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At least 415 records · Page 23

Three-dimensional nanoscale characterisation of materials by atom probe tomography

The development of three-dimensional (3D), characterization techniques with high spatial and mass resolution is crucial for understanding and developing advanced materials for many engineering applications as well as for understanding natural materials. In recent decades, atom probe tomography (APT) which combines a point projection microscope and time-of-flight mass spectrometer has evolved to be an excellent characterization technique capable of providing 3D nanoscale characterization of materials with sub-nanometer scale spatial resolution, with equal sensitivity for all elements. This review discusses the current state as of beginning of the year 2016 of APT instrumentation, new developments in sample preparation methods, experimental procedures for different material classes, reconstruction of APT results, the current status of correlative microscopy, and application of APT for microstructural characterization in established scientific areas like structural materials as well as new applications in semiconducting nanowires, semiconductor devices, battery materials, catalyst materials, geological materials and biological materials. Finally, a brief perspective is given regarding the future of APT.

Atom Probe Tomography, characterization, microstru↗

Energetic neutral atoms measured by the interstellar boundary explorer (IBEX): Evidence for multiple heliosheath populations

Energetic neutral atoms (ENAs) observed by the Interstellar Boundary Explorer (IBEX) provide powerful diagnostics about the origin of the progenitor ion populations and the physical mechanisms responsible for their production. In this paper, we extend the work of Desai et al. and Fuselier et al. and combine and compare ENA spectra from the first 3 yr of observations by the IBEX-Hi and -Lo ENA imagers along the lines-of-sight (LOSs) from the inner heliosphere through to the locations of Voyager 1 and 2 with results from an updated physics-based model of the three-dimensional heliosphere and its constituent ion populations. Our results show that (1) IBEX ENA fluxes and spectra above ∼0.7 keV measured along the LOSs of the Voyagers are consistent with several models in which the parent pickup ion (PUI) populations originate in the inner heliosheath, and (2) a significant fraction of lower energy ENAs between ∼0.1-0.5 keV may originate from interstellar neutral gas charge-exchanging with a non-thermalized (hot) population of PUIs in the outer heliosheath beyond the heliopause. We discuss the implications of ENAs observed by IBEX originating from distinct parent populations as well as from two distinct locations in the heliospheric interface. These results indicate that ENA spectral measurements at various energies can be used to remotely probe distinct physical processes operating in vastly different regions of the distant heliosphere.

79 ASTRONOMY AND ASTROPHYSICS↗

Latitudinal and energy dependence of energetic neutral atom spectral indices measured by the Interstellar Boundary Explorer

We investigate the latitudinal and energy dependence of the globally distributed 0.5–6 keV energetic neutral atom (ENA) spectra measured by the Interstellar Boundary Explorer (IBEX) during the first 3 yrs of the mission. Our results are: (1) the ENA spectral indices at the two lowest energies (0.89 and 1.47 keV) exhibit no clear trend with ecliptic latitude θ, while those at ∼2.29 and ∼3.41 keV exhibit a clear latitudinal pattern; flatter spectra occur above 60° latitude and steeper spectra occur ±30° of the equator. (2) The latitudinal dependence of the spectral indices at different energies can be represented by the cosine function γ=a{sub 0}+a{sub 1}cos(a{sub 2}θ) with unique offsets, amplitudes, and phase angles; the higher energy ENA indices transition to successively larger amplitudes within ±45° of the equator. Our results confirm the previously reported latitudinal organization of the ENA spectra and their remarkable similarity to that of the solar wind (SW) speed observed by Ulysses in the inner heliosphere. While earlier studies showed that the ∼0.5–6 keV globally distributed ENA spectral indices could be represented as single power laws over much of the sky, our new results indicate that this is an over-simplification because the spectral indices have an energy and latitude dependence. This dependence is an important factor that must be taken into consideration by models and simulations that seek to map the IBEX ENA observations back to the latitudinal profile of the SW speed structure observed in the inner heliosphere.

79 ASTRONOMY AND ASTROPHYSICS↗

SIMULATIONS OF A DYNAMIC SOLAR CYCLE AND ITS EFFECTS ON THE INTERSTELLAR BOUNDARY EXPLORER RIBBON AND GLOBALLY DISTRIBUTED ENERGETIC NEUTRAL ATOM FLUX

Since 2009, observations by the Interstellar Boundary Explorer (IBEX) have vastly improved our understanding of the interaction between the solar wind (SW) and local interstellar medium through direct measurements of energetic neutral atoms (ENAs), which inform us about the heliospheric conditions that produced them. An enhanced feature of flux in the sky, the so-called IBEX ribbon, was not predicted by any global models before the first IBEX observations. A dominating theory of the origin of the ribbon, although still under debate, is a secondary charge-exchange process involving secondary ENAs originating from outside the heliopause. According to this mechanism, the evolution of the solar cycle should be visible in the ribbon flux. Therefore, in this paper we simulate a fully time-dependent ribbon flux, as well as globally distributed flux from the inner heliosheath (IHS), using time-dependent SW parameters from Sokół et al. as boundary conditions for our time-dependent heliosphere simulation. After post-processing the results to compute H ENA fluxes, our results show that the secondary ENA ribbon indeed should be time dependent, evolving with a period of approximately 11 yr, with differences depending on the energy and direction. Our results for the IHS flux show little periodic change with the 11 yr solar cycle, but rather with short-term fluctuations in the background plasma. While the secondary ENA mechanism appears to emulate several key characteristics of the observed IBEX ribbon, it appears that our simulation does not yet include all of the relevant physics that produces the observed ribbon.

79 ASTRONOMY AND ASTROPHYSICS↗

Dark atoms: asymmetry and direct detection

We present a simple UV completion of Atomic Dark Matter (aDM) in which heavy right-handed neutrinos decay to induce both dark and lepton number densities. This model addresses several outstanding cosmological problems: the matter/anti-matter asymmetry, the dark matter abundance, the number of light degrees of freedom in the early universe, and the smoothing of small-scale structure. Additionally, this realization of aDM may reconcile the CoGeNT excess with recently published null results and predicts a signal in the CRESST Oxygen band. We also find that, due to unscreened long-range interactions, the residual unrecombined dark ions settle into a diffuse isothermal halo.

79 ASTRONOMY AND ASTROPHYSICS↗

Spin-squeezing-induced enhancement of the sensitivity of an atomic clock using coherent population trapping

The coherent population trapping (CPT) effect is used for making compact atomic clocks. There are two types of CPT clocks: the one in which the Raman beams are applied continuously and the one in which two CPT pulses separated by a dark period are applied (Ramsey scheme). It is obvious that the technique of spin squeezing can only be applied to the Ramsey CPT clock to enhance the sensitivity. However, it is not apparent how to adapt to the CPT clock the protocols for the microwave clock using one-axis-twist squeezing (OATS), since the Ramsey CPT clock is not trivially equivalent to the Ramsey microwave clock. In this paper, we show explicitly how to adapt two protocols using OATS, namely, the Schrödinger cat state protocol (SCSP) and the generalization thereof, and the echo squeezing protocol (ESP), to the CPT clock. The ESP magnifies the phase shift by a factor of N / e , while the SCSP magnifies the phase shift by a factor of N / 2 , making it able to achieve a higher sensitivity in the presence of excess noise.

Li, Jinyang↗

Atom-atom correlations in time-of-flight imaging of ultracold bosons in optical lattices

We study the spatial correlations of strongly interacting bosons in a ground state, confined in a two-dimensional square and a three-dimensional cubic lattice. Using the combined Bogoliubov method and the quantum rotor approach, we map the Hamiltonian of strongly interacting bosons onto U(1) phase action in order to calculate the atom-atom correlations' decay along the principal axis and a diagonal of the lattice-plane direction as a function of distance. Lower tunneling rates lead to quicker decays of the correlations, whose character becomes exponential. Finally, correlation functions allow us to calculate quantities that are directly bound to experimental outcomes, namely time-of-flight absorption images and resulting visibility. Our results contain all the characteristic features present in experimental data (transition from Mott insulating blob to superfluid peaks, etc.), emphasizing the usability of the proposed approach.

74 ATOMIC AND MOLECULAR PHYSICS↗

Atomic layer deposition of 2D and 3D standards for synchrotron-based quantitative composition and structure analysis methods

Atomic layer deposition (ALD) is a scalable deposition technique known for producing uniform, conformal films of a wide range of compounds on nearly any substrate material. These traits make it an ideal deposition method for producing films to replace the National Institute of Standards and Technology (NIST) standards and create Standard Reference Materials (SRMs) on a wide range of relevant two-dimensional and three-dimensional substrates. The use of SRM from NIST for quantitative analysis of chemical composition using synchrotron based x-ray fluorescence (SR-XRF) and scanning transmission x-ray microscopy (STXM) is common. Such standards, however, can suffer from inhomogeneity in chemical composition and thickness and often require further calculations, based on sample mounting and detector geometry, to obtain quantitative results. These inhomogeneities negatively impact the reproducibility of the measurements and the quantitative measure itself. Utilizing Rutherford backscattering, x-ray reflectivity, quartz crystal microbalance, STXM, and SR-XRF, the authors show that ALD is capable of producing high quality standards that are homogenous over scales ranging from nanometers to 100s of micrometers.

Becker, Nicholas G.↗

Nonlinear spectroscopic effects in quantum gases induced by atom-atom interactions

We consider nonlinear spectroscopic effects-interaction-enhanced double resonance and spectrum instability-that appear in ultracold quantum gases owing to collisional frequency shift of atomic transitions and, consequently, due to the dependence of the frequencies on the population of various internal states of the particles. Special emphasis is put to two simplest cases, (a) the gas of two-level atoms and (b) double resonance in a gas of three-level bosons, in which the probe transition frequency remains constant.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Ion-Atom Cold Collisions and Atomic Clocks

This paper is an investigation of ion-atom interactions in the cold and ultra-cold temperature regime. Some of the collisional ion-atom interactions present at room temperature are very much reduced in the low temperature regime.

Ion-Atom↗

High-Performance High-Loading Lithium-Sulfur Batteries by Low Temperature Atomic Layer Deposition of Aluminum Oxide on Nanophase S Cathodes

This study examines the effects of nanophase S and surface coatings via atomic layer deposition (ALD) on high-loading sulfur cathodes for developing high-performance and high-energy lithium-sulfur (Li-S) batteries. It is first verified that ball milling is an effective and facile route for nanoengineering microsized S powders and the resultant nanoscale S particles exhibit better performance. Using these ball milled nanoscale S cathodes, it is found that ALD Al2O3 performed at 50 degrees C yields deposits that evolve with ALD cycles from dispersed nanoparticles, to porous, connected films, and finally to dense and continuous films. Moreover, this low temperature ALD process suppresses S loss by sublimation. The ALD Al2O3 greatly improves sulfur cathode sustainable capacity and Coulombic efficiency. This study postulates two different mechanisms underlying the effects of ALD Al2O3 surface coatings depending on their morphology. ALD Al2O3 nanoparticles dispersed on the sulfur surface mainly function to adsorb polysulfides, thereby inhibiting S shuttling and improving sustainable capacity and Coulombic efficiency. By contrast, ALD Al2O3 films behave as a physical barrier to prevent polysulfides from contacting the liquid electrolyte and dissolving. The dispersed Al2O3 nanoparticles improve both sustainable capacity and Coulombic efficiency while the closed Al2O3 films improve Coulombic efficiency while decreasing the capacity

25 ENERGY STORAGE↗

Atomic Gradient Structures: Atomic Gradient Structure Alters Electronic Structure in 3D across the Bulk and Enhances Photoactivity

Understanding structure–function relationships enables the design of materials with tailored functionalities. The long-standing challenge is to design materials with high active volume to improve the efficiency. Tailored grain boundaries and lattice defects are traditionally used to tune the electronic structure near interfaces or defects to promote electron and hole separation. However, the active volume of point defect sites or interfaces in these traditional photocatalysts is extremely low. In this work, we report a structure with continuous atomic positional deformation across the bulk, altering the electronic structure in three-dimension and creating a significantly high active volume. Such a structure in anatase is obtained and tuned by phase transformation during heating process. Transmission electron microscopy and density functional theory results reveal that atomic deformations result in continuous band bending across the particles, facilitating electron–hole separation, inhibiting their recombination, and inducing dramatically enhanced photoactivity. These findings enable a different materials design paradigm that can potentially be harnessed for a broad range of applications.

TiO2↗

Kinetic studies of excited singlet oxygen atom O( 1 D) reactions with ethanol

In this work, themultichannel reaction of excited singlet oxygen atom with ethanol, O( 1 D) + C 2 H 5 OH (1), was studied in a photolysis flow reactor coupled with mid-infrared Faraday rotation spectroscopy (FRS) and UV-IR direct absorption spectroscopy (DAS) at 297 K with reactor pressures of 60, 120, and 150 Torr (bath He). The excited singlet oxygen atom was generated through the photolysis of O 3 at 266 nm. The photon flux and O( 1 D) concentrations were determined by in situ actinometry based on O 3 depletion. Temporal profiles of OH and H 2 O were monitored via DAS signals at ca. 3568.62 and 3568.29 cm –1 , while temporal profiles of HO 2 were measured via FRS signals at ca. 1396.90 cm –1 . The branching ratios of the target reaction (1) were determined by fitting temporal profiles to simulations from an in-house reaction mechanism. Two major reaction channels were identified as CH 3 CHOH + OH and CH 3 O + CH 2 OH, and their branching ratios were determined as 0.46 ± 0.12 and 0.42 ± 0.11, respectively. A specific HO 2 + RO 2 reaction between HO 2 and O 2 CH 2 CH 2 OH (β-RO 2 ) at the low-temperature range is estimated in this work as HO 2 + O 2 CH 2 CH 2 OH → products with a rate constant of 7 × 10 –12 cm 3 molecule –1 s –1 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Self-Assembled Fe-N-Doped Carbon Nanotube Aerogels with Single-Atom Catalyst Feature as High-Efficiency Oxygen Reduction Electrocatalysts

Finely controlled synthesis of high active and robust non-precious metal catalysts with excellent electrocatalytic efficiency towards oxygen reduction reaction is extremely vital for successful implementation of fuel cells and metal batteries. Unprecedented oxygen reduction reaction electrocatalytic performances and the diversified synthetic procedure in term of favorable structure/morphology characteristics make transition metals-derived M–N–C (M=Fe, Co) structures the most promising nanocatalysts. Herein, using the nitrogen-containing small molecular and inorganic salt as precursors and ultrathin tellurium nanowires as templates, we successfully synthesized a series of well-defined M-N-doped hollow carbon nanowire aerogels through one step hydrothermal route and subsequent facile annealing treatment. Taking advantage of the porous nanostructures, one-dimensional building block as well as homogeneity of active sites, the resultant Fe-N-doped carbon hollow nanowire aerogels exhibited excellent ORR electrocatalytic performance even better than commercial Pt/C in alkaline solution, holding great potential in fuel cell applications.

Environmental Molecular Sciences Laboratory↗

Porous Carbon-Hosted Atomically Dispersed Iron-Nitrogen Moiety as Enhanced Electrocatalysts for Oxygen Reduction Reaction in a Wide Range of pH

As one of the alternatives to replace precious metal catalysts, transition-metal–nitrogen–carbon (M–N–C) electrocatalysts have attracted great research interest due to their low cost and good catalytic activities. Despite nanostructured M–N–C catalysts can achieve good electrochemical perfor-mances, they are vulnerable to aggregation and insufficient catalytic sites upon continuous catalytic reaction. In this work, metal–organic frameworks derived porous single-atom electrocatalysts (SAEs) were successfully prepared by simple pyrolysis procedure without any further posttreatment. Combining the X-ray absorption near-edge spectroscopy and electrochemical measure-ments, the SAEs have been identified with superior oxygen reduction reaction (ORR) activity and stability compared with Pt/C catalysts in alkaline condition. More impressively, the SAEs also show excellent ORR electrocatalytic perfor-mance in both acid and neutral media. This study of nonprecious catalysts provides new insights on nanoengineering catalytically active sites and porous structures for nonprecious metal ORR catalysis in a wide range of pH.

Environmental Molecular Sciences Laboratory↗