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At least 253 records · Page 14

Imaging Carrier Dynamics and Transport in Hybrid Perovskites with Transient Absorption Microscopy

In this review, the recent progress in using transient absorption microscopy to image charge transport and dynamics in semiconducting hybrid organic–inorganic perovskites is discussed. The basic principles, instrumentation, and resolution of transient absorption microscopy are outlined. With temporal resolution as high as 10 fs, sub-diffraction-limit spatial resolution, and excited-state structural resolution, these experiments have provided crucial details on charge transport mechanisms that have been previously obscured in conventional ultrafast spectroscopy measurements. Morphology-dependent mapping unveils spatial heterogeneity in carrier recombination and cooling dynamics. By spatially separating the pump and probe beams, carrier transport across grain boundaries has been directly visualized. Further, femtosecond temporal resolution allows for the examination of nonequilibrium transport directly, revealing extraordinarily long-range hot carrier migration. The application of transient absorption microscopy is not limited to hybrid perovskites but can also be useful for other polycrystalline materials in which morphology plays an important role in carrier transport.

36 MATERIALS SCIENCE↗

Flexural rigidity of the Basin and Range-Colorado Plateau-Rocky Mountain transition from coherence analysis of gravity and topography

Stochastic inversion for flexural loads and flexural rigidity of the continental elastic layer can be accomplished most effectively by using the coherence of gravity and topography. However, the spatial resolution of coherence analysis has been limited by use of two-dimensional periodogram spectra from very large (greater than 10(exp 5)sq km) windows that generally include multiple tectonic features. Using a two-dimensional spectral estimator based on the maximum entropy method, the spatial resolution of flexural proerties can be enhanced by a factor of 4 or more, enabling more detailed analysis at the scale of individual tectonic features. This new approach is used to map the spatial variation of flexural rigidity along the Basin and Range transition to the Colorado Plateau and Middle Rocky Mountains physiographic provinces. Large variations in flexural isostatic responses are found, with rigidities ranging from as low as 8.7 x 10(exp 20) N m (elastic thickness (T(sub e) = 4.6 km) in the Basin and Range to as high as 4.1 x 10(exp 24) N m T(sub e) = 77 km) in the Middle Rocky Mountains. These results compare favorably woith independent determinations of flexural rigidity in the region. Areas of low flexural rigidity correlate strongly with areas of high surface heat flow, as is expected from the contingence of flexural rigidity on a temperature-dependent flow law. Also, late Cenozoic normal faults with large displacements are found primarily in area of low flexural rigidity region. The highest flexural rigidity is found within the Archean Wyoming craton, where evidence suggests that deeply rooted cratonic lithosphere may play a role in determining the distribution of tectonism at the surface.

Lowery, Anthony R.↗

Status Report on Characterization of High Burnup Fuel with Advanced Nondestructive Pulsed Neutron PIE

Characterizing irradiated or spent nuclear fuels with pulsed neutron techniques provides microstructural data such as phase fractions as well as crystallographic data, e.g. lattice parameters, from diffraction analysis. Diffraction characterization is complemented by spatially resolved mapping of isotope densities from energy-resolved neutron imaging, in particular neutron absorption resonance imaging, and overall bulk isotope assay with better sensitivity for minority isotopes from neutron absorption resonance spectroscopy without spatial resolution. Furthermore, after characterization at ambient condition, heating of irradiated or spent fuel will allow to characterize differences of e.g. lattice thermal expansion or phase transition temperature and kinetics compared to fresh fuel as well as enable the study of disappearance of irradiation defects. This data enables benchmarking of predictions of properties of irradiated fuels for which otherwise experimental data is sparse. The effort described here strives to characterize a section cut from a high-burnup fuel. Volumes smaller than entire fuel pellets or rodlets as proposed here, e.g. sections cut from a fuel pellet, to pave the way to characterize entire pellets or rodlets in the future.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Calibration of the ROSAT HRI Spectral Response

The ROSAT High Resolution Imager has a limited (2-band) spectral response. This spectral capability can give X-ray hardness ratios on spatial scales of 5 arcseconds. The spectral response of the center of the detector was calibrated before the launch of ROSAT, but the gain decreases-with time and also is a function of position on the detector. To complicate matters further, the satellite is "wobbled", possibly moving a source across several spatial gain states. These difficulties have prevented the spectral response of the ROSAT HRI from being used for scientific measurements. We have used Bright Earth data and in-flight calibration sources to map the spatial and temporal gain changes, and written software which will allow ROSAT users to generate a calibrated XSPEC response matrix and hence determine a calibrated hardness ratio. In this report, we describe the calibration procedure and show how to obtain a response matrix. In Section 2 we give an overview of the calibration procedure, in Section 3 we give a summary of HRI spatial and temporal gain variations. Section 4 describes the routines used to determine the gain distribution of a source. In Sections 5 and 6, we describe in detail how the Bright Earth database and calibration sources are used to derive a corrected response matrix for a given observation. Finally, Section 7 describes how to use the software.

Prestwich, Andrea↗

New approaches to an old problem: addressing spatial gaps in the World Stress Map

Abstract A well-recognized characteristic of the World Stress Map (WSM) database is the continued presence of large spatial gaps in the distribution of the data records despite the more than 40-year development history of the database. The current release has more than 30 000 high-quality (A–C) data records (often referred to as ‘stress indicators’), but while some continental areas (such as Australia) have seen a significant increase in spatial converge with the latest release, other continental regions (Africa, central Asia, most of South America) remain markedly sparse. In this contribution we (1) review the current state of the spatial distribution of stress indicators in the continental regions (above sea-level); (2) quantify the clustering of the stress indicators in the latest WSM release using the Hopkins statistic as a way to explore the current spatial distribution of the indicators and assess future WSM releases; and (3) present three approaches (joint inversion, seismic anisotropy and InSAR) that provide a way to fill in the gaps (both in the S Hmax orientation and principal stress magnitudes) in regions that lack active seismicity and where borehole drilling is cost prohibitive. These three approaches have the potential to guide procedures for improving a priori estimates of the ambient stress field in the Earth's crust and reduce the uncertainty in predicting both the magnitude and orientation of the principal tectonic stresses.

58 GEOSCIENCES↗

Calibration of the ROSAT HRI Spectral Response

The ROSAT High Resolution Imager has a limited (2-band) spectral response. This spectral capability can give X-ray hardness ratios on spatial scales of 5 arcseconds. The spectral response of the center of the detector was calibrated before the launch of ROSAT, but the gain decreases with time and also is a function of position on the detector. To complicate matters further, the satellite is 'wobbled', possibly moving a source across several spatial gain states. These difficulties have prevented the spectral response of the ROSAT High Resolution Imager (HRI) from being used for scientific measurements. We have used Bright Earth data and in-flight calibration sources to map the spatial and temporal gain changes, and written software which will allow ROSAT users to generate a calibrated XSPEC (an x ray spectral fitting package) response matrix and hence determine a calibrated hardness ratio. In this report, we describe the calibration procedure and show how to obtain a response matrix. In Section 2 we give an overview of the calibration procedure, in Section 3 we give a summary of HRI spatial and temporal gain variations. Section 4 describes the routines used to determine the gain distribution of a source. In Sections 5 and 6, we describe in detail how, the Bright Earth database and calibration sources are used to derive a corrected response matrix for a given observation. Finally, Section 7 describes how to use the software.

Prestwich, Andrea H.↗

Global petrologic variations on the moon - A ternary-diagram approach

An improved method for global petrologic mapping of the moon is presented, which uses a color-coded ternary diagram whose apexes are assigned the average Fe and Th/Ti ratio (normalized to chondrites) compositions of KREEP/Mg-suite rocks, mare basalts, and ferroan anorthosites. The composition of each pixel within these Apollo orbital gamma ray data bases is used to determine its position within the ternary diagram. The color corresponding to this ternary position is then placed on a classification map at that pixel's position within the orbital data bases. The resultant classification map shows spatial transitions among petrologic units, allows direct determination of the relative proportions of each end-member composition in a pixel, and provides more geologic information than can be obtained by using only the elemental data. The map units correspond remarkably well to previously delineated geologic provinces.

Davis, Philip A.↗

Mesoscale monitoring of the soil freeze/thaw boundary from orbital microwave radiometry

A technique was developed for mapping the spatial extent of frozen soils from the spectral characteristics of the 10.7 to 37 GHz radiobrightness. Through computational models for the spectral radiobrightness of diurnally heated freesing soils, a distinctive radiobrightness signature was identified for frozen soils, and the signature was cast as a discriminant for unsupervised classification. In addition to large area images, local area spatial averages of radiobrightness were calculated for each radiobrightness channel at 7 meteorologic sites within the test region. Local area averages at the meteorologic sites were used to define the preliminary boundaries in the Freeze Indicator discriminate. Freeze Indicator images based upon Nimbus 7, Scanning Multichannel Microwave Radiometer (SMMR) data effectively map temporal variations in the freeze/thaw pattern for the northern Great Plains at the time scale of days. Diurnal thermal gradients have a small but measurable effect upon the SMMR spectral gradient. Scale-space filtering can be used to improve the spatial resolution of a freeze/thaw classified image.

Dobson, Craig↗

Spatially resolved spectrophotometry of Comet P/Stephan-Oterma

Observations of Comet P/Stephan-Oterma were made with an Intensified Dissector Scanner spectrograph on the McDonald Observatory 2.7-m telescope during the period from July 1980 to February 1981. These spectra cover a range of heliocentric distances from 2.3 AU preperihelion to 1.8 AU postperihelion. A small aperture was used to map the spatial distributions of the gases in the coma. Column densities of the observed cometary emissions (CN, C3, CH, and C2) were calculated, and it is shown that Stephan-Oterma appeared nearly spherically symmetric. These date are used by Cochran (1985) to constrain chemical models of Stephan-Oterma.

Cochran, A. L.↗

Automated Identification and Differentiation of Spectrally Similar Hydrothermal Minerals on Mars

Early telescopic observations corroborated hydration related absorptions on Mars in the infrared. Images from the Viking missions led to speculation of hydrothermal alteration and were followed by two missions which mapped the spatial variability of the ~ 3 μm hydration feature. Since then, the Compact Reconnaissance Imager for Mars (CRISM) has provided high spatial resolution (up to 18m) spectral identification of a suite of hydrothermal and diagenetic minerals which have illuminated a range of formation mechanisms. Presence/absence and spatial segregation or mixing of minerals like prehnite, epidote, chlorite amphiboles, and mixed-layer Fe/Mg smectite-chlorite provide valuable evidence for the geologic setting of deposits on Earth, and these phases are often used as temperature and aqueous chemistry indicators in terrestrial systems. Mapping the distribution of these phases will help to answer whether Mars had widespread conditions favorable for low-grade metamorphism and diagenesis, or only focused hydrothermal systems in areas of high heat flow. Further characterizing the chemistry and structure of these phases will then help to answer how most of the widespread Fe/Mg phyllosilicates formed, further defining early geochemical cycling and climate. A fully automated approach for accurate mapping of important hydrothermal mineral phases on Mars has been a challenge. Due to overlapping features in the M-OH region (~2.2-2.4 μm), the strongest absorption features of chlorite, prehnite, and epidote in the short-wave infrared are difficult to distinguish from one another and from the most commonly occurring hydrated silicates on Mars, Fe/Mg smectites. Weaker absorptions are present in both prehnite and epidote which help to distinguish them from chlorite and smectites, but their relative strength in the presence of noise and spatial mixing is often too low to confidently identify them without the noise suppression and feature enhancement methods described here. The spectral signatures of mixed-layer Fe/Mg smectite-chlorite and partially chloritized Fe/Mg smectites have not yet been adequately assessed. Here we evaluate the effectiveness of two empirical and statistical methods for identifying and differentiating these phases using CRISM data.

Rasmussen, B. P.↗

The Dawn of Geostationary Air Quality Monitoring: Case Studies from Seoul and Los Angeles

With the near-future launch of geostationary pollution monitoring satellite instruments over North America, East Asia, and Europe, the air quality community is preparing for an integrated global atmospheric composition observing system at unprecedented spatial and temporal resolutions. One of the ways that NASA has supported this community preparation is through demonstration of future space-borne capabilities using the Geostationary Trace gas and Aerosol Sensor Optimization (GeoTASO) airborne instrument. This paper integrates repeated high-resolution maps from GeoTASO, ground-based Pandora spectrometers, and low Earth orbit measurements from the Ozone Mapping and Profiler Suite (OMPS), for case studies over two metropolitan areas: Seoul, South Korea on June 9, 2016 and Los Angeles, California on June 27, 2017. This dataset provides a unique opportunity to illustrate how geostationary air quality monitoring platforms and ground-based remote sensing networks will close the current spatiotemporal observation gap. GeoTASO observes large differences in diurnal behavior between these urban areas, with NO2 accumulating within the Seoul Metropolitan Area through the day but NO2 peaking in the morning and decreasing throughout the afternoon in the Los Angeles Basin. In both areas, the earliest morning maps exhibit spatial patterns similar to emission source areas (e.g., urbanized valleys, roadways, major airports). These spatial patterns change later in the day due to boundary layer dynamics, horizontal transport, and chemistry. The nominal resolution of GeoTASO is finer than will be obtained from geostationary platforms, but when NO2 data over Los Angeles are up-scaled to the expected resolution of TEMPO, spatial features discussed are conserved. Pandora instruments installed in both metropolitan areas capture the diurnal patterns observed by GeoTASO, continuously and over longer time periods, and will play a critical role in validation of the next generation of satellite measurement. These case studies demonstrate that different regions can have diverse diurnal patterns and that day-to-day variability due to meteorology or anthropogenic patterns such as weekday/weekend variations in emissions is large. Low Earth orbit measurements, despite their inability to capture the diurnal patterns at fine spatial resolution, will be essential for intercalibrating the geostationary radiances and cross-validating the geostationary retrievals in an integrated global observing system.

Geostationary↗

Planetary Fabry-Perot spectroscopy

Application of high spectral resolution, Earth-based Fabry-Perot spectroscopy to the study of planetary atmospheres, for which current topics are outer planet HD and H2 spectra (atmospheric structure, D/H ratio), Mars CO2, CO, O2, and H2O spectra (atomspheric photochemistry), Venus H2O and HDO, associated laboratory spectroscopy (especially H2 overtone bands, HDO) was accomplished. Monochromatic charge coupled device (CCD) imaging photometry of the Jovian nebula, with images taken in rapid sequence among the diagnostic spectral lines of ionized sulfur species, provided self-supporting snapshots of the Jupiter/Io plasma conditions (spatially resolved electron and ion densities and temperatures), covering the post-Voyager period from 1981 and leading up to the Galileo tour in the early 1990s. High spectral resolution Fabry-Perot/charge coupled device (CCD) imaging of comets (OI, CI, and H2O(+) velocity maps and spatial distriubtions), and Io's charge exchanged neutral jet was studied.

Trauger, J. T.↗

Synchrotron-based X-ray fluorescence microscopy mapping the ionome of a toxic freshwater cyanobacterium

Harmful algal blooms (HABs) pose a major environmental concern across the globe. In abundance, cyanobacteria, or so-called green-blue algae can produce extremely dangerous cyanotoxins that harm humans and animals. This study focused on the mapping and distribution of intracellular macro-and micronutrients of the widespread freshwater cyanobacteria Microcystis aeruginosa (M. aeruginosa). Towards a better understanding of trace metal uptake and homeostasis throughout the cell cycle, we quantitatively mapped the spatial distribution of the elements P, K, Fe, Ca, Zn, Mn, and Cu across the ultrastructure of frozen-hydrated single cells using state-of-theart X-ray nanofluorescence imaging at the Advanced Photon Source (APS) at Argonne National Laboratory. Further, bulk cellular nutrient and trace metal content correlated well with the total intracellular elemental content in individual cells obtained by quantitative synchrotron X-ray fluorescence measurements. Multi-dimensional mappings showed P and K atoms colocalized as discrete semicircular hotspots that were analyzed with respect to their stoichiometry. Elevated Cu and Ca concentrations were detected along division plane of cells. P and K were found to have similar spatial elemental distribution with about 65% and 69% of the total cellular P and K, respectively, located at the hotspots. The P and K colocalization were refined further using nanotomography, showing a K envelope surrounding the P core. Inorganic P and organic P compounds were specified using solution-state 31 P nuclear magnetic resonance (NMR) spectroscopy from M. aeruginosa. Of the total extracted P determined by 31 P NMR spectroscopy, 47% were found to be nucleotides while only 11% were polyphosphates. Multimodal X-ray imaging provides a better understanding of intracellular biochemical processes in cyanobacteria, helping us monitor and combat an emerging environmental threat.

31P NMR spectroscopy↗

Spatio-Spectral Characterization of Multipolar Plasmonic Modes of Au Nanorods via Tip-Enhanced Raman Scattering

Tip-enhanced Raman (TER) spectral images of 4-thiobenzonitrile-coated Au nanorods map the spatial profiles and trace the resonances of dipolar and multipolar plasmonic modes that are characteristic of the imaged particles. For any particular rod, we observe sequential transitions between high-order modes at low frequency shifts and lower-order modes at higher frequencies. We also notice that higher-order modes (up to $m$ = 4) are generally observed for long rods as compared to their shorter analogues, where longitudinal dipolar resonances ($m$ = 1) are observable. In effect, this research adds a new dimension to local optical field mapping via TERS, which we have previously explored. Not only can the magnitudes, vector components, local/nonlocal characters of local optical fields be imaged through molecular TERS, but spatially varying local optical resonances are also direct observables.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Daily Kilometer-Scale MODIS Satellite Maps of PM2.5 Describe Wintertime Episodes

The San Joaquin Valley (SJV) suffers from severe health-endangering episodes of PM2.5 aerosol loadings in wintertime; episodes last approximately 5 days and differ in geographical distribution and composition. PM2.5 stations are scattered; consequently the use of remote sensing to map variable regional patterns of these varying respirable aerosol concentrations is desirable. High-precision AOT retrievals can capture column particulate loading. However,PM2.5 mapping is challenging due to several reasons: particularly thin mixed layers (ML) and thus relatively low aerosol optical thickness (AOT) close to current measurement limits, variable and a typical composition of the aerosols, and complex surface bidirectional reflectance. However, the West does present some advantages in analysis. Air basins are isolated from long-distance transport, and experience predominant strong meteorological subsidence. Thus these Western basin regions have fewer problematic cases of overriding aerosol layers detached from the surface. To counter such local overriding, Chu et al. have described an approach for the Eastern US, and He et al have described a synoptic classification approach useful in Shanghai. The Bay Area Air Quality Management District (BAAQMD) expands our experience with the use of AOT, with lower PM2.5 and several isolated sub-basins. We have prepared daily maps of episodes in each region. We present also a sequence of increasingly detailed statistical models, AOT initially appears to contribute little information; however, inclusion of weather information reveals its utility. Lyapustin and Wang's MultiAngle Implementation of Atmospheric Correction (MAIAC) retrieval for AOT provided the most useful operational remote sensing information for these regions. It provides high (1-km) spatial resolution maps and a high percentage of availability. Empirical regression methods have found that random effects regression models (aka mixed effects models, ME) employing AOT provide good estimates of ground PM2.5 concentrations.Here, we attempt to extend these methods and evaluate the usefulness of AOT with greater physical analysis, based on DISCOVER-AQ4 experience.

Chatfield, Robert B.↗

Revisiting Newly Large Magellanic Cloud Age-gap Star Clusters

Recently, a noticeable number of new star clusters was identified in the outskirts of the Large Magellanic Cloud (LMC) populating the so-called star-cluster age gap, a space of time (∼4–12 Gyr) where the only known star cluster is up-to-date ESO 121-SC 03. We used Survey of the Magellanic Stellar History DR2 data sets, as well as those employed to identify these star-cluster candidates, to produce relatively deep color–magnitude diagrams (CMDs) of 17 out of 20 discovered age-gap star clusters with the aim of investigating them in detail. Our analysis relies on a thorough CMD cleaning procedure of the field-star contamination, which presents variations in its stellar density and astrophysical properties, such as luminosity and effective temperature, around the star-cluster fields. We built star-cluster CMDs from stars with membership probabilities assigned from the cleaning procedure. These CMDs and their respective spatial distribution maps favor the existence of LMC star field density fluctuations rather than age-gap star clusters, although a definitive assessment on them will be possible from further deeper photometry.

47 OTHER INSTRUMENTATION↗

Metal concentration and leaf spatial distribution assessed by synchrotron µXRF in Brazilian nickel hyperaccumulators

Background and Aims: The limited number of known hyperaccumulator species in tropical regions, including Brazil, has hampered the development of nickel (Ni) agromining. In addition, the mechanisms underlying metal accumulation and distribution in these species remain poorly understood, despite their pivotal role in identifying species with economic potential. Furthermore, this study assessed the accumulation potential and foliar spatial distribution of metals in three Brazilian hyperaccumulator species (Pfaffia sarcophylla, Justicia lanstyakii, and Lippia lupulina) growing in one of the world’s largest mafic–ultramafic complexes. Methods Concentrations of Ni and other metals in leaves were determined using portable X-ray fluorescence (pXRF) and inductively coupled plasma optical emission spectroscopy (ICP-OES). Synchrotron-based X-ray microfluorescence (SR-µXRF) was employed to map the spatial distribution of metals across intact leaves. Results: The results revealed leaf Ni concentrations ranging from 320 to 1,950 mg kg⁻ 1 in P. sarcophylla, 1,640 to 6,810 mg kg⁻ 1 in L. lupulina, and 1,990 to 4,900 mg kg⁻ 1 in J. lanstyakii. Nickel, Mn, and Co exhibited similar distribution patterns, concentrating mainly in the leaf margins and veins across all species, while Ca, K, and Mg co-localization suggests regulatory mechanisms for adaptation. Conclusion: Although these plants exhibited Ni hyperaccumulation, our findings suggest limited commercial potential for agromining. Further research on genetic variability and nutrient assimilation, particularly in P. sarcophylla, is recommended to elucidate the mechanisms underlying Ni accumulation and intraspecific variability.

36 MATERIALS SCIENCE↗

Application of a Near Infrared Imaging System for Thermographic Imaging of the Space Shuttle during Hypersonic Re-Entry

High resolution calibrated near infrared (NIR) imagery was obtained of the Space Shuttle s reentry during STS-119, STS-125, and STS-128 missions. The infrared imagery was collected using a US Navy NP-3D Orion aircraft using a long-range infrared optical package referred to as Cast Glance. The slant ranges between the Space Shuttle and Cast Glance were approximately 26-41 nautical miles at point of closest approach. The Hypersonic Thermodynamic Infrared Measurements (HYTHIRM) project was a NASA Langley led endeavor sponsored by the NASA Engineering Safety Center, the Space Shuttle Program Office and the NASA Aeronautics Research Mission Directorate to demonstrate a quantitative thermal imaging capability. HYTHIRM required several mission tools to acquire the imagery. These tools include pre-mission acquisition simulations of the Shuttle trajectory in relationship to the Cast Glance aircraft flight path, radiance modeling to predict the infrared response of the Shuttle, and post mission analysis tools to process the infrared imagery to quantitative temperature maps. The spatially resolved global thermal measurements made during the Shuttle s hypersonic reentry provides valuable flight data for reducing the uncertainty associated with present day ground-to-flight extrapolation techniques and current state-of-the-art empirical boundary-layer transition or turbulent heating prediction methods. Laminar and turbulent flight data is considered critical for the development of turbulence models supporting NASA s next-generation spacecraft. This paper will provide the motivation and details behind the use of an upgraded NIR imaging system used onboard a Navy Cast Glance aircraft and describe the characterizations and procedures performed to obtain quantitative temperature maps. A brief description and assessment will be provided of the previously used analog NIR camera along with image examples from Shuttle missions STS-121, STS-115, and solar tower test. These thermal observations confirmed the challenge of a long-range acquisition during re-entry. These challenges are due to unknown atmospheric conditions, image saturation, vibration etc. This provides the motivation for the use of a digital NIR sensor. The characterizations performed on the digital NIR sensor included radiometric, spatial, and spectral measurements using blackbody radiation sources and known targets. An assessment of the collected data for three Space Shuttle atmospheric re-entries, STS-119, STS-125, and STS-128, are provided along with a description of various events of interest captured using the digital NIR imaging system such as RCS firings and boundary layer transitions. Lastly the process used to convert the raw image counts to quantitative temperatures is presented along with comparisons to the Space Shuttle's onboard thermocouples.

Zalameda, Joseph N.↗