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At least 1,135 records · Page 63

Improving performance of inverse Compton sources through laser chirping

We present a new method for computation of radiation spectra in the non-linear regime of operation of inverse Compton sources characterized by high laser intensities. The resulting simulations agree well with the experiments. Increasing the laser intensity changes the longitudinal velocity of the electrons during their collision, leading to considerable non-linear broadening in the scattered radiation spectra. The effects of such ponderomotive broadening are so deleterious that most inverse Compton sources either remain at low laser intensities or pay a steep price to operate at a small fraction of the physically possible peak spectral output. This ponderomotive broadening can be reduced by a suitable frequency modulation (also referred to as "chirping", which is not necessarily linear) of the incident laser pulse, thereby drastically increasing the peak spectral density. This frequency modulation, included in the new code as an optional functionality, is used in simulations to motivate the experimental implementation of this transformative technique.

Terzić, B.↗

Burning conditions and transportation pathways determine biomass-burning aerosol properties in the Ascension Island marine boundary layer

African biomass-burning aerosol (BBA) in the southeast Atlantic Ocean (SEA) marine boundary layer (MBL) is an important contributor to Earth’s radiation budget yet its representation remains poorly constrained in regional and global climate models. Data from the Layered Atlantic Smoke Interactions with Clouds (LASIC) field campaign on Ascension Island (-7.95° N, -14.36° E) detail how fire source regions (burning conditions and fuel type), transport pathways, and longer-term chemical processing affect the chemical, microphysical, and optical properties of the BBA in the remote MBL between June and September of 2017. Ten individual plume events characterize the seasonal evolution of BBA characteristics. Inefficient burning conditions, determined by the mass ratio of refractory black carbon to above-background carbon monoxide (rBC:ΔCO), enhance organic- and sulfate-rich aerosol concentrations in June–July. In contrast, the heart of the burning season exhibited higher rBC:ΔCO values indicative of efficient burning conditions, correlating with more rBC-enriched BBA. Toward the end of the burning season, a mix of burning conditions results in increased variation of the BBA properties. The BBA transit to Ascension Island was predominantly through slow-moving pathways in the MBL and lower free troposphere (FT), facilitating prolonged chemical transformations through heterogeneous and aqueous phase processes. Heterogeneous oxidation can persist for up to 10 days, resulting in a considerable decrease in organic aerosol (OA) mass. OA to rBC mass ratios (OA:rBC) in the MBL between 2 and 5 contrast to higher values of 5 to 15 observed in the nearby FT. Conversely, early-season aqueous-phase processes primarily contributed to aerosol oxidation and some aerosol production, but not appreciable aerosol removal. These two chemical processes yield more light-absorbing BBA in the MBL than in the FT and explain the notably low scattering albedo at 530 nm (SSA 530 ) values (< 0.80) at Ascension Island. This study establishes a robust correlation between SSA 530 and OA:rBC across both MBL and FT, underscoring the dependency of optical properties on chemical composition. These findings highlight how the interplay between chemical composition and atmospheric processing can be improved in global and regional climate models. Questions remain on the mixing of aerosols with different pathway histories, and on what accounts for the doubling of the mass absorption coefficient in the boundary layer.

54 ENVIRONMENTAL SCIENCES↗

Twilight Intensity Variation of the Infrared Hydroxyl Airglow

The vibration rotation bands of the hydroxyl radical are the strongest features in the night airglow and are exceeded in intensity in the dayglow only by the infrared atmospheric bands of oxygen. The variation of intensity during evening twilight is discussed. Using a ground-based Fourier Transform Spectrometer (FTS), hydroxyl intensity measurements as early as 3 deg solar depression were made. Models of the twilight behavior show that this should be sufficient to provide measurement of the main portion of the twilight intensity change. The instrument was equipped with a liquid nitrogen-cooled germanium detector whose high sensitivity combined with the efficiency of the FTS technique permits spectra of the region 1.1 to 1.6 microns at high signal-to-noise to be obtained in two minutes. The use of a polarizer at the entrance aperture of the instrument reduces the intensity of scattered sunlight by a factor of at least ten for zenith observations.

Lowe, R. P.↗

Forward-Looking IED Detector Ground Penetrating Radar

There have been many developments of mine or metal detectors based on ground penetrating radar techniques, usually in hand-held or rover-mounted devices. In most mine or metal detector applications, conditions are in a stationary mode and detection speed is not an important factor. A novel, forward-looking, stepped-frequency ground penetrating radar (GPR) has been developed with a capability to detect improvised explosive devices (IEDs) at vehicular speeds of 15 to 20 mph (24 to 32 km/h), 10 to 20 m ahead of the vehicle, to ensure adequate time for response. The GPR system employs two horn antennas (1.7 to 2.6 GHz, 20 dBi) as transmit and receive. The detector system features a user-friendly instantaneous display on a laptop PC and is a low-power-consumption (3 W) compact system with minimal impact on vehicle operations. In practice, the whole GPR system and a laptop PC can be powered by plugging into a cigarette lighter of a vehicle. The stepped-frequency continuous-wave (CW) radar scans frequency from 1.7 to 2.6 GHz in 1,000 steps of 0.9 MHz, with the full frequency scan in 60 ms. The GPR uses a bi-static configuration with one horn antenna used as a transmitter and the other used as a receiver so that isolation between transmitter and receiver is improved. Since the horn antennas (20 dBi) are mounted on the roof of a vehicle at a shallow inclination angle (15 to 25 with respect to horizontal), there is a first-order reduction in ground reflection so that a significant amount of the total reflected power received by the GPR comes from the scattering of RF energy off of buried objects. The stepped-frequency technique works by transmitting a tone at a particular frequency, while the received signal is mixed with the transmitted tone. As a result, the output of the mixer produces a signal that indicates the strength of the received signal and the extent to which it is in phase or out of phase with the transmitted tone. By taking measurements of the phase relationship between the transmitted and received signals over a wide frequency range, an interference pattern is produced showing all target reflections. When a Fourier transform is performed on this pattern, the result is a time-domain representation of targets. Among the advantages of this technique over impulse radar is the ability to transmit and receive much more total energy, and to use non-damped, highly focused horn antennas. The novelty of the IED detector GPR has been achieved by miniaturization of GPR electronics (single electronics board, 10x5x2 cm), low power consumption (3 W), faster signal processing capability, and minimal impact on vehicle operations.

Kim, Soon Sam↗

Potential absence of observed π2 linear-chain structures in 14O via 10C(α,α) resonances scattering

Background: The preference for light nuclear systems to coagulate into -particle clusters has been well-studied. The possibility of a linear chain configuration of -particles would allow for a new way to study this phenomenon. Purpose: A rotational band of states in C has been claimed showing a linear chain structure. The mirror system, O, has been studied here to examine how this linear chain structure is affected by replacing the valence neutrons with protons. Method: A beam of C was incident into a chamber filled with He:CO gas with the tracks recorded inside the TexAT Time Projection Chamber and the recoil -particles detected by a silicon detector array to measure the cross section. Results: The experimental cross section was compared with previous studies and fit using R-Matrix theory with the previously-observed O states being transformed to the C using mirror symmetry. The measured cross section does not replicate the claimed states, with the predicted cross section exceeding that observed at several energies and angles. Conclusion: A series of possibilities are highlighted with the most likely being that the originally-seen C states did not constitute a rotational band with a potentially incorrect spin assignment due to the limitations of the angular correlation method with non-zero spin particles. The work highlights the difficulties in measuring broad resonances corresponding to a linear chain state in a high level density.

Bishop, J.↗

GoAmazon 2014/15. SRI-PTR-ToFMS Field Campaign Report

Our science team, including Dr. Alex Guenther (previously at Pacific Northwest National Laboratory (PNNL) and now at the University of California, Irvine) Dr. Saewung Kim and Dr. Roger Seco, and Dr. Jim Smith (previously at NCAR and now at UC Irvine), deployed a selected reagent ion – proton transfer reaction – time-of-flight mass spectrometer (SRI-PTR-TOFMS) to the T3 site during the GoAmazon study. One of the major uncertainties in climate model simulations is the effects of aerosols on radiative forcing, and a better understanding of the factors controlling aerosol distributions and life cycle is urgently needed. Aerosols contribute directly to the Earth’s radiation balance by scattering or absorbing light as a function of their physical properties and indirectly through particle-cloud interactions that lead to cloud formation and the modification of cloud properties. On a global scale, the dominant source of organic aerosol is biogenic volatile organic compounds (BVOC) emitted from terrestrial ecosystems. These organic aerosols are a major part of the total mass of all airborne particles and are currently not sufficiently represented in climate models. To incorporate quantitatively the effects of BVOCs and their oxidation products on biogenic organic aerosol (BOA) requires parameterization of their production in terrestrial ecosystems and their atmospheric transformations. This project was designed to reduce the gaps in our understanding of how these processes control BVOCs and BOAs, and their impact on climate. This was accomplished by wet and dry season measurements at the U.S. Department of Energy (DOE)’s Atmospheric Radiation Measurement (ARM) Climate Research Facility T3 site along with a comprehensive suite of complementary measurements. The specific goals were to 1) measure and mechanistically understand the factors affecting aerosol distributions over a tropical rain forest, especially the effects of anthropogenic pollution as a perturbation to the natural state, and 2) develop and implement an upscaling analysis from this new data set and knowledge of aerosol distributions to prognosticate possible climatic impacts of present-day urban pollution and possibly greater pollution in the future.

54 ENVIRONMENTAL SCIENCES↗

Synthesis and in situ high pressure Raman spectroscopy study of AlN dendritic crystal

Graphical abstract: - Highlights: • The sample is the typical dendritic crystal structure. • The phase transition of AlN dendritic crystal is researched. • The Raman signal of rock salt AlN is observed under high pressure. • Grüneisen parameters and phase transition criterion are discussed. - Abstract: AlN dendritic crystal was synthesized by the direct current arc discharge apparatus. X-ray diffraction (XRD) patterns indicated that the sample is hexagonal AlN and preferentially grown along the a-axis direction. Scanning electron microscopy (SEM) and Transmission electron microscopy (TEM) images reveal that the product mainly consists of micron AlN dendritic crystal. In situ high pressure Raman spectra of AlN dendritic crystal has been measured in the pressure ranged from ambient pressure to 32.97 GPa at room temperature by using diamond anvil cell. According to the Raman scattering results, the phase transition from the wurtzite to rock salt was found at about 20.73 GPa by the appearance of a new Raman signal. Above 20.73 GPa, a new Raman signal due to disorder-activated Raman scattering in the rock salt phase was observed. In addition, the pressure coefficients, phase transition criterion, and mode Grüneisen parameters of AlN dendritic crystal, which could be different from that of other AlN, are carefully discussed.

36 MATERIALS SCIENCE↗

Taking the Plunge: Nanoscale Chemical Imaging of Functionalized Gold Triangles in H2O via TERS

We demonstrate fast (0.25 s/pixel) nanoscale chemical imaging in aqueous solution via tip-enhanced Raman scattering (TERS), with sub-15 nm spatial resolution. The substrate consists of 4-mercaptobenzonitrile-functionalized monocrystalline gold triangular platelets immersed in H2O, which we map using a gold-coated AFM probe illuminated using a 633 nm laser source. We find that the recorded TERS images trace the enhanced local optical fields that are sustained towards the edges and corners of the triangles. In effect, we directly map local optical fields of a plasmonic substrate in aqueous solution through molecular TERS. Overall, our described platform and approach may generally be used for chemical and biological imaging, and potentially, to follow chemical transformations at solid-liquid interfaces through TERS.

Bhattarai, Ashish↗

Harnessing interpretable and unsupervised machine learning to address big data from modern X-ray diffraction

The information content of crystalline materials becomes astronomical when collective electronic behavior and their fluctuations are taken into account. In the past decade, improvements in source brightness and detector technology at modern X-ray facilities have allowed a dramatically increased fraction of this information to be captured. Now, the primary challenge is to understand and discover scientific principles from big datasets when a comprehensive analysis is beyond human reach. We report the development of an unsupervised machine learning approach, X-ray diffraction (XRD) temperature clustering (X-TEC), that can automatically extract charge density wave order parameters and detect intraunit cell ordering and its fluctuations from a series of high-volume X-ray diffraction measurements taken at multiple temperatures. We benchmark X-TEC with diffraction data on a quasi-skutterudite family of materials, (Ca x Sr 1–x ) 3 Rh 4 Sn 13 , where a quantum critical point is observed as a function of Ca concentration. We apply X-TEC to XRD data on the pyrochlore metal, Cd 2 Re 2 O 7 , to investigate its two much-debated structural phase transitions and uncover the Goldstone mode accompanying them. We demonstrate how unprecedented atomic-scale knowledge can be gained when human researchers connect the X-TEC results to physical principles. Specifically, we extract from the X-TEC–revealed selection rules that the Cd and Re displacements are approximately equal in amplitude but out of phase. This discovery reveals a previously unknown involvement of 5d 2 Re, supporting the idea of an electronic origin to the structural order. Our approach can radically transform XRD experiments by allowing in operando data analysis and enabling researchers to refine experiments by discovering interesting regions of phase space on the fly.

36 MATERIALS SCIENCE↗

Symmetry-dependent broadening parameters for methane

Experimental results for the pressure-broadened linewidths gamma of methane are presented and compared with theoretical results. A solar Fourier transform spectrometer with spectral resolving power of about one million was used together with a 6-m base length multitraversal absorption cell. Pressures were determined to an accuracy of + or - 0.2 Torr by means of a capacitance manometer. The pressuring gases were N2, H2, and He. Results are presented for numerical averages of all linewidths corresponding to a given tetrahedral symmetry for J = 0-6. For all cases studied, gamma(E) is found to be substantially less than gamma(A), and gamma(A) is found to be near to, but significantly smaller than, gamma(F). Relative inelastic cross sections calculated for argon scattering from methane are compared with relative pressure-broadened linewidths measured in several experiments involving methane and other gases.

Fox, K.↗

The Burst and Transient Source Experiment Earth Occultation Technique

An Earth orbiting detector sensitive to gamma-ray photons will see step-like occultation features in its count rate when a gamma-ray point source crosses the Earth's limb. This is due to the change in atmospheric attenuation of the gamma rays along the line of sight. In an uncollimated detector, these occultation features can be used to locate and monitor astrophysical sources provided their signals can be individually separated from the detector background. We show that the Earth occultation technique applied to the Burst and Transient Source Experiment (BATSE) on the Compton Gamma Ray Observatory (CGRO) is a viable and flexible all-sky monitor in the low-energy gamma-ray and hard X-ray energy range (20 keV-1 MeV). The method is an alternative to more sophisticated photon imaging devices for astronomy and can serve well as a cost-effective science capability for monitoring the high energy sky. Here we describe the Earth occultation technique for locating new sources and for measuring source intensity and spectra without the use of complex background models. Examples of transform imaging, step searches, spectra, and light curves are presented. Systematic uncertainties due to source confusion, detector response, and contamination from rapid background fluctuations are discussed and analyzed for their effect on intensity measurements. A sky location-dependent average systematic error is derived as a function of Galactic coordinates. The sensitivity of the technique is derived as a function of incident photon energy and also as a function of angle between the source and the normal to the detector entrance window. Occultations of the Crab Nebula by the Moon are used to calibrate Earth occultation flux measurements independent of possible atmospheric scattering effects.

Harmon, B. A.↗

Direct dioxygen evolution in collisions of carbon dioxide with surfaces

The intramolecular conversion of CO 2 to molecular oxygen is an exotic reaction, rarely observed even with extreme optical or electronic excitation means. Here we show that this reaction occurs readily when CO 2 ions scatter from solid surfaces in a two-step sequential collision process at hyperthermal incidence energies. The produced O 2 is preferentially ionized by charge transfer from the surface over the predominant atomic oxygen product, leading to direct detection of both O 2 + and O 2 - . First-principles simulations of the collisional dynamics reveal that O 2 production proceeds via strongly-bent CO 2 configurations, without visiting other intermediates. Bent CO 2 provides dynamic access to the symmetric dissociation of CO2 to C+O2 with a calculated yield of 1 to 2% depending on molecular orientation. This unexpected collision-induced transformation of individual CO 2 molecules provides an accessible pathway for generating O 2 in astrophysical environments and may inspire plasmadriven electro- and photo-catalytic strategies for terrestrial CO 2 reduction.

59 BASIC BIOLOGICAL SCIENCES↗

Revisiting metal fluorides as lithium-ion battery cathodes

Metal fluorides, promising lithium-ion battery cathode materials, have been classified as conversion materials due to the reconstructive phase transitions widely presumed to occur upon lithiation. We challenge this view by studying FeF 3 using X-ray total scattering and electron diffraction techniques that measure structure over multiple length scales coupled with density functional theory calculations, and by revisiting prior experimental studies of FeF 2 and CuF 2 . Metal fluoride lithiation is instead dominated by diffusion-controlled displacement mechanisms, and a clear topological relationship between the metal fluoride F- sublattices and that of LiF is established. Initial lithiation of FeF3 forms FeF2 on the particle's surface, along with a cation-ordered and stacking-disordered phase, A-Li x Fe y F 3 , which is structurally related to alpha-/beta-LiMn 2+ Fe 3+ F 6 and which topotactically transforms to B- and then C-Li x Fe y F 3 , before forming LiF and Fe. Lithiation of FeF 2 and CuF 2 results in a buffer phase between FeF 2 /CuF 2 and LiF. Overall, the resulting principles will aid future developments of a wider range of isomorphic metal fluorides.

25 ENERGY STORAGE↗

Impact of Cation Insertion on Semiconducting Polymer Thin Films toward Electrochemical Energy Conversion

Semiconducting polymers are being explored for electrochemical and photoelectrochemical energy transformation and storage applications. For these applications, it is critical to understand how ion insertion from the electrolyte into polymer electrodes modulates the polymer electronic structure and electron doping levels. Here, this study explores electrochemical cation insertion in the n-type conjugated redox polymer P90, composed of alternating naphthalene diimide (NDI) acceptor and bithiophene (T2) donor units, where the NDI units are functionalized with heptaethylene glycol (HEG, 90%) and 2-octyl dodecyl (OD, 10%) side chains. By combining in situ techniques (UV-vis absorption and Raman spectroscopies with electrochemistry), structural analysis using ex situ grazing-incidence wide-angle X-ray scattering (GIWAXS), and density functional theory (DFT) calculations, we reveal that dications enable negative polaron and bipolaron formation in the P90 at less reducing potentials while supporting more bipolaron formation than the monocations; moreover, larger dications with smaller hydrated radii increase the maximum P90 electron doping level. We also determine that the monocations lead to more thermodynamically stabilized polarons compared with the dications. These findings highlight the critical role of cation identity in tuning electrochemical charging, charge stabilization, and electronic structure of n-type conjugated redox polymers, providing guidance on the rational design of polymer-based (photo)electrochemical applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

All-optical image denoising using a diffractive visual processor

Abstract Image denoising, one of the essential inverse problems, targets to remove noise/artifacts from input images. In general, digital image denoising algorithms, executed on computers, present latency due to several iterations implemented in, e.g., graphics processing units (GPUs). While deep learning-enabled methods can operate non-iteratively, they also introduce latency and impose a significant computational burden, leading to increased power consumption. Here, we introduce an analog diffractive image denoiser to all-optically and non-iteratively clean various forms of noise and artifacts from input images – implemented at the speed of light propagation within a thin diffractive visual processor that axially spans <250 × λ, where λ is the wavelength of light. This all-optical image denoiser comprises passive transmissive layers optimized using deep learning to physically scatter the optical modes that represent various noise features, causing them to miss the output image Field-of-View (FoV) while retaining the object features of interest. Our results show that these diffractive denoisers can efficiently remove salt and pepper noise and image rendering-related spatial artifacts from input phase or intensity images while achieving an output power efficiency of ~30–40%. We experimentally demonstrated the effectiveness of this analog denoiser architecture using a 3D-printed diffractive visual processor operating at the terahertz spectrum. Owing to their speed, power-efficiency, and minimal computational overhead, all-optical diffractive denoisers can be transformative for various image display and projection systems, including, e.g., holographic displays.

36 MATERIALS SCIENCE↗

Visualizing heavy fermion confinement and Pauli-limited superconductivity in layered CeCoIn 5

Layered material structures play a key role in enhancing electron–electron interactions to create correlated metallic phases that can transform into unconventional superconducting states. The quasi-two-dimensional electronic properties of such compounds are often inferred indirectly through examination of bulk properties. Here we use scanning tunneling microscopy to directly probe in cross-section the quasi-two-dimensional electronic states of the heavy fermion superconductor CeCoIn 5 . Our measurements reveal the strong confined nature of quasiparticles, anisotropy of tunneling characteristics, and layer-by-layer modulated behavior of the precursor pseudogap gap phase. In the interlayer coupled superconducting state, the orientation of line defects relative to the d-wave order parameter determines whether in-gap states form due to scattering. Spectroscopic imaging of the anisotropic magnetic vortex cores directly characterizes the short interlayer superconducting coherence length and shows an electronic phase separation near the upper critical in-plane magnetic field, consistent with a Pauli-limited first-order phase transition into a pseudogap phase.

36 MATERIALS SCIENCE↗

Synchrotron Radiation in Analysis of Structural Transformations Under Friction Conditions of Carbon Steel

The paper presents results of the structural transformations in the surface of carbon steel specimens during the first tens of cycles of the friction loading with a hard-alloy indenter. The widespread type AISI 1020 carbon steel is used in the experiments which are carried out on the Microfocus Beamline ID13 of the European Synchrotron Radiation Facility. The experimental setup is designed to record the diffraction patterns during the friction. It is shown that at the initial stage of friction, the diffraction maxima significantly broaden due to the defect accumulation in the crystal lattice and, as a consequence, the growth in elastic micro-distortions and the size reduction of the coherent scattering areas. A serious increase is observed in the intensity of reflection from planes of {110} family due to the formation of the respective texture in the surface layers of steel specimens. A non-destructive method is used to detect the diffraction patterns both for non-moving and moving specimens.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Development of Great Lakes algorithms for the Nimbus-G coastal zone color scanner

A series of experiments in the Great Lakes designed to evaluate the application of the Nimbus G satellite Coastal Zone Color Scanner (CZCS) were conducted. Absorption and scattering measurement data were reduced to obtain a preliminary optical model for the Great Lakes. Available optical models were used in turn to calculate subsurface reflectances for expected concentrations of chlorophyll-a pigment and suspended minerals. Multiple nonlinear regression techniques were used to derive CZCS water quality prediction equations from Great Lakes simulation data. An existing atmospheric model was combined with a water model to provide the necessary simulation data for evaluation of the preliminary CZCS algorithms. A CZCS scanner model was developed which accounts for image distorting scanner and satellite motions. This model was used in turn to generate mapping polynomials that define the transformation from the original image to one configured in a polyconic projection. Four computer programs (FORTRAN IV) for image transformation are presented.

Tanis, F. J.↗