Single-Event Characterization of the 16 nm FinFET Xilinx UltraScale+? RFSoC Field-Programmable Gate Array under Proton Irradiation.
Abstract not provided.
Davis, Philip↗
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Capture of Single Silver Nanoparticles in Nanopore Arrays Detected by Simultaneous Amperometry and Surface-Enhanced Raman Scattering
The attoliter volumes and confinement abilities of zero-dimensional nanopore-electrode arrays (NEAs) hold considerable promise for examining the behavior of single nanoparticles. In this work, we use surface-enhanced Raman scattering (SERS) in tandem with amperometry in order to monitor single Ag Raman-sentinel nanoparticles transported to and captured in single nanopores. To that end, highly ordered solid-state NEAs were fabricated to contain periodic arrays of nanopores, each housing a single recessed Au-ring electrode. These were used to electrostatically capture and trap single silver nanoparticles (AgNPs) functionalized with the electrochemically stable Raman reporter, 1,4-bis(2-methylstyryl)benzene (bis-MSB). Transport and capture of the bis-MSB-tagged AgNPs in the nanopores was followed by simultaneous amperometry and SERS signals characteristic of AgNP oxidation and enhanced Raman scattering by bis-MSB at silver–gold hot spots, respectively. The frequency and magnitude of oxidation-current spikes increased with stepwise increases in DC voltage, and characteristic bis-MSB SERS spectra were observed. Under AC excitation, on the other hand, two distinctly different types of SERS signals were observed, independent of frequency and amplitude: (1) strong, transient (<10 s) spectra and (2) slow (>100 s) monotonically diminishing spectra. We hypothesize that the former behavior results from AgNP aggregates, whereas the latter occurs as a result of multiple incomplete AgNP-oxidation events in succession. Here, these results show that attoliter-volume NEAs are competent for acquiring concurrent SERS spectra and for amperometry of single nanoparticles and that together these measurements can illuminate the collision dynamics of nanoparticles in confined environments.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Reactivity of a Carbon-Supported Single-Site Molybdenum Dioxo Catalyst for Biodiesel Synthesis
A single-site molybdenum dioxo catalyst, (O c ) 2 Mo(=O)2@C, was prepared via direct grafting of MoO 2 Cl 2 (dme) (dme = 1,2-dimethoxyethane) on high-surface-area activated carbon. The physicochemical and chemical properties of this catalyst were fully characterized by N 2 physisorption, ICP-AES/OES, PXRD, STEM, XPS, XAS, temperature-programmed reduction with H 2 (TPR-H 2 ), and temperature-programmed NH 3 desorption (TPD-NH 3 ). The single-site nature of the Mo species is corroborated by XPS and TPR-H2 data, and it exhibits the lowest reported MoO x T max of reduction reported to date, suggesting a highly reactive Mo VI center. (O c ) 2 Mo(=O) 2 @C catalyzes the transesterification of a variety of esters and triglycerides with ethanol, exhibiting high activity at moderate temperatures (60–90 °C) and with negligible deactivation. (O c ) 2 Mo(=O) 2 @C is resistant to water and can be recycled at least three times with no loss of activity. The transesterification reaction is determined experimentally to be first order in [ethanol] and first order in [Mo] with ΔH ‡ = 10.5(8) kcal mol –1 and ΔS ‡ = –32(2) eu. Here, the low energy of activation is consistent with the moderate conditions needed to achieve rapid turnover. This highly active carbon-supported single-site molybdenum dioxo species is thus an efficient, robust, and low-cost catalyst with significant potential for transesterification processes.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Understanding the Intrinsic Surface Reactivity of Single-Layer and Multilayer PdO(101) on Pd(100)
In this work, we investigated the intrinsic reactivity of CO on single and multilayer PdO(101) grown on Pd(100) using temperature programmed reaction spectroscopy (TPRS) and reflection absorption infrared spectroscopy (RAIRS) experiments as well as density functional theory (DFT) calculations. We find that CO binds more strongly on multilayer than single-layer PdO(101) (~119 vs. 43 kJ/mol), and that CO oxidizes negligibly on single-layer PdO(101) whereas nearly 90% of a saturated layer of CO oxidizes on multilayer PdO(101) during TPRS experiments. RAIRS further shows that CO molecules adsorb on both bridge and atop-Pd cus sites (coordinatively-unsaturated Pd sites) of single-layer PdO(101)/Pd(100), while CO binds exclusively on atop-Pd cus sites of multilayer PdO(101). The DFT calculations reproduce the much stronger binding of CO on multilayer PdO(101) as well as the observed binding site preferences, and reveal that the stronger binding is entirely responsible for the higher CO oxidation activity of multilayer PdO(101)/Pd(100). We show that the O-atom below the Pd cus site, present only on multi-layer PdO(101), modifies the electronic states of the Pd cus atom in a way that enhances the CO-Pd cus bonding. Lastly, we show that a precursor-mediated kinetic model, with energetics determined from the present study, predicts that the intrinsic CO oxidation rates achieved on both single and multilayer PdO(101)/Pd(100) can be expected to exceed the gaseous CO diffusion rate to the surface during steady-state CO oxidation at elevated pressures, even though the intrinsic reaction rates are 4-5 orders of magnitude lower on single layer than on multilayer PdO(101)/Pd(100).
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Neighboring Pd single atoms surpass isolated single atoms for selective hydrodehalogenation catalysis
Single atom catalysts have been found to exhibit superior selectivity over nanoparticulate catalysts for catalytic reactions such as hydrogenation due to their single-site nature. However, improved selectively is often accompanied by loss of activity and slow kinetics. Here we demonstrate that neighboring Pd single atom catalysts retain the high selectivity merit of sparsely isolated single atom catalysts, while the cooperative interactions between neighboring atoms greatly enhance the activity for hydrogenation of carbon-halogen bonds. Experimental results and computational calculations suggest that neighboring Pd atoms work in synergy to lower the energy of key meta-stable reactions steps, i.e., initial water desorption and final hydrogenated product desorption. The placement of neighboring Pd atoms also contribute to nearly exclusive hydrogenation of carbon-chlorine bond without altering any other bonds in organohalogens. The promising hydrogenation performance achieved by neighboring single atoms sheds light on a new approach for manipulating the activity and selectivity of single atom catalysts that are increasingly studied in multiple applications.
36 MATERIALS SCIENCE↗
A single-Pt-atom-on-Ru-nanoparticle electrocatalyst for CO-resilient methanol oxidation
Single Pt atom catalysts are key targets because a high exposure of Pt substantially enhances electrocatalytic activity. In addition, PtRu alloy nanoparticles are the most active catalysts for the methanol oxidation reaction. To combine the exceptional activity of single Pt atom catalysts with an active Ru support we must overcome the synthetic challenge of forming single Pt atoms on noble metal nanoparticles. In this report we demonstrate a process that grows and spreads Pt islands on Ru branched nanoparticles to create single-Pt-atom-on-Ru catalysts. By following the spreading process by in situ TEM, we found that the formation of a stable single atom structure is thermodynamically driven by the formation of strong Pt–Ru bonds and the lowering of the surface energy of the Pt islands. The stability of the single-Pt-atom-on-Ru structure and its resilience to CO poisoning result in a high current density and mass activity for the methanol oxidation reaction over time.
36 MATERIALS SCIENCE↗
Cryogenic Preamplification of a Single-Electron-Transistor using a Silicon-Germanium Heterojunction-Bipolar-Transistor
We examine a silicon-germanium heterojunction bipolar transistor (HBT) for cryogenic pre-amplification of a single electron transistor (SET). The SET current modulates the base current of the HBT directly. The HBT-SET circuit is immersed in liquid helium, and its frequency response from low frequency to several MHz is measured. The current gain and the noise spectrum with the HBT result in a signal-to-noise-ratio (SNR) that is a factor of 10–100 larger than without the HBT at lower frequencies. Furthermore, the transition frequency defined by SNR = 1 has been extended by as much as a factor of 10 compared to without the HBT amplification. The power dissipated by the HBT cryogenic pre-amplifier is approximately 5 nW to 5 μW for the investigated range of operation. We found that the circuit is also operated in a single electron charge read-out configuration in the time-domain as a proof-of-principle demonstration of the amplification approach for single spin read-out.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Note: Time-gated 3D single quantum dot tracking with simultaneous spinning disk imaging
We describe recent upgrades to a 3D tracking microscope to include simultaneous Nipkow spinning disk imaging and time-gated single-particle tracking (SPT). Simultaneous 3D molecular tracking and spinning disk imaging enable the visualization of cellular structures and proteins around a given fluorescently labeled target molecule. The addition of photon time-gating to the SPT hardware improves signal to noise by discriminating against Raman scattering and short-lived fluorescence. In contrast to camera-based SPT, single-photon arrival times are recorded, enabling time-resolved spectroscopy (e.g., measurement of fluorescence lifetimes and photon correlations) to be performed during single molecule/particle tracking experiments.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Phase coexistence and domain configuration in Pb(Mg 1/3 Nb 2/3 )O 3 -0.34PbTiO 3 single crystal revealed by synchrotron-based X-ray diffractive three-dimensional reciprocal space mapping and piezoresponse force microscopy
The crystalline phases and domain configuration in the morphotropic phase boundary composition Pb(Mg 1/3 Nb 2/3 )O 3 -0.34PbTiO 3 (PMN-0.34PT) single crystal have been investigated by synchrotronbased X-ray 3D Reciprocal Space Mapping (3D-RSM) and Piezoresponse Force Microscopy. The coexistence of tetragonal (T) and monoclinic MC phases in this PMN-0.34PT single crystal is confirmed. The affiliation of each diffraction spot in the 3D-RSM was identified with the assistance of qualitative simulation. Most importantly, the twinning structure between different domains in such a mixed phase PMN-PT crystal is firmly clarified, and the spatial distribution of different twin domains is demonstrated. Additionally, the lattice parameters of T and MC phases in PMN-0.34PT single crystal as well as the tilting angles of crystal lattices caused by the interfacial lattice mismatch are determined.
36 MATERIALS SCIENCE↗
Single-pulse x-ray diffraction using polycapillary optics for in situ dynamic diffraction
Diagnostic use of single-pulse x-ray diffraction (XRD) at pulsed power facilities can be challenging due to factors such as the high flux and brightness requirements for diffraction and the geometric constraints of experimental platforms. By necessity, the x-ray source is usually positioned very close, within a few inches of the sample. On dynamic compression platforms, this puts the x-ray source in the debris field. We coupled x-ray polycapillary optics to a single-shot needle-and-washer x-ray diode source using a laser-based alignment scheme to obtain high-quality x-ray diffraction using a single 16 ns x-ray pulse with the source >1 m from the sample. Additionally, the system was tested on a Mo sample in reflection geometry using 17 keV x-rays from a Mo anode. We also identified an anode conditioning effect that increased the x-ray intensity by 180%. Quantitative measurements of the x-ray focal spot produced by the polycapillary yielded a total x-ray flux on the sample of 3.3 ± 0.5 × 10 7 molybdenum Kα photons.
47 OTHER INSTRUMENTATION↗
Detecting element specific electrons from a single cobalt nanocluster with synchrotron x-ray scanning tunneling microscopy
Here, we use a nanofabricated scanning tunneling microscope tip as a detector to investigate local X-ray induced tunneling and electron emission from a single cobalt nanocluster on a Au(111) surface. The tip-detector is positioned a few angstroms above the nanocluster, and ramping the incident X-ray energy across the Co photoabsorption K-edge enables the detection of element specific electrons. Atomic-scale spatial dependent changes in the X-ray absorption cross section are directly measured by taking the X-ray induced current as a function of X-ray energy. From the measured sample and tip currents, element specific X-ray induced current components can be separated and thereby the corresponding yields for the X-ray induced processes of the single cobalt nanocluster can be determined. The detection of element specific synchrotron X-ray induced electrons of a single nanocluster opens a new avenue for materials characterization on a one particle at-a-time basis.
36 MATERIALS SCIENCE↗
Oscillating and static universes from a single barotropic fluid
We consider cosmological solutions to general relativity with a single barotropic fluid, where the pressure is a general function of the density, p=f(ρ). We derive conditions for static and oscillating solutions and provide examples, extending earlier work to these simpler and more general single-fluid cosmologies. Generically we expect such solutions to suffer from instabilities, through effects such as quantum fluctuations or tunneling to zero size. We also find a classical instability (“no-go” theorem) for oscillating solutions of a single barotropic perfect fluid due to a necessarily negative squared sound speed.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Volume IV. The DUNE far detector single-phase technology
The preponderance of matter over antimatter in the early universe, the dynamics of the supernovae that produced the heavy elements necessary for life, and whether protons eventually decay -- these mysteries at the forefront of particle physics and astrophysics are key to understanding the early evolution of our universe, its current state, and its eventual fate. DUNE is an international world-class experiment dedicated to addressing these questions as it searches for leptonic charge-parity symmetry violation, stands ready to capture supernova neutrino bursts, and seeks to observe nucleon decay as a signature of a grand unified theory underlying the standard model. Central to achieving DUNE's physics program is a far detector that combines the many tens-of-kiloton fiducial mass necessary for rare event searches with sub-centimeter spatial resolution in its ability to image those events, allowing identification of the physics signatures among the numerous backgrounds. In the single-phase liquid argon time-projection chamber (LArTPC) technology, ionization charges drift horizontally in the liquid argon under the influence of an electric field towards a vertical anode, where they are read out with fine granularity. A photon detection system supplements the TPC, directly enhancing physics capabilities for all three DUNE physics drivers and opening up prospects for further physics explorations. The DUNE far detector technical design report (TDR) describes the DUNE physics program and the technical designs of the single- and dual-phase DUNE liquid argon TPC far detector modules. Volume IV presents an overview of the basic operating principles of a single-phase LArTPC, followed by a description of the DUNE implementation. Each of the subsystems is described in detail, connecting the high-level design requirements and decisions to the overriding physics goals of DUNE.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Fluctuation localization imaging-based fluorescence in situ hybridization (fliFISH) for accurate detection and counting of RNA copies in single cells
Here, quantitative gene expression analysis in intact single cells can be achieved using single molecule-based fluorescence in situ hybridization (smFISH). This approach relies on fluorescence intensity to distinguish between true signals, emitted from an RNA copy hybridized with multiple oligonucleotide probes, and background noise. Thus, the precision in smFISH is often compromised by partial or nonspecific probe binding and tissue autofluorescence, especially when only a small number of probes can be fitted to the target transcript. Here we provide an accurate approach for setting quantitative thresholds between true and false signals, which relies on on-off duty cycles of photoswitchable dyes. This fluctuation localization imaging-based FISH (fliFISH) uses on-time fractions (measured over a series of exposures) collected from transcripts bound to as low as 8 probes, which are distinct from on-time fractions collected from nonspecifically bound probes or autofluorescence. Using multicolor fliFISH, we identified radial gene expression patterns in mouse pancreatic islets for insulin, the transcription factor, NKX2-2 and their ratio ( Nkx2 - 2/Ins2 ). These radial patterns, showing higher values in β cells at the islet core and lower values in peripheral cells, were lost in diabetic mouse islets. In summary, fliFISH provides an accurate, quantitative approach for detecting and counting true RNA copies and rejecting false signals by their distinct on-time fractions, laying the foundation for reliable single-cell transcriptomics.
59 BASIC BIOLOGICAL SCIENCES↗
Inclusive cross sections for pairs of identified light charged hadrons and for single protons in e + e - at s = 10.58 GeV
We report the first double differential cross sections of two charged pions and kaons (e + e - →hhX) in electron-positron annihilation as a function of the fractional energies of the two hadrons for any charge and hadron combination. The dependence of these di-hadron cross sections on the topology (same, opposite-hemisphere or anywhere) is also studied with the help of the event shape variable thrust and its axis. The ratios of these di-hadron cross sections for different charges and hadron combinations directly shed light on the contributing fragmentation functions. For example, we find that the ratio of same-sign pion pairs over opposite-sign pion pairs drops toward higher fractional energies where disfavored fragmentation is expected to be suppressed. These di-hadron results are obtained from a 655fb -1 data sample collected near the Υ(4S) resonance with the Belle detector at the KEKB asymmetric-energy e + e - collider. Extending the previously published single-pion and single-kaon cross sections, single-proton (e + e - →pX) cross sections are extracted from a 159fb -1 data sub-sample.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Single-Step Shear-Based Deformation Processing of Electrical Conductor Wires
Commercial electrical conductor wires are currently produced from aluminum alloys by multi-step deformation processing involving rolling and drawing. These processes typically require 10 to 20 steps of deformation, since the plastic strain or reduction that can be imposed in a single step is limited by material workability and process mechanics. Here, we demonstrate a fundamentally different, single-step approach to produce flat wire aluminum products using machining-based deformation that also ensures adequate material workability in the formed product. Two process routes are proposed: (1) chip formation by free-machining (FM), with a post-machining, light drawing reduction (<20%) to achieve desired finish and (2) constrained chip formation by large strain extrusion machining (LSEM). Using commercially pure aluminum conductor alloys (Al 1100 and EC1350) as representative material systems, we demonstrate key features of the machining-based processing, including (a) single-step processing to achieve flat wire geometries, (b) surface finish (Ra = 0.2 to 1.0 μm) comparable to that of commercial wire products made by drawing/rolling, (c) deformation control independent of wire size, and (d) hardness increases of 50–150% over that of annealed wires, while retaining high electrical conductivity (>56% IACS). Here, the wire microstructure, which can also be varied via the large-strain deformation parameters, is correlated with mechanical and electrical properties. Implications for commercial manufacture of flat wire products are discussed.
36 MATERIALS SCIENCE↗
Readout optimization of multi-amplifier sensing charge-coupled devices for single-quantum measurement
The non-destructive readout capability of the Skipper Charge Coupled Device (CCD) has been demonstrated to reduce the noise limitation of conventional silicon devices to levels that allow single-photon or single-electron counting. The noise reduction is achieved by taking multiple measurements of the charge in each pixel. These multiple measurements come at the cost of extra readout time, which has been a limitation for the broader adoption of this technology in particle physics, quantum imaging, and astronomy applications. This work presents recent results of a novel sensor architecture that uses multiple non-destructive floating-gate amplifiers in series to achieve sub-electron readout noise in a thick, fully-depleted silicon detector to overcome the readout time overhead of the Skipper-CCD. This sensor is called the Multiple-Amplifier Sensing Charge-Coupled Device (MAS-CCD) can perform multiple independent charge measurements with each amplifier, and the measurements from multiple amplifiers can be combined to further reduce the readout noise. We will show results obtained for sensors with 8 and 16 amplifiers per readout stage in new readout operations modes to optimize its readout speed. The noise reduction capability of the new techniques will be demonstrated in terms of its ability to reduce the noise by combining the information from the different amplifiers, and to resolve signals in the order of a single photon per pixel. The first readout operation explored here avoids the extra readout time needed in the MAS-CCD to read a line of the sensor associated with the extra extent of the serial register. The second technique explore the capability of the MAS-CCD device to perform a region of interest readout increasing the number of multiple samples per amplifier in a targeted region of the active area of the device.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗