋西北国家实验室）；University of California, Santa Barbara（加州大学圣塔芭芭拉分校）；Brookhaven National Laboratory（布鲁克海文国家实验室）
Oxygen migration in tantalum oxide, a promising next-generation storage material, is studied using in-operando x-ray absorption spectromicroscopy and is used to microphysically describe accelerated evolution of conduction channel and device failure. The resulting ring-like patterns of oxygen concentration are modeled using thermophoretic forces and Fick diffusion, establishing the critical role of temperature-activated oxygen migration that has been under question lately.
Fabrication and Structural Analysis of Trilayers for Tantalum Josephson Junctions with Ta$_2$O$_5$ Barriers
University of Washington（华盛顿大学）；Colorado School of Mines（科罗拉多矿业学院）；National Laboratory of the Rockies（落基山国家实验室）；Pacific Northwest National Laboratory（太平洋西北国家实验室）；Rigetti Computing, Inc.（里盖蒂计算公司）
Enhanced Tantalum Superconducting Resonator Performance via All-Surface Organic Monolayer Passivation
Technical University of Munich（慕尼黑工业大学）；Indian Institute of Technology Roorkee（罗克基印度理工学院）；Fraunhofer Institute for Electronic Microsystems and Solid State Technologies (EMFT)（弗劳恩霍夫电子微系统和固态技术研究所）
Memristors are receiving keen interest because of their potential varied applications and promising large-scale information storage capabilities. Tantalum oxide is a memristive material that has shown promise for high-performance nonvolatile computer memory. The microphysics has been elusive because of the small scale and subtle physical changes that accompany conductance switching. In this study, we probed the atomic composition, local chemistry and electronic structure of functioning tantalum oxide memristors through spatially mapped O K-edge x-ray absorption. We developed a time-multiplexed…
We investigated the impact of surface oxygen on the ion yield for He$^+$ ions scattered from different single crystalline surfaces in low-energy ion scattering. Initially clean Al(111) and Ta(111) were exposed to molecular oxygen and ion spectra for different oxidation stages and different primary energies were recorded. A comparison of ion yields normalized to the differential scattering cross section as well as experimental factors allows obtaining information about the influence of oxygen on charge exchange processes. The decrease in the ion yield of both metals with exposure cannot be expl…
A thorough investigation of the dielectric properties of Cu2Ta4O12, a material crystallizing in a pseudo-cubic, perovskite-derived structure is presented. We measured the dielectric constant and conductivity of single crystals in an exceptionally broad frequency range up to GHz frequencies and at temperatures from 25 - 500 K. The detected dielectric constant is unusually high (reaching values up to 105) and almost constant in a broad frequency and temperature range. Cu2Ta4O12 possesses a crystal structure similar to CaCu3Ti4O12, the compound for which such an unusually high dielectric constant…
The argon content of titanium dioxide doped tantalum pentoxide thin films was quantified in a spatially resolved way using HAADF images and DualEELS. Films annealed at 300$^{\circ}$C, 400$^{\circ}$C and 600$^{\circ}$C were investigated to see if there was a relationship between annealing temperature and bubble formation. It was shown using HAADF imaging that argon is present in most of these films and that bubbles of argon start to form after annealing at 400$^{\circ}$C and coarsen after annealing at 600$^{\circ}$C. A semi-empirical standard was created for the quantification using argon data …
We report the successful fabrication of superconducting tantalum nitride (TaN) thin films using a pulsed laser deposition technique with 1064 nm radiation. Films with thickness $ \sim $ 100 nm deposited on MgO (100) single crystals and on oxidized silicon (SiO$_{2} $) substrates exhibited a superconducting transition temperature of $\sim $ 8 K and 6 K, respectively. The topography of these films were investigated using atomic force and scanning electron microscopy, revealing fairly large area particulate free and smooth surfaces, while the structure of the films were investigated using standar…
In situ Al$_2$O$_3$ passivation of epitaxial tantalum and aluminum films enables long-term stability in superconducting microwave resonators
Grad. Institute of Applied Physics and Dept. of Physics, National Taiwan University（国立台湾大学应用物理研究所及物理系）；Department of Physics, National Tsing Hua University（国立清华大学物理系）；National Synchrotron Radiation Research Center（国家同步辐射研究中心）；Taiwan Semiconductor Research Institute（台湾半导体研究院）
Tantalum, tantalum oxide and their hetero-interfaces are of tremendous technological interest in several applications spanning electronics, thermal management, catalysis and biochemistry. For example, local oxygen stoichiometry variation in TaOx memristors comprising of metallic (Ta) and insulating oxide (Ta2O5) have been shown to result in fast switching on the sub-nanosecond timescale over a billion cycles, relevant to neuromorphic computation. Despite its broad importance, an atomistic scale understanding of oxygen stoichiometry variation across Ta/TaOx hetero-interfaces, such as during ear…
Germanium thin films are an excellent candidate for use as a low-loss dielectric in superconducting microwave resonators, a low-loss inter-layer metal wiring dielectric, and passivation layers in microwave and Josephson junction devices. In Ge/Nb structures deposited at 400 °C, we observe intermixing over as much as 20 nm. The addition of a 10 nm Ta diffusion barrier layer reduces the superconductor/dielectric intermixing to less than 5 nm and enhances the structural properties of deposited a-Ge layers based on Raman spectroscopy. Additionally, superconducting microwave resonators fabricated a…
As a compound in between the tantalum oxide and nitride, the tantalum oxynitride TaON is expected to combine their advantages and act as an efficient visible-light-driven photocatalyst. In this letter, using hybrid functional calculations we show that TaON has different defect properties from the binary tantalum oxide and nitride: (i) instead of O or N vacancies or Ta interstitials, the $O_N$ antisite is the dominant defect, which determines its intrinsic n-type conductivity and the p-type doping difficulty; (ii) the $O_N$ antisite has a shallower donor level than O or N vacancies, with a delo…
The systems Nb$_2$O$_5$-Ta$_2$O$_5$ and Nb$_2$O$_5$-V$_2$O$_5$ were investigated using thermal analysis, X-ray powder diffraction and thermodynamic simulations. Solid solution formation is possible for both systems; furthermore, both contain one intermediate compound, VNb$_9$O$_{25}$ or Ta$_2$Nb$_4$O$_{15}$, respectively. Phase relationships for pure niobium(V)-oxide and tantalum(V)-oxide were studied under ambient pressure. It was found that both compounds can occur in two stable solid modifications. For niobium(V)-oxide this are the monoclinic high-temperature modification (H-Nb$_2$O$_5$) an…
Recently the oxygen-reconstructed tantalum surface Ta(001)-p(3$\times$3)-O has experienced considerable attention due its use as a potential platform for Majorana physics in adatom chains. Experimental studies using scanning tunneling microscopy and spectroscopy found rich atomic and electronic structures already for the clean Ta(001)-O surface, which we combine here with $ab~initio$ methods. We discover two metastable superstructures at the root of the different topographic patterns, discuss its emergence during annealing, and identify the electronic properties. The latter is determined as th…
Quasiparticle spectroscopy in tantalum films with different Ta/sapphire interfaces
Ames National Laboratory（艾姆斯国家实验室）；Iowa State University（爱荷华州立大学）；National Institute of Standards and Technology（国家标准与技术研究院）；University of Virginia（弗吉尼亚大学）
The crystal structure of solid-state materials with unique lattices is considered one of the main factors determining physical properties, including superconductivity. Materials with honeycomb lattices have inspired intense research interest for their novel properties. A previously unknown compound, Ta4CoSi, are discussed herein and its crystal structure and superconducting properties. It crystallizes in a CuAl2-type structure (space group P4/mcm, No. 124) with the lattice parameters a = b = 6.17755(7)Å and c = 4.98443(8) Å, featuring honeycomb networks of Ta-Ta in (110) plane. Superconductivi…
Absence of Charge Offset Drift in a Transmon Qubit
Ecole Normale Supérieure de Lyon, CNRS, Laboratoire de Physique（里昂高等师范学院，法国国家科学研究中心，物理实验室）；Departamento de Física, Facultad de Ciencias Físicas y Matemáticas, Universidad de Chile（智利大学理学院物理与数学系）；Institut Quantique and Département de Physique, Université de Sherbrooke（舍布鲁克大学量子研究所及物理系）
Tantalum oxides (Ta$_2$O$_5$) are characterised by attractive physical and chemical properties, such as high dielectric constants and anti-reflection behaviour. Recently, Ta$_2$O$_5$ nanoparticles have also been proposed as possible enhancers of the relative biological effectiveness in hadrontherapy for cancer treatment. In principle, their electronic properties can be accurately investigated from first-principles simulations. However, the existence of several stable polymorphs of these oxides represents a major difficulty in order to calculate and disentangle their respective spectral feature…
Substrate material imperfections and surface losses are one of the major factors limiting superconducting quantum circuitry from reaching the scale and complexity required to build a practicable quantum computer. One potential path towards higher coherence of superconducting quantum devices is to explore new substrate materials with a reduced density of imperfections due to inherently different surface chemistries. Here, we examine two ternary metal oxide materials, spinel (MgAl2O4) and lanthanum aluminate (LaAlO3), with a focus on surface and interface characterization and preparation. Device…
Reconfigurable Superconducting Quantum Circuits Enabled by Micro-Scale Liquid-Metal Interconnects
Quantum Science Center of Guangdong-Hong Kong-Macao Greater Bay Area（粤港澳大湾区量子科学中心）；Division of Materials Science and Engineering, Boston University（波士顿大学材料科学与工程系）；Department of Electrical and Computer Engineering, Boston University（波士顿大学电气与计算机工程系）；Department of Physics, Boston University（波士顿大学物理系）；IBM Quantum, IBM T.J. Watson Research Center（IBM量子，IBM托马斯·J·沃森研究中心）；Department of Chemistry, Boston University（波士顿大学化学系）；Department of Mechanical Engineering, Boston University（波士顿大学机械工程系）；Department of Biomedical Engineering, Boston University（波士顿大学生物医学工程系）
Decoherence in superconducting qubits has long been attributed to two level systems arising from the surfaces and interfaces present in real devices. A recent significant step in reducing decoherence was the replacement of superconducting niobium by superconducting tantalum, resulting in a tripling of transmon qubit lifetimes (T1). One of these surface variables, the identity, thickness, and quality of the native surface oxide, is thought to play a major role as tantalum only has one oxide whereas niobium has several. Here we report the development of a thermodynamic metric to rank materials b…
The two-loop temperature hysteresis of integrated intensity of Raman scattering of light is explained theoretically for a line of frequency 50 cm-1 in a superconducting oxide Ba1-xKxBiO3 single crystal.
We investigate the effect of post-deposition annealing (for temperatures from 848 K to 1273 K) on the chemical properties of crystalline Ta$_2$O$_5$ films grown on Si(100) substrates by radio frequency magnetron sputtering. The atomic arrangement, as determined by X-ray diffraction, is predominately hexagonal ($δ$-Ta$_2$O$_5$) for the films exposed to heat treatments at 948 K and 1048 K; orthorhombic ($β$-Ta$_2$O$_5$) for samples annealed at 1148 K and 1273 K; and amorphous for samples annealed at temperatures below 948 K. X-ray photoelectron spectroscopy for Ta $4f$ and O $1s$ core-levels wer…
This work is concerned with Al/Al-oxide(AlO$_{x}$)/Al-layer systems which are important for Josephson-junction-based superconducting devices such as quantum bits. The device performance is limited by noise, which has been to a large degree assigned to the presence and properties of two-level tunneling systems in the amorphous AlO$_{x}$ tunnel barrier. The study is focused on the correlation of the fabrication conditions, nanostructural and nanochemical properties and the occurrence of two-level tunneling systems with particular emphasis on the AlO$_{x}$-layer. Electron-beam evaporation with tw…
We report on the characterization of microwave loss of thin aluminum oxide films at low temperatures using superconducting lumped resonators. The oxide films are fabricated using plasma oxidation of aluminum and have a thickness of 5 nm. We measure the dielectric loss versus microwave power for resonators with frequencies in the GHz range at temperatures from 54 to 303 mK. The power and temperature dependence of the loss is consistent with the tunneling two-level system theory. These results are relevant to understanding decoherence in superconducting quantum devices. The obtained oxide films …
Simulation of 'hybrid' superconductors of 3d-, 4d- and 5d-transition elements consisting of two different superconducting fragments located between positively charged ions planes - B'O2 oxide planes and B2C2 intermetallic layers - has been performed on the basis of the structure of Sr2Mn3As2O2 (A2(B2C2)(B'O2)). The oxide planes are similar to those of CuO2 in high-temperature superconducting cuprates while the intermetallic layers - to those of Ni2B2 in low-temperature superconducting borocarbides RNi2B2C and Fe2As2 layers in high-temperature superconducting oxypnictides RFeAsO1-xFx.
Superconducting thin films of niobium have been extensively employed in transmon qubit architectures. Although these architectures have demonstrated remarkable improvements in recent years, further improvements in performance through materials engineering will aid in large-scale deployment. Here, we use information retrieved from secondary ion mass spectrometry and electron microscopy to conduct a detailed assessment of the surface oxide that forms in ambient conditions for transmon test qubit devices patterned from a niobium film. We observe that this oxide exhibits a varying stoichiometry wi…
We study the stability of Li-O compounds as a function of pressure, with Li ion battery applications and fundamental chemical interest in mind. Using the ab initio evolutionary algorithm, we predict stability of novel compounds LiO4, Li5O3 and Li6O under pressure. LiO4, formed at the pressure of just 6 GPa, can be seen as ε-O8 accepting two electrons from two Li atoms. This phase is superconducting, with Tc up to 12.2 K at 10 GPa. This is remarkable, because elemental oxygen becomes superconducting at much higher pressure (96 GPa) and has much lower Tc (<0.6 K), and suggests that chemical allo…
