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At least 793 records · Page 44

Directing Matter: Toward Atomic-Scale 3D Nanofabrication

Here we report that enabling memristive, neuromorphic, and quantum based computing as well as efficient mainstream energy storage and conversion technologies requires next generation of materials customized at the atomic scale. This requires full control of atomic arrangement and bonding in three dimensions. The last two decades witnessed substantial industrial, academic, and government research efforts directed towards this goal through various lithographies and scanning probe based methods. These technologies emphasize 2D surface structures, with some limited 3D capability. Recently, a range of focused electron and ion based methods have demonstrated compelling alternative pathways to achieving atomically precise manufacturing of 3D structures in solids, liquids, and at interfaces. Electron and ion microscopies offer a platform that can simultaneously observe dynamic and static structures at the nano and atomic scales, and also induce structural rearrangements and chemical transformation. The addition of predictive modeling or rapid image analytics and feedback enables guiding these in a controlled manner. Here, we review the recent results that used focused electron and ion beams to create free-standing nanoscale 3D structures, radiolysis and the fabrication potential with liquid precursors, epitaxial crystallization of amorphous oxides with atomic layer precision, as well as visualization and control of individual dopant motion within a 3D crystal lattice. These works lay the foundation for new approaches to directing nanoscale level architectures and offer a potential roadmap to full 3D atomic control in materials. Lastly, in this perspective we lay out the gaps that currently constrain the processing range of these platforms, reflect on indirect requirements, such as the integration of large scale data analysis with theory, and discuss future prospects of these technologies.

36 MATERIALS SCIENCE↗

Assessing the influence of processing parameters and external loading on the nanoporous structure and morphology of nanoporous gold toward catalytic applications

Nanoporous gold structure gains several unique physical and chemical properties from its nanoscale foam structure composed of ligaments and connected pores. The high specific surface area and interconnected pores make its structure ideal for gas catalysis. Catalytic activity arises in part from the high number density of surface steps and kinks at points of high curvature in the nanoporous structure. However, the structure also makes the material macroscopically brittle and unreliable for many applications due to poor mechanical stability. The ligament diameter, which regulates both desirable chemical properties and mechanical instability, can be tuned to over three orders of magnitude, but few morphology features can be adjusted independently of this. In this report we fabricate nanoporous gold with an average ligament diameter of around 10 nm while varying synthesis parameters and quantify the resulting morphology in order to evaluate the effect of processing on the resulting nanoscale foam structure. In situ tensile experiments are performed to observe how both individual ligaments and the foam structure's features change during deformation in real-time. We found two new morphology features that are independently controllable through synthesis parameters and are likely to influence mechanical stability while preserving or enhancing catalytic activity. The curvature of the ligaments can be increased by stirring the electrolyte during dealloying and the width of the ligament diameter size distribution can be adjusted by controlling the coarsening rate. In situ mechanical tests show that grain boundaries can influence crack propagation and that ligaments removed from the crack tip experience both elastic and plastic stress.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Synthesis of nano-sized ZnO particles by co-precipitation method with variation of heating time

Zinc oxide powders have been synthesized by a co-precipitation method at low temperature (85 °C), using zinc acetate dihydrate, ammonia, hydrochloric acid solutions as the reactants. A number of process parameters such as reaction temperature, solution basicity or pH and heating time are the main factors affecting the morphology and physical properties of the ZnO nanostructures. In this work the effect of heating time on the morphology and particles size were studied. The as-synthesized ZnO powders were characterized using transmission electron microscopy (TEM) and X-ray diffraction (XRD) techniques. The samples were also analyzed using Fourier transform infrared (FTIR). Rietveld refinement of XRD data confirms that ZnO crystallizes in the hexagonal wurtzite structure with high degree of purity and the (101) plane predominant. The XRD results show that the average crystallite sizes were about 66, 27 and 12 nm for 3, 4 and 5 h of heating times, respectively. The XRD analysis indicated that a fraction of nano-sized ZnO powders were in the form of aggregates, which was also verified by TEM image. The TEM photograph demonstrated that the nano-sized ZnO particles were a pseudo-spherical shape.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High-speed x-ray phase contrast imaging and digital image correlation analysis of microscale shock response of an additively manufactured energetic material simulant

The performance of energetic materials subjected to dynamic loading significantly depends on their micro- and meso-scale structural morphology. The geometric versatility offered by additive manufacturing opens new pathways to tailor the performance of these materials. Additively manufactured energetic materials (AMEMs) have a wide range of structural characteristics with a hierarchy of length scales and process-inherent heterogeneities, which are hitherto difficult to precisely control. It is important to understand how these features affect AMEMs’ response under dynamic/shock loading. Therefore, temporally and spatially resolved measurements of both macroscopic behavior and micro- and meso-level processes influencing macroscopic behavior are required. In this paper, we analyze the shock compression response of an AMEM simulant loaded under several impact conditions and orientations. Furthermore, x-ray phase contrast imaging (PCI) is used to track features across the observed shock front and determine the linear shock velocity vs particle velocity equation of state, as well as to quantify the interior deformation fields via digital image correlation (DIC) analyses. Photon Doppler velocimetry is simultaneously used to measure the particle velocities of the specimens, which are consistent with those obtained from x-ray PCI. The DIC analyses provide an assessment of the average strain fields inside the material, showing that the average axial strain depends on the loading intensity and reaches as high as 0.23 for impact velocities up to 1.5 km/s. The overall results demonstrate the utility of x-ray PCI for probing “in-material” equation of state and interior strains associated with dynamic shock compression behavior of the AMEM simulant.

3D printing↗

Multiple-Event, Single-Photon Counting Imaging Sensor

The single-photon counting imaging sensor is typically an array of silicon Geiger-mode avalanche photodiodes that are monolithically integrated with CMOS (complementary metal oxide semiconductor) readout, signal processing, and addressing circuits located in each pixel and the peripheral area of the chip. The major problem is its single-event method for photon count number registration. A single-event single-photon counting imaging array only allows registration of up to one photon count in each of its pixels during a frame time, i.e., the interval between two successive pixel reset operations. Since the frame time can t be too short, this will lead to very low dynamic range and make the sensor merely useful for very low flux environments. The second problem of the prior technique is a limited fill factor resulting from consumption of chip area by the monolithically integrated CMOS readout in pixels. The resulting low photon collection efficiency will substantially ruin any benefit gained from the very sensitive single-photon counting detection. The single-photon counting imaging sensor developed in this work has a novel multiple-event architecture, which allows each of its pixels to register as more than one million (or more) photon-counting events during a frame time. Because of a consequently boosted dynamic range, the imaging array of the invention is capable of performing single-photon counting under ultra-low light through high-flux environments. On the other hand, since the multiple-event architecture is implemented in a hybrid structure, back-illumination and close-to-unity fill factor can be realized, and maximized quantum efficiency can also be achieved in the detector array.

Zheng, Xinyu↗

TU-F-18C-03: X-Ray Scatter Correction in Breast CT: Advances and Patient Testing

Purpose: To further develop and perform patient testing of an x-ray scatter correction algorithm for dedicated breast computed tomography (BCT). Methods: A previously proposed algorithm for x-ray scatter signal reduction in BCT imaging was modified and tested with a phantom and on patients. A wireless electronic positioner system was designed and added to the BCT system that positions a tungsten plate in and out of the x-ray beam. The interpolation used by the algorithm was replaced with a radial basis function-based algorithm, with automated exclusion of non-valid sampled points due to patient motion or other factors. A 3D adaptive noise reduction filter was also introduced to reduce the impact of scatter quantum noise post-reconstruction. The impact on image quality of the improved algorithm was evaluated using a breast phantom and seven patient breasts, using quantitative metrics such signal difference (SD) and signal difference-to-noise ratios (SDNR) and qualitatively using image profiles. Results: The improvements in the algorithm resulted in a more robust interpolation step, with no introduction of image artifacts, especially at the imaged object boundaries, which was an issue in the previous implementation. Qualitative evaluation of the reconstructed slices and corresponding profiles show excellent homogeneity of both the background and the higher density features throughout the whole imaged object, as well as increased accuracy in the Hounsfield Units (HU) values of the tissues. Profiles also demonstrate substantial increase in both SD and SDNR between glandular and adipose regions compared to both the uncorrected and system-corrected images. Conclusion: The improved scatter correction algorithm can be reliably used during patient BCT acquisitions with no introduction of artifacts, resulting in substantial improvement in image quality. Its impact on actual clinical performance needs to be evaluated in the future. Research Agreement, Koning Corp., Hologic Inc., Barco Corp Consultant Agreement, Fujifilm Medical Systems.

60 APPLIED LIFE SCIENCES↗

Three-dimensional ultrasonic imaging of concrete elements using different SAFT data acquisition and processing schemes

Ultrasonic testing systems using transducer arrays and the SAFT (Synthetic Aperture Focusing Technique) reconstruction allow for imaging the internal structure of concrete elements. At one-sided access, three-dimensional representations of the concrete volume can be reconstructed in relatively great detail, permitting to detect and localize objects such as construction elements, built-in components, and flaws. Different SAFT data acquisition and processing schemes can be utilized which differ in terms of the measuring and computational effort and the reconstruction result. In this contribution, two methods are compared with respect to their principle of operation and their imaging characteristics. The first method is the conventional single-channel SAFT algorithm which is implemented using a virtual transducer that is moved within a transducer array by electronic switching. The second method is the Combinational SAFT algorithm (C-SAFT), also named Sampling Phased Array (SPA) or Full Matrix Capture/Total Focusing Method (TFM/FMC), which is realized using a combination of virtual transducers within a transducer array. Five variants of these two methods are compared by means of measurements obtained at test specimens containing objects typical of concrete elements. The automated SAFT imaging system FLEXUS is used for the measurements which includes a three-axis scanner with a 1.0 m × 0.8 m scan range and an electronically switched ultrasonic array consisting of 48 transducers in 16 groups. On the basis of two-dimensional and three-dimensional reconstructed images, qualitative and some quantitative results of the parameters image resolution, signal-to-noise ratio, measurement time, and computational effort are discussed in view of application characteristics of the SAFT variants.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Invited Article: Coherent imaging using seeded free-electron laser pulses with variable polarization: First results and research opportunities

FERMI-Elettra, the first vacuum ultraviolet and soft X-ray free-electron laser (FEL) using by default a 'seeded' scheme, became operational in 2011 and has been opened to users since December 2012. The parameters of the seeded FERMI FEL pulses and, in particular, the superior control of emitted radiation in terms of spectral purity and stability meet the stringent requirements for single-shot and resonant coherent diffraction imaging (CDI) experiments. The advantages of the intense seeded FERMI pulses with variable polarization have been demonstrated with the first experiments performed using the multipurpose experimental station operated at the diffraction and projection imaging (DiProI) beamline. The results reported here were obtained with fixed non-periodic targets during the commissioning period in 2012 using 20-32 nm wavelength range. They demonstrate that the performance of the FERMI FEL source and the experimental station meets the requirements of CDI, holography, and resonant magnetic scattering in both multi- and single-shot modes. Moreover, we present the first magnetic scattering experiments employing the fully circularly polarized FERMI pulses. The ongoing developments aim at pushing the lateral resolution by using shorter wavelengths provided by double-stage cascaded FERMI FEL-2 and probing ultrafast dynamic processes using different pump-probe schemes, including jitter-free seed laser pump or FEL-pump/FEL-probe with two color FEL pulses generated by the same electron bunch.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Microscopic studies of nonlocal spin dynamics and spin transport (invited)

Understanding the behavior of spins coupling across interfaces in the study of spin current generation and transport is a fundamental challenge that is important for spintronics applications. The transfer of spin angular momentum from a ferromagnet into an adjacent normal material as a consequence of the precession of the magnetization of the ferromagnet is a process known as spin pumping. We find that, in certain circumstances, the insertion of an intervening normal metal can enhance spin pumping between an excited ferromagnetic magnetization and a normal metal layer as a consequence of improved spin conductance matching. We have studied this using inverse spin Hall effect and enhanced damping measurements. Scanned probe magnetic resonance techniques are a complementary tool in this context offering high resolution magnetic resonance imaging, localized spin excitation, and direct measurement of spin lifetimes or damping. Localized magnetic resonance studies of size-dependent spin dynamics in the absence of lithographic confinement in both ferromagnets and paramagnets reveal the close relationship between spin transport and spin lifetime at microscopic length scales. Finally, detection of ferromagnetic resonance of a ferromagnetic film using the photoluminescence of nitrogen vacancy spins in neighboring nanodiamonds demonstrates long-range spin transport between insulating materials, indicating the complexity and generality of spin transport in diverse, spatially separated, material systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Characterization of coplanar poled electro optic polymer films for Si-photonic devices with multiphoton microscopy

We imaged coplanar poled electro optic (EO) polymer films on transparent substrates with a multiple-photon microscope in reflection and correlated the second-harmonic light intensity with the results of Pockels coefficient (r{sub 33}) measurements. This allowed us to make quantitative measurements of poled polymer films on non-transparent substrates like silicon, which are not accessible with traditional Pockels coefficient measurement techniques. Phase modulators consisting of silicon waveguide devices with EO polymer claddings with a known Pockels coefficient (from V{sub π} measurements) were used to validate the correlation between the second-harmonic signal and r{sub 33}. This also allowed us to locally map the r{sub 33} coefficient in the poled area.

36 MATERIALS SCIENCE↗

Liquid jet breakup regimes at supercritical pressures

Previously, a theory has been presented that explains how discrete vapor–liquid interfaces become diminished at certain high-pressure conditions in a manner that leads to well known qualitative trends observed from imaging in a variety of experiments. Rather than surface tension forces, transport processes can dominate over relevant ranges of conditions. In this paper, this framework is now generalized to treat a wide range of fuel-oxidizer combinations in a manner consistent with theories of capillary flows and extended corresponding states theory. Different flow conditions and species-specific molecular properties are shown to produce distinct variations of interfacial structures and local free molecular paths. These variations are shown to occur over the operating ranges in a variety of propulsion and power systems. Despite these variations, the generalized analysis reveals that the envelope of flow conditions at which the transition from classical sprays to diffusion-dominated mixing occurs exhibits a characteristic shape for all liquid–gas combinations. As a result, for alkane-oxidizer mixtures, it explains that these conditions shift to higher pressure flow conditions with increasing carbon number and demonstrates that, instead of widely assumed classical spray atomization, diffusion-dominated mixing may occur under relevant high-pressure conditions in many modern devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Temperature Measurement of Laser-Irradiated Metals Using Hyperspectral Imaging

Accurate noncontact surface-temperature measurements during laser-based materials processing remain challenging due to the difficulty of establishing reliable emissivity values as a function of temperature and wavelength. Direct measurement of emissivity is difficult, as the emissivity may be changing constantly in the laser-material interaction region, where the temperature gradients are extreme and surface displacement can complicate the measurement. Here, we present a hyperspectral imaging method using a multiwavelength camera to capture the spectral radiance in eight different bands and fit the wavelength-dependent radiance to Planck’s law. Time-resolved temperature measurements during microsecond pulsed-laser irradiation of a metal plate made of the titanium alloy Ti -6 Al -4 V provide temperature information about the irradiated surface with an estimated accuracy of ± 10 % . The extracted wavelength-dependent emissivity slope compares well with reported results for macroscale titanium melts obtained using IR spectroscopy, which measure temperature without any built-in assumptions about the emissivity. The results are directly applicable to temperature monitoring during welding, additive manufacturing, and semiconductor growth.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

The Effect of Adsorbed Volatile Organic Compounds on an Ultrathin Water Film Measurement

Using surface plasmon resonance imaging (SPRi), we have recently shown for the first time the existence of a monolayer water film between droplets during dropwise condensation. This study examines the effect of adsorbed volatile organic compounds (VOCs) on the ultrathin film measurement using SPRi. Further, the work presents the proper surface-treatment process that enables measurements of the ultrathin water layer during high-speed imaging of dropwise condensation at 3000 frame per second. In this study, two methods were applied for cleaning the surface (gold-coated glass)—(1) standard cleaning procedure (SCP) using acetone, isopropyl alcohol, and deionized water and (2) SCP followed by air plasma cleaning. This work discusses the effect of the cleaning procedures on surface roughness, contact angle, and surface chemistry using atomic force microscopy, optical microscopy, and an X-ray photoelectron spectroscope meter. The results showed that SCP before the SPRi is a proper surface-treatment method. The effect of adsorbed VOCs during dropwise condensation on a surface treated with SCP was measured to be 0.0025 (reflectivity unit), which was 70% smaller than the reflectance associated with a monolayer water film. The results of this work confirm a monolayer water film observation during the dropwise condensation, which has been reported before.

36 MATERIALS SCIENCE↗

Direct imaging of thermally-activated grain-boundary diffusion in Cu/Co/IrMn/Pt exchange-bias structures using atom-probe tomography

Magnetic devices are often subject to thermal processing steps, such as field cooling to set exchange bias and annealing to crystallize amorphous magnetic electrodes. These processing steps may result in interdiffusion and the subsequent deterioration of magnetic properties. In this study, we investigated thermally-activated diffusion in Cu/Co/IrMn/Pt exchange biased polycrystalline thin-film structures using atom probe tomography. Images taken after annealing at 400 °C for 60 min revealed Mn diffusion into Co grains at the Co/IrMn interface and along Pt grain boundaries for the IrMn/Pt stack, i.e., a Harrison type C regime. Annealing at 500 °C showed further Mn diffusion into Co grains. At the IrMn/Pt interface, annealing at 500 °C led to a type B behavior since Mn diffusion was detected both along Pt grain boundaries and also into Pt grains. The deterioration of the films' exchange bias properties upon annealing was correlated to the observed diffusion. In particular, the topmost Pt capping layer thickness turned out to be crucial since a faster deterioration of the exchange bias properties for thicker caps was observed. This is consistent with the idea that Pt acts as a getter for Mn, drawing Mn out of the IrMn layer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Further Support of the Development of Advanced Multilayer Optics Coatings for X-Ray Imaging

SAO is working with LLNL to develop Wolter-I optics for x-ray imaging applications at energies of 15-50 keV and above at NNSA facilities. Our work includes R&D on advanced multilayer coatings as well as fabrication and testing of Wolter-I multilayer coated optics. It also includes delivery of custom 3.05-meter focal length Wolter optics with response at energies of interest to Sandia National Laboratories and LLNL. The mandrels for the custom optics are fabricated at MSFC. In previous contracts, SAO delivered several optics to LLNL with response at various energies. During this present contract period two tasks were carried out. Task1: the coating, replication and characterization of a custom optic with peak response at 22.8 keV, using the custom-designed SANZ mandrels. Task2: carrying out modifications to the coating chamber at SAO to accommodate new, longer, custom-designed mandrels (SANZlong) that will be fabricated at NASA MSFC in FY2020. The longer mandrels are necessary to mitigate end effects observed in the replication process for the small optics currently being fabricated.

36 MATERIALS SCIENCE↗

Element-resolved atomic structure imaging of rocksalt Ge{sub 2}Sb{sub 2}Te{sub 5} phase-change material

Disorder-induced electron localization and metal-insulator transitions (MITs) have been a very active research field starting from the seminal paper by Anderson half a century ago. However, pure Anderson insulators are very difficult to identify due to ubiquitous electron-correlation effects. Recently, an MIT has been observed in electrical transport measurements on the crystalline state of phase-change GeSbTe compounds, which appears to be exclusively disorder driven. Subsequent density functional theory simulations have identified vacancy disorder to localize electrons at the Fermi level. Here, we report a direct atomic scale chemical identification experiment on the rocksalt structure obtained upon crystallization of amorphous Ge{sub 2}Sb{sub 2}Te{sub 5}. Our results confirm the two-sublattice structure resolving the distribution of chemical species and demonstrate the existence of atomic disorder on the Ge/Sb/vacancy sublattice. Moreover, we identify a gradual vacancy ordering process upon further annealing. These findings not only provide a structural underpinning of the observed Anderson localization but also have implications for the development of novel multi-level data storage within the crystalline phases.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Real-space observation of ergodicity transitions in artificial spin ice

Abstract Ever since its introduction by Ludwig Boltzmann, the ergodic hypothesis became a cornerstone analytical concept of equilibrium thermodynamics and complex dynamic processes. Examples of its relevance range from modeling decision-making processes in brain science to economic predictions. In condensed matter physics, ergodicity remains a concept largely investigated via theoretical and computational models. Here, we demonstrate the direct real-space observation of ergodicity transitions in a vertex-frustrated artificial spin ice. Using synchrotron-based photoemission electron microscopy we record thermally-driven moment fluctuations as a function of temperature, allowing us to directly observe transitions between ergodicity-breaking dynamics to system freezing, standing in contrast to simple trends observed for the temperature-dependent vertex populations, all while the entropy features arise as a function of temperature. These results highlight how a geometrically frustrated system, with thermodynamics strictly adhering to local ice-rule constraints, runs back-and-forth through periods of ergodicity-breaking dynamics. Ergodicity breaking and the emergence of memory is important for emergent computation, particularly in physical reservoir computing. Our work serves as further evidence of how fundamental laws of thermodynamics can be experimentally explored via real-space imaging.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

The triple decomposition of a fluctuating velocity field in a multiscale flow

A new method for the triple decomposition of a multiscale flow, which is based on the novel optimal mode decomposition (OMD) technique, is presented. OMD provides low order linear dynamics, which fits a given data set in an optimal way and is used to distinguish between a coherent (periodic) part of a flow and a stochastic fluctuation. The method needs no external phase indication since this information, separate for coherent structures associated with each length scale introduced into the flow, appears as the output. The proposed technique is compared against two traditional methods of the triple decomposition, i.e., bin averaging and proper orthogonal decomposition. This is done with particle image velocimetry data documenting the near wake of a multiscale bar array. It is shown that both traditional methods are unable to provide a reliable estimation for the coherent fluctuation while the proposed technique performs very well. The crucial result is that the coherence peaks are not observed within the spectral properties of the stochastic fluctuation derived with the proposed method; however, these properties remain unaltered at the residual frequencies. This proves the method’s capability of making a distinction between both types of fluctuations. The sensitivity to some prescribed parameters is checked revealing the technique’s robustness. Additionally, an example of the method application for analysis of a multiscale flow is given, i.e., the phase conditioned transverse integral length is investigated in the near wake region of the multiscale object array.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗