Systematic Improvements in Transmon Qubit Coherence Enabled by Niobium Surface Encapsulation

We present a novel transmon qubit fabrication technique that yields systematic improvements in T$_1$ coherence times. We fabricate devices using an encapsulation strategy that involves passivating the surface of niobium and thereby preventing the formation of its lossy surface oxide. By maintaining the same superconducting metal and only varying the surface structure, this comparative investigation examining different capping materials and film substrates across different qubit foundries definitively demonstrates the detrimental impact that niobium oxides have on the coherence times of superconducting qubits, compared to native oxides of tantalum, aluminum or titanium nitride. Our surface-encapsulated niobium qubit devices exhibit T$_1$ coherence times 2 to 5 times longer than baseline niobium qubit devices with native niobium oxides. When capping niobium with tantalum, we obtain median qubit lifetimes above 200 microseconds. Our comparative structural and chemical analysis suggests that amorphous niobium suboxides may induce higher losses. These results are in line with high-accuracy measurements of the niobium oxide loss tangent obtained with ultra-high Q superconducting radiofrequency (SRF) cavities. This new surface encapsulation strategy enables further reduction of dielectric losses via passivation with ambient-stable materials, while preserving fabrication and scalable manufacturability thanks to the compatibility with silicon processes

Mapping Buried Hydrogen-Bonding Networks.

We map buried hydrogen-bonding networks within self-assembled monolayers of 3-mercapto-N-nonylpropionamide on Au{111}. The contributing interactions include the buried S-Au bonds at the substrate surface and the buried plane of linear networks of hydrogen bonds. Both are simultaneously mapped with submolecular resolution, in addition to the exposed interface, to determine the orientations of molecular segments and directional bonding. Two-dimensional mode-decomposition techniques are used to elucidate the directionality of these networks. We find that amide-based hydrogen bonds cross molecular domain boundaries and areas of local disorder

Copper Ion Binding Site in β-Amyloid Peptide.

β-Amyloid aggregates in the brain play critical roles in Alzheimer's disease, a chronic neurodegenerative condition. Amyloid-associated metal ions, particularly zinc and copper ions, have been implicated in disease pathogenesis. Despite the importance of such ions, the binding sites on the β-amyloid peptide remain poorly understood. In this study, we use scanning tunneling microscopy, circular dichroism, and surface-enhanced Raman spectroscopy to probe the interactions between Cu2+ ions and a key β-amyloid peptide fragment, consisting of the first 16 amino acids, and define the copper-peptide binding site. We observe that in the presence of Cu2+, this peptide fragment forms β-sheets, not seen without the metal ion. By imaging with scanning tunneling microscopy, we are able to identify the binding site, which involves two histidine residues, His13 and His14. We conclude that the binding of copper to these residues creates an interstrand histidine brace, which enables the formation of β-sheets

Segmentation of scanning tunneling microscopy images using variational methods and empirical wavelets

In the fields of nanoscience and nanotechnology, it is important to be able to functionalize surfaces chemically for a wide variety of applications. Scanning tunneling microscopes (STMs) are important instruments in this area used to measure the surface structure and chemistry with better than molecular resolution. Self-assembly is frequently used to create monolayers that redefine the surface chemistry in just a single-molecule-thick layer (Love et al. in Chem Rev 105(4):1103–1170, 2005; Nuzzo and Allara in J Am Chem Soc 105(13):4481–4483, 1983; Smith et al. in Prog Surf Sci 75(1):1–68, 2004). Indeed, STM images reveal rich information about the structure of self-assembled monolayers since they convey chemical and physical properties of the studied material. In order to assist in and to enhance the analysis of STM and other images (Thomas et al. in ACS Nano 10(5):5446–5451, 2016; Thomas et al. in ACS Nano 9(5):4734–4742, 2015), we propose and demonstrate an image processing framework that produces two image segmentations: One is based on intensities (apparent heights in STM images) and the other is based on textural patterns. The proposed framework begins with a cartoon + texture decomposition, which separates an image into its cartoon and texture components. Afterward, the cartoon image is segmented by a modified multiphase version of the local Chan–Vese model (Wang et al. in Pattern Recognit 43(3):603–618, 2010), while the texture image is segmented by a combination of 2D empirical wavelet transform and a clustering algorithm. Overall, our proposed framework contains several new features, specifically in presenting a new application of cartoon + texture decomposition and of the empirical wavelet transforms and in developing a specialized framework to segment STM images and other data. To demonstrate the potential of our approach, we apply it to raw STM images of various monolayers and present their corresponding segmentation results

Supramolecular Assemblies on Surfaces: Nanopatterning, Functionality, and Reactivity

Understanding how molecules interact to form large-scale hierarchical structures on surfaces holds promise for building designer nanoscale constructs with defined chemical and physical properties. Here, we describe early advances in this field and highlight upcoming opportunities and challenges. Both direct intermolecular interactions and those that are mediated by coordinated metal centers or substrates are discussed. These interactions can be additive, but they can also interfere with each other, leading to new assemblies in which electrical potentials vary at distances much larger than those of typical chemical interactions. Earlier spectroscopic and surface measurements have provided partial information on such interfacial effects. In the interim, scanning probe microscopies have assumed defining roles in the field of molecular organization on surfaces, delivering deeper understanding of interactions, structures, and local potentials. Self-assembly is a key strategy to form extended structures on surfaces, advancing nanolithography into the chemical dimension and providing simultaneous control at multiple scales. In parallel, the emergence of graphene and the resulting impetus to explore 2D materials have broadened the field, as surface-confined reactions of molecular building blocks provide access to such materials as 2D polymers and graphene nanoribbons. In this Review, we describe recent advances and point out promising directions that will lead to even greater and more robust capabilities to exploit designer surfaces.status: publishe

Mapping Buried Hydrogen-Bonding Networks

We map buried hydrogen-bonding networks within self-assembled monolayers of 3-mercapto-<i>N</i>-nonylpropionamide on Au{111}. The contributing interactions include the buried S–Au bonds at the substrate surface and the buried plane of linear networks of hydrogen bonds. Both are simultaneously mapped with submolecular resolution, in addition to the exposed interface, to determine the orientations of molecular segments and directional bonding. Two-dimensional mode-decomposition techniques are used to elucidate the directionality of these networks. We find that amide-based hydrogen bonds cross molecular domain boundaries and areas of local disorder

Acid-Base Control of Valency within Carboranedithiol Self-Assembled Monolayers: Molecules Do the Can-Can.

We use simple acid-base chemistry to control the valency in self-assembled monolayers of two different carboranedithiol isomers on Au{111}. Monolayer formation proceeds via Au-S bonding, where manipulation of pH prior to or during deposition enables the assembly of dithiolate species, monothiol/monothiolate species, or combination. Scanning tunneling microscopy (STM) images identify two distinct binding modes in each unmodified monolayer, where simultaneous spectroscopic imaging confirms different dipole offsets for each binding mode. Density functional theory calculations and STM image simulations yield detailed understanding of molecular chemisorption modes and their relation with the STM images, including inverted contrast with respect to the geometric differences found for one isomer. Deposition conditions are modified with controlled equivalents of either acid or base, where the coordination of the molecules in the monolayers is controlled by protonating or deprotonating the second thiol/thiolate on each molecule. This control can be exercised during deposition to change the valency of the molecules in the monolayers, a process that we affectionately refer to as the "can-can." This control enables us to vary the density of molecule-substrate bonds by a factor of 2 without changing the molecular density of the monolayer