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arXiv:2204.06041

Multi-modal electron microscopy study on decoherence sources and their stability in Nb based superconducting qubit

Jin‐Su Oh, Xiaotian Fang, Taehoon Kim, Matt Lynn, Matthew Joseph Kramer, Mehdi Zarea, James A. Sauls, Alexander Romanenko, Sam Posen, A. Grassellino, Cameron Kopas, Mark Field, Jayss Marshall, Hilal Cansizoglu, J. Mutus, Matthew J. Reagor, Lin Zhou

Published Apr 12, 2022• 1 citation
arXivHTMLPDF

Abstract

Niobium is commonly used for superconducting quantum systems as readout resonators, capacitors, and interconnects. The coherence time of the superconducting qubits is mainly limited by microwave dissipation attributed to two-level system defects at interfaces, such as the Nb/Si and Nb/air interface. One way to improve the Nb/air interface quality is by thermal annealing, as shown by extensive studies in 3D superconducting radio frequency (SRF) cavities. However, it is unclear how the microstructure and chemistry of the interface structures change during heat treatment. To address this knowledge gap, we comprehensively characterized Nb films deposited on Si wafers by physical vapor deposition, including (1) an Nb film from a transmon and (2) an Nb film without any patterning step, using an aberration-corrected transmission electron microscope. Both Nb films exhibit columnar growth with strong [110] textures. There is a double layer between the Nb film and Si substrate, which are amorphous niobium silicides with different Nb and Si concentrations. After in-situ heating of the heterostructure at 360°C inside the microscope, the composition of the double layers at the Nb-Si interface remains almost the same despite different thickness changes. The initial amorphous niobium oxide layer on Nb surface decomposes into face-centered cubic Nb nanograins in the amorphous Nb-O matrix upon heating.

DOI
10.48550/arxiv.2204.06041

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Niobium is commonly used for superconducting quantum systems as readout resonators, capacitors, and interconnects. The coherence time of the superconducting qubits is mainly limited by microwave dissipation attributed to two-level system defects at interfaces, such as the Nb/Si and Nb/air interface. One way to improve the Nb/air interface quality is by thermal annealing, as shown by extensive studies in 3D superconducting radio frequency (SRF) cavities. However, it is unclear how the microstructure and chemistry of the interface structures change during heat treatment. To address this knowledge gap, we comprehensively characterized Nb films deposited on Si wafers by physical vapor deposition, including (1) an Nb film from a transmon and (2) an Nb film without any patterning step, using an aberration-corrected transmission electron microscope. Both Nb films exhibit columnar growth with strong [110] textures. There is a double layer between the Nb film and Si substrate, which are amorphous niobium silicides with different Nb and Si concentrations. After in-situ heating of the heterostructure at 360°C inside the microscope, the composition of the double layers at the Nb-Si interface remains almost the same despite different thickness changes. The initial amorphous niobium oxide layer on Nb surface decomposes into face-centered cubic Nb nanograins in the amorphous Nb-O matrix upon heating.
In superconducting transmon qubits, macroscopic characterization is the primary method for probing performance metrics, such as relaxation T1 and dephasing T2 times, resonance frequency, and quality factor. While these measurements can aid our understanding of the dielectric loss of a transmon, they do not allow us to characterize the structural and chemical inhomogeneity of the interfaces which directly impacts this energy loss. These fundamental materials problems must be studied using transmission electron microscopy (TEM) to provide insight into these defects across different qubit interfaces at an atomic scale. In this contribution, we will examine qubits, such as those shown in Figure 1, fabricated at Fermi National Accelerator Laboratory (SQMS Center) [1]. The qubit devices consist of superconducting metal base layers, typically sputter deposited Nb or Ta, and Al/AlOx/Al junctions, where the AlOx barrier is roughly 3nm in thickness and prepared through in-situ oxidation [2]. Characterizing this system prior to its integration within a superconducting radio frequency cavity establishes a baseline for the system, allowing us to isolate fabrication-induced defects before they manifest in performance degradation during quantum measurements. With the samples and fabrication process well known on a macroscopic scale, we study the atomic structure and chemistry of different heterointerfaces within the Josephson junction (JJ) of the transmon qubit and between the sapphire substrate and Nb resonator pads to identify potential defects contributing to the decoherence for qubits constructed with particular geometries. To resolve these defects, atomic-resolution imaging, energy-dispersive X-ray spectroscopy (EDS), and electron-energy loss spectroscopy (EELS) are performed using the JEOL-ARM200CF, an aberration-corrected scanning transmission electron microscope (STEM). Figure 2 provides a clear image of the stacked layers formed as the JJ, but with the addition of a platinum and carbon protective coating added during the focus ion beam (FIB) milling process to preserve pristine Al/AlOx/Al interfaces. 4D-STEM approaches, such as ptychography, orientation mapping and nanoscale diffraction will be employed to further study the layered interfaces and defects in real space and reciprocal space. These techniques can also provide insight into any damage that incurs during lamella preparation using the FIB [3]. Magnetic field-free atomic resolution imaging, differential phase contrast mapping, and monochromated EELS can be achieved using the new MARS-MONO STEM (JEM-Z200MF) without inducing current fluctuations or magnetic field related distortions [4]. By integrating this work across the functional interfaces of the transmon qubits and their different geometries, we will identify possible structural and chemical defects which limit device performance using our multi-modal approach [5]. SQMS fabricated transmon qubits fabricated on HEMEX sapphire substrate imaged via a) ZEISS optical microscope, b) SEM and c) EDS. TEM image of Josephson Junction layered interface at on JEOL-ARM200CF on the ClearView camera with a 200kV accelerating voltage.
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Superconducting qubits have emerged as a potentially foundational platform technology for addressing complex computational problems deemed intractable with classical computing. Despite recent advances enabling multiqubit designs that exhibit coherence lifetimes on the order of hundreds of μs, material quality and interfacial structures continue to curb device performance. Two-level system defects in the thin superconducting film and adjacent dielectric regions introduce stochastic noise and dissipate electromagnetic energy at the cryogenic operating temperatures. In this study, we utilize time-of-flight secondary ion mass spectrometry to understand the role specific fabrication procedures play in introducing such dissipation mechanisms in these complex systems. We interrogated Nb thin films and transmon qubit structures fabricated through slight modifications in the processing and vacuum conditions. We find that when the Nb film is sputtered onto the Si substrate, oxide and silicide regions are generated at various interfaces. We also observe that impurity species, such as niobium hydrides and carbides, are incorporated within the niobium layer during the subsequent lithographic patterning steps. The formation of these resistive compounds likely impacts the superconducting properties of the Nb thin film. Additionally, we observe the presence of halogen species distributed throughout the patterned thin films. We conclude by hypothesizing the source of such impurities in these structures in an effort to intelligently fabricate superconducting qubits and extend coherence times moving forward.
Materials imperfections in Nb -based superconducting quantum circuits—in particular, two-level-system (TLS) defects—are a major source of decoherence, ultimately limiting the performance of quantum computation and sensing. Thus, identifying and understanding the microscopic origin of possible TLS defects in these devices will help develop strategies that eliminate them, which are key to superconducting qubit performance improvement. In this paper, we demonstrate an order-of-magnitude reduction in two-level system losses in three-dimensional superconducting radio frequency (SRF) niobium resonators by a 10-h high vacuum (HV) heat treatment at 650 °C, even after exposure to air and high-pressure rinsing (HPR). X-ray photoelectron spectroscopy (XPS) and high-resolution scanning transmission electron microscopy (STEM) reveal an alteration of the native oxide composition regrown after air exposure and HPR and the creation of nanoscale crystalline oxide regions, which correlates with the measured tenfold quality factor enhancement at low fields of the 1.3 GHz niobium resonator. Tunneling spectroscopy measurements show a pronounced proximity effect that further confirms the presence of metallic layers on the niobium surface.
Superconducting qubits have arisen as a leading technology platform for quantum computing which is on the verge of revolutionizing the world's calculation capacities. Nonetheless, the fabrication of computationally reliable qubit circuits requires increasing the quantum coherence lifetimes, which are predominantly limited by the dissipations of two-level system (TLS) defects present in the thin superconducting film and the adjacent dielectric regions. In this paper, we demonstrate the reduction of two-level system losses in three-dimensional superconducting radio frequency (SRF) niobium resonators by atomic layer deposition (ALD) of a 10 nm aluminum oxide Al2O3 thin films followed by a high vacuum (HV) heat treatment at 650 °C for few hours. By probing the effect of several heat treatments on Al2O3-coated niobium samples by X-ray photoelectron spectroscopy (XPS) plus scanning and conventional high resolution transmission electron microscopy (STEM/HRTEM) coupled with electron energy loss spectroscopy (EELS) and (EDX) , we witness a dissolution of niobium native oxides and the modification of the Al2O3-Nb interface, which correlates with the enhancement of the quality factor at low fields of two 1.3 GHz niobium cavities coated with 10 nm of Al2O3.
Niobium thin films are key components of superconducting microwave resonators. Interest in these devices has increased dramatically because of their application in quantum systems. Despite tremendous effort to improve their performance, loss mechanisms are still not well understood. Nb/substrate and Nb/air interfaces are likely culprits in contributing to decoherence and ultimately limiting the performance of superconducting devices. Here, we investigate the Nb/substrate interface by studying the effect of hydrogen-passivated H:Si(111) substrates on the local superconducting properties of ∼40 nm thick Nb films compared to Nb films grown on typical Si(001) substrates. Specifically, low-temperature scanning tunneling microscopy and spectroscopy are employed to compare nanoscale material properties. The atomically flat monohydride H:Si(111) substrates are found to yield a smoother and less defective interface with the Nb film. Correspondingly, the Nb films grown on H:Si(111) substrates present more uniform superconducting properties and exhibit less quasiparticle broadening.