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At least 91 records · Page 5

Enhanced gamma ray sensitivity in bismuth triiodide sensors through volumetric defect control

In some of the more attractive semiconducting compounds for ambient temperature radiation detector applications are impacted by low charge collection efficiency due to the presence of point and volumetric defects. This has been particularly true in the case of BiI 3 , which features very attractive properties (density, atomic number, band gap, etc.) to serve as a gamma ray detector, but has yet to demonstrate its full potential. Here, we show that by applying growth techniques tailored to reduce defects, the spectral performance of this promising semiconductor can be realized. Gamma ray spectra from >100 keV source emissions are now obtained from high quality Sb:BiI 3 bulk crystals with limited concentrations of defects (point and extended). The spectra acquired in these high quality crystals feature photopeaks with resolution of 2.2% at 662 keV. Infrared microscopy is used to compare the local microstructure between radiation sensitive and non-responsive crystals. Our work demonstrates that BiI 3 can be prepared in melt-grown detector-grade samples with superior quality and can acquire the spectra from a variety of gamma ray sources.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

The Einstein@Home gamma-ray pulsar survey. I. Search methods, sensitivity, and discovery of new young gamma-ray pulsars

We report on the results of a recent blind search survey for gamma-ray pulsars in Fermi Large Area Telescope (LAT) data being carried out on the distributed volunteer computing system, Einstein@Home. The survey has searched for pulsations in 118 unidentified pulsar-like sources, requiring about 10,000 years of CPU core time. In total, this survey has resulted in the discovery of 17 new gamma-ray pulsars, of which 13 are newly reported in this work, and an accompanying paper. These pulsars are all young, isolated pulsars with characteristic ages between 12 kyr and 2 Myr, and spin-down powers between 10{sup 34} and 4 × 10{sup 36} erg s{sup −1}. Two of these are the slowest spinning gamma-ray pulsars yet known. One pulsar experienced a very large glitch Δf/f≈3.5×10{sup −6} during the Fermi mission. In this, the first of two associated papers, we describe the search scheme used in this survey, and estimate the sensitivity of our search to pulsations in unidentified Fermi-LAT sources. One such estimate results in an upper limit of 57% for the fraction of pulsed emission from the gamma-ray source associated with the Cas A supernova remnant, constraining the pulsed gamma-ray photon flux that can be produced by the neutron star at its center. We also present the results of precise timing analyses for each of the newly detected pulsars.

79 ASTRONOMY AND ASTROPHYSICS↗

Sensitivity to Thermonuclear Reaction Rates in Modeling the Abundance Anomalies of NGC 2419

Abundance anomalies in globular clusters provide strong evidence for multiple stellar populations within each cluster. These populations are usually interpreted as distinct generations, with the currently observed second-generation stars having formed in part from the ejecta of massive, first-generation “polluter” stars, giving rise to the anomalous abundance patterns. The precise nature of the polluters and their enrichment mechanism are still unclear. Even so, the chemical abundances measured in second-generation stars within the globular cluster NGC 2419 provide insight into this puzzling process. Previous work used Monte Carlo nuclear reaction network calculations to constrain the temperature–density conditions that could reproduce the observed abundances, thereby placing robust limits on the origins of the polluter material. The effect of individual reaction rates on these conditions has not been studied, however. Thus, we perform an exhaustive sensitivity study on the nuclear physics input to determine which reactions have the greatest impact on these predictions. We find that the {sup 30}Si(p,γ){sup 31}P, {sup 37}Ar(p,γ){sup 38}K, {sup 38}Ar(p,γ){sup 39}K, and {sup 39}K(p,γ){sup 40}Ca reactions are all critical in determining the temperature–density conditions, and ultimately, the origins of the polluter material. We conclude with recommendations for future experiments.

79 ASTRONOMY AND ASTROPHYSICS↗

The impact of lidar detection sensitivity on assessing aerosol direct radiative effects: LIDAR SENSITIVITY AND AEROSOL DRE

Spaceborne lidar observations have great potential to provide accurate global estimates of the aerosol direct radiative effect (DRE) in both clear and cloudy conditions. However, comparisons between observations from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite (CALIPSO) and multiple years of Atmospheric Radiation Measurement (ARM) program's ground-based Raman lidars (RL) show that CALIPSO does not detect all radiatively significant aerosol, i.e., aerosol that directly modifies the Earth's radiation budget. We estimated that using CALIPSO observations results in an underestimate of the magnitude of the global mean aerosol DRE by up to 54%. The ARM RL data sets along with NASA Langley airborne high spectral resolution lidar data from multiple field campaigns are used to derive the detection sensitivity required to accurately resolve the aerosol DRE. This shows that a lidar with a backscatter coefficient detection sensitivity of about 1–2 × 10 -4 km -1 sr -1 at 532 nm would resolve all the aerosol needed to derive the DRE to within 1%.

54 ENVIRONMENTAL SCIENCES↗

Structure Sensitivity of Acrolein Hydrogenation by Platinum Nanoparticles on Ba x Sr 1- x TiO 3 Nanocuboids

The structure sensitivity of Pt nanoparticles (Pt N ) for gas-phase acrolein (AC) hydrogenation was probed for Pt N on Ba x Sr 1- x TiO 3 nanocuboid supports with (0 0 1) facets in a combined theoretical and experimental study. The in situ selectivity for allyl alcohol increased with the increase of the Sr concentration in the support, which corresponds to modifications in the stable Winterbottom shape and lattice strain of the Pt nanoparticles as a result of the interfacial energy between Pt and the Ba x Sr 1- x TiO 3 supports. “Local model” nanofacets of the Pt surface, edge, and corner morphologies were developed as compact representations of adsorption and reaction sites. DFT was used as the primary modeling tool for the equilibrium adsorption states. We argue that adsorption on edge sites is critically important for the overall allyl alcohol selectivity of Pt N catalysts. A simple model was developed to represent Pt N strain effects caused by its interaction with the substrate. Bader topological atom, spherical volume averaging charge, and modified bond valence sum analyses were used to understand the bonding structure. Density of states analysis was performed for the structures of Pt N , adsorbed AC, and intermediate products to examine adsorbate–particle interactions. The simulated hydrogenation of AC on Pt N nanofacets was compared to the in situ hydrogenation of AC by Pt N on Ba x Sr 1- x TiO 3 to examine the effects of facet, edge, and corner sites on the overall selectivity.

bio-inspired↗

Electrochemically Mediated Oxidation of Sensitive Propargylic Benzylic Alcohols

The electrochemical oxidation of sensitive propargylic benzylic alcohols having varying substituents is reported. We describe the preparation and characterization of N-hydroxytetrafluorophthalimide (TFNHPI) and pseudo-high-throughput development of a green electrochemical oxidation protocol for sensitive propargylic benzylic alcohols that employs TFNHPI as a stable electrochemical mediator. Here, the electrochemical oxidation of propargylic benzylic alcohols was leveraged to develop short synthetic pathways for preparing gram quantities of resveratrol natural products such as pauciflorols.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

π-Extended Porphyrin–Phthalocyanine Heterojunction Devices Exhibiting High Ammonia Sensitivity with a Remarkable Light Effect

π-Extended porphyrins represent an attractive class of organic compounds because of their unique photophysical, optoelectronic, and physicochemical properties. Herein, cross-conjugated (Ace-PQ-Ni) and linear-conjugated (AM6) porphyrins are used to build double-layer heterojunction devices by combining them with a lutetium bisphthalocyanine complex (LuPc 2 ). The heterojunction effect at the porphyrin–phthalocyanine interface plays a key role in the charge transport properties. Both devices exhibit exceptionally high ammonia sensitivity at room temperature and under ambient relative humidity, with limit of detection values of 156 and 115 ppb for Ace-PQ-Ni/LuPc 2 and AM6/LuPc 2 sensors, respectively. Interestingly, the Ace-PQ-Ni/LuPc 2 and AM6/LuPc 2 sensors display opposite effects upon light illumination. While the former sensors show largely decreased ammonia sensitivity under light illumination, the current variation of the latter under ammonia is remarkably enhanced with a multiplication factor of 13 and a limit of detection (LOD) of 83 ppb. Here, the striking difference in their sensing properties upon light illumination is attributed to their different π-conjugation pathways (cross-conjugation versus linear conjugation).

conductometric transducer↗

Layer-by-Layer Molecular Assemblies for Dye-Sensitized Photoelectrosynthesis Cells Prepared by Atomic Layer Deposition

In a Dye Sensitized Photoelectrosynthesis Cell (DSPEC) the relative orientation of catalyst and chromophore play important roles. Here we introduce a new, robust, Atomic Layer Deposition (ALD) procedure for the preparation of assemblies on wide bandgap semiconductors. In the procedure, phosphonated metal complex precursors react with metal ion bridging to an external chromophore or catalyst to give assemblies bridged by Al(III), Sn(IV), Ti(IV), or Zr(IV) metal oxide units as bridges. The procedure has been extended to chromophore-catalyst assemblies for water oxidation catalysis. A SnO2 bridged assembly on SnO2/TiO2 core/shell electrodes undergoes water splitting with an incident photon conversion efficiency (IPCE) of 17.1% at 440 nm. Reduction of water at a Ni(II)-based catalyst on NiO films has been shown to give H2. Compared to conventional solution-based procedures, the ALD approach offers significant advantages in scope and flexibility for the preparation of stable surface structures.

DSPEC, core/shell, Atomic Layer Deposition, self-a↗

Increasing flame ionization detector (FID) sensitivity using post-column oxidation–methanation

The flame ionization detector (FID) is a robust tool in gas chromatography (GC) due to its sensitivity and linear response in the detection of common organic compounds. However, FID response to oxygenated or highly functionalized organic molecules is low, or in some cases non-existent, making it difficult or impossible to detect and quantify some organic compounds. In this work, the combination of a GC/FID system with a catalytic microreactor, which performs post-column combustion–methanation to convert organic compounds to methane, is shown to be an effective approach for quantifying low-response organic compounds. Molecules that were previously undetectable by conventional FID, including carbon monoxide and carbon dioxide, respond with the same high response of methane in the FID. Low-response molecules, including formaldehyde, formic acid, formamide, and ten other oxygenates also demonstrated enhanced detector response equivalent to that of methane in the FID. Here, the linear response of the FID to these molecules and the equivalent sensitivity to methane indicate that accurate quantification is possible without the usual calibration-corrections (e.g., response factors or correction factors) to the FID response.

99 GENERAL AND MISCELLANEOUS↗

An array of virtual Frisch-grid CdZnTe detectors and a front-end application-specific integrated circuit for large-area position-sensitive gamma-ray cameras

We developed a robust and low-cost array of virtual Frisch-grid CdZnTe (CZT) detectors coupled to a front-end readout ASIC for spectroscopy and imaging of gamma rays. The array operates as a self-reliant detector module. It is comprised of 36 close-packed 6x6x15 mm 3 detectors grouped into 3x3 sub-arrays of 2x2 detectors with the common cathodes. The front-end analog ASIC accommodates up to 36 anode and 9 cathode inputs. Several detector modules can be integrated into a single- or multi-layer unit operating as a Compton or a coded-aperture camera. We present the results from testing two fully assembled modules and readout electronics. The further enhancement of the arrays’ performance and reduction of their cost are made possible by using position-sensitive virtual Frisch-grid detectors, which allow for accurate corrections of the response of material non-uniformities caused by crystal defects.

36 MATERIALS SCIENCE↗

Uncertainty quantification in elastic constants of SiC f /SiC m tubular composites using global sensitivity analysis

Silicon carbide fiber and silicon carbide matrix (SiC f /SiC m ) tubes produced through the chemical vapor infiltration process have become a candidate cladding material in nuclear applications. The performance of this composite is influenced by many variables such as braiding angle, porosity, material properties, etc., which vary over a range of values due to the inherent fluctuations in the manufacturing process. In this study, the variability in elastic constants of SiC f /SiC m composite has been quantified through multiscale finite element (FE) simulations, variable screening, and high-fidelity surrogate modeling. The key variables dominantly affecting the elastic constants of SiC f /SiC m tubes were identified using global sensitivity analysis. A surrogate to the high-fidelity FE-based model was used in Monte Carlo simulations to generate a hundred thousand samples from which the uncertainty in elastic constants was assessed. It turned out that the coefficient of variation was less than 10%.

Materials Science↗

Global Sensitivity Analysis and Estimation of Model Error, Toward Uncertainty Quantification in Scramjet Computations

The development of scramjet engines is an important research area for advancing hypersonic and orbital flights. Progress toward optimal engine designs requires accurate flow simulations together with uncertainty quantification. However, performing uncertainty quantification for scramjet simulations is challenging due to the large number of uncertain parameters involved and the high computational cost of flow simulations. These difficulties are addressed in this paper by developing practical uncertainty quantification algorithms and computational methods, and deploying them in the current study to large-eddy simulations of a jet in crossflow inside a simplified HIFiRE Direct Connect Rig scramjet combustor. First, global sensitivity analysis is conducted to identify influential uncertain input parameters, which can help reduce the system’s stochastic dimension. Second, because models of different fidelity are used in the overall uncertainty quantification assessment, a framework for quantifying and propagating the uncertainty due to model error is presented. In conclusion, these methods are demonstrated on a nonreacting jet-in-crossflow test problem in a simplified scramjet geometry, with parameter space up to 24 dimensions, using static and dynamic treatments of the turbulence subgrid model, and with two-dimensional and three-dimensional geometries.

33 ADVANCED PROPULSION SYSTEMS↗