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All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

Multi-Group Formulation of the Temperature-Dependent Resonance Scattering Model and its Impact on Reactor Core Parameters

A multi-group formulation for the exact neutron elastic scattering kernel is developed. It incorporates the neutron up-scattering effects, stemming from lattice atoms thermal motion and accounts for it within the resulting effective nuclear cross-section data. The effects pertain essentially to resonant scattering off of heavy nuclei. The formulation, implemented into a standalone code, produces effective nuclear scattering data that are then supplied directly into the DRAGON lattice physics code where the effects on Doppler Reactivity and neutron flux are demonstrated. The correct accounting for the crystal lattice effects influences the estimated values for the probability of neutron absorption and scattering, which in turn affect the estimation of core reactivity and burnup characteristics. The results show an increase in values of Doppler temperature feedback coefficients up to -10% for UOX and MOX LWR fuels compared to the corresponding values derived using the traditional asymptotic elastic scattering kernel. This paper also summarizes the results done on this topic to date.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2016

Synthesis, electronic transport and optical properties of Si:α-Fe 2 O 3 single crystals

We report the synthesis of silicon-doped hematite (Si:α-Fe2O3) single crystals via chemical vapor transport, with Si incorporation on the order of 1019 cm-3. The conductivity, Seebeck and Hall effect were measured in the basal plane between 200 and 400 K. Distinct differences in electron transport were observed above and below the magnetic transition temperature of hematite at ~265 K (the Morin transition, TM). Above 265 K, transport was found to agree with the adia-batic small-polaron model, the conductivity was characterized by an activation energy of ~100 meV and the Hall effect was dominated by the weak ferromagnetism of the material. A room temperature electron drift mobility of ~10-2 cm2 V-1 s-1 was estimated. Below TM, the activation energy increased to ~160 meV and a conventional Hall coefficient could be de-termined. In this regime, the Hall coefficient was negative and the corresponding Hall mobility was temperature-independent with a value of ~10-1 cm2 V-1 s-1. Seebeck coefficient measurements indicated that the silicon donors were fully ionized in the temperature range studied. Finally, in the doped species we observe a very broad infrared absorption fea-ture centered near 0.4 eV that does not appear to be hydroxyl related but is tentatively assigned to photon-assisted small-polaron hops. These results are discussed in the context of existing hematite transport studies.

Rettie, Alexander J. E.↗
DOE OSTI2025

Direct measurements for the kinetics of C–C bond fission in the high temperature decomposition of isopropanol

The thermal decomposition of isopropanol was studied experimentally and theoretically with a view to isolate and directly measure rate coefficients for the dominant radical channel in this multi-channel process. Two complementary shock tube methods, laser schlieren densitomtery and H-atom atomic resonance absorption spectroscopy, were used to obtain rate coefficents for the C–C bond fission channel. The experimental ranges span temperatures from 1200–2100 K and pressures between 30–690 torr. These are the most direct measurements of this rate coefficent in the fall-off regime of relevance to high-temperature reacting systems. Theoretical studies also performed in this work confirm that the title reaction and a molecular elimination involving dehydration were the sole unimolecular processes at high temperatures. A master equation analysis yielded k ( T, P ) for the C–C fission and these are shown to be in good agreement with the present experimental measurements. Comparisons with prior experimental and theoretical studies in the literature indicate branching ratios as well as absolute k ( T, P ) for C–C bond-fission have been under-predicted for this decomposition reaction. Consequently, results from the present studies place an increased emphasis on radical-driven secondary processes in high-temperature pyrolysis of this simplest secondary alcohol.

Kim, John H. [Univ. of Michigan, Ann Arbor, MI (Un↗
DOE OSTI2017

Mn{sub 0.1}Ag{sub 0.9}In{sub 4.7}S{sub 7.6} single crystals: Crystal structure, band gap, and thermal expansion

Mn{sub 0.1}Ag{sub 0.9}In{sub 4.7}S{sub 7.6} single crystals are for the first time grown by the Bridgman method (vertical variant). The single crystals crystallize in the cubic spinel structure. The band gap of the single crystals is determined from the transmittance spectra in the region of the fundamental absorption edge at temperatures of T = 295 and 80 K. Thermal expansion is studied by the dilatometric method in the temperature range 80–500 K. The coefficients of thermal expansion, the Debye temperatures, and the rms (root mean square) dynamic displacements of atoms are calculated.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Single-shot Z eff dense plasma diagnostic through simultaneous refraction and attenuation measurements with a Talbot–Lau x-ray moiré deflectometer

The Talbot–Lau x-ray moiré deflectometer is a powerful plasma diagnostic capable of delivering simultaneous refraction and attenuation information through the accurate detection of x-ray phase shift and intensity. The diagnostic can provide the index of refraction n = 1 - δ + iβ of an object (dense plasma, for example) placed in the x-ray beam by independently measuring both δ and β, which are directly related to the electron density ne and the attenuation coefficient μ, respectively. Since δ and β depend on the effective atomic number Z eff , a map can be obtained from the ratio between phase and absorption images acquired in a single shot. The Talbot–Lau x-ray moiré deflectometer and its corresponding data acquisition and processing are briefly described to illustrate how the above is achieved; Z eff values of test objects within the 4–12 range were obtained experimentally through simultaneous refraction and attenuation measurements. We show that Z eff mapping of objects does not require previous knowledge of sample length or shape. The determination of Z eff from refraction and attenuation measurements with Moiré deflectometry could be of high interest to various domains of HED research, such as shocked materials and ICF experiments, as well as material science and NDT.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Optical bistability in PECVD silicon-rich nitride

We present a study of optical bi-stability in a 3.02 refractive index at 1550nm plasma enhanced chemical vapor deposition (PECVD) silicon-rich nitride (SRN) film, as it pertains to bi-stable switching, memory applications, and thermal sensing applications. In this work we utilize an SRN ring resonator device, which we first characterize at low-power and then compare thermo-optic coefficients, (2.12 ± 0.125) × 10 −4 /°C, obtained from thermal-heating induced resonance shifts to optically induced resonance shifts as well as estimated propagation loss and absorption. We then measure the time response of this nonlinearity demonstrating the relaxation time to be 18.7 us, indicating the mechanism to be thermal in nature. Finally, we demonstrate bi-stable optical switching.

42 ENGINEERING↗
NASA NTRS1978

Development of improved lithium tantalate pyroelectric detectors

A program was undertaken to increase the detectivity of LiTaO3 pyroelectric detectors to meet a performance requirement of D star (500 K, 15 Hz)=4x10 to the 9th power cm Hz1/2W-1. Emphasis was placed on reduction of the thermal conductance of the detector element to its surroundings, thinning the detector wafer to a thickness less than 3 micrometers, and increasing the absorptivity of the standard metallic film coatings. During the program, thermal conductance was reduced 41 percent through the use of reticulated (slotted) structures. Self-supported detector wafers less than 2 micrometers thick were fabricated. Multiple layer coatings, including an AR coating, with 16 percent more absorptance, were designed and fabricated. Later refinements in the multilayer design program have absorptivities of 75-80 percent, but detectors with these coatings had to be more than 2 micrometers thick because of a mismatch in the thermal expansion coefficients with LiTaO3.

Byer, N. E.↗
NASA NTRS1988

Temperature dependence of the hydrogen-broadening coefficient for the nu 9 fundamental of ethane

Experimental results for the temperature dependence of the H2-broadening coefficient for the nu 9 fundamental of ethane are reported. Measurements were made over the temperature range 95-300 K using a novel low-temperature absorption cell. These spectra were recorded with the Doppler-limited diode laser spectrometer at NASA Goddard. The results are compared with recent measurements and model predictions.

Halsey, G. W.↗
NASA NTRS2005

Bulk Surface Momentum Parameters for Satellite-Derived Vegetation Fields

The bulk aerodynamic parameters associated with the absorption of surface momentum by vegetated landscapes are theoretically estimated within the context of Raupach's roughness sublayer formulation. The parameters include the bulk plant drag coefficient, maximum u*/U(sub h), sheltering coefficient, and canopy area density at onset of sheltering. Parameters are estimated for the four principal IGBP land cover classes within the U.S. Southern Great Plains: evergreen needleleaf forests, grasslands, croplands, and open shrublands. The estimation approach applies the Method of Moments to roughness data from several international field experiments and other published sources. The results provide the necessary land surface parameters for satellite-based estimation of momentum aerodynamic roughness length and zero-plane displacement height for seasonally variable vegetation fields employed in most terrestrial and atmospheric simulation models used today. Construction of sample displacement and roughness maps over the Southern United States using MODIS land products demonstrates the potential of this approach for regional to global applications.

Jasinski, Michael F.↗
NASA NTRS2016

Monitoring Orbital Precession of EO-1 Hyperion With Three Atmospheric Correction Models in the Libya-4 PICS

Spaceborne spectrometers require spectral-temporal stability characterization to aid in validation of derived data products. Earth Observation 1 (EO-1) began orbital precession in 2011 after exhausting onboard fuel resources. In the Libya-4 pseudo-invariant calibration site (PICS), this resulted in a progressive shift from a mean local equatorial crossing time of approximately10:00 A.M. in 2011 to approximately 8:30 A.M. in late 2015. Here, we studied precession impacts to Hyperion surface reflectance products using three atmospheric correction approaches from 2004 to 2015. Combined difference estimates of surface reflectance were less than 5 percent in the visible near infrared (VNIR) and less than 10 percent for most of the shortwave infrared (SWIR). Combined coefficient of variation estimates in the VNIR ranged from 0.025 to 0.095, and in the SWIR it ranged from 0.025 to 0.06, excluding bands near atmospheric absorption features. Reflectances produced with different atmospheric models were correlated (R squared) in VNIR from 0.25 to 0.94 and in SWIR from 0.12 to 0.88 (p value (calculated probability) less than 0.01). The uncertainties in all the models increased with a terrain slope up to 15 degrees and selecting dune flats could reduce errors. We conclude that these data remain a valuable resource over this period for sensor intercalibration despite orbital decay.

Neigh, Christopher S. R.↗
NASA NTRS2022

Simultaneous Retrievals of Biomass Burning Aerosols and Trace Gases From the Ultraviolet to Near-Infrared Over Northern Thailand During the 2019 Pre-Monsoon Season

With the advent of spaceborne spectroradiometers in a geostationary constellation, measuring high spectral resolution ultraviolet–visible (UV-VIS) and selected near-/shortwave-infrared (NIR/SWIR) radiances can enable the probing of the life cycle of key atmospheric trace gases and aerosols at higher temporal resolutions over the globe. The UV-VIS measurements are important for retrieving several key trace gases (e.g., O 3 , SO 2 , NO 2 , and HCHO) and particularly for deriving aerosol characteristics (e.g., aerosol absorption and vertical profile). This study examines the merit of simultaneous retrievals of trace gases and aerosols using a ground-based spectroradiometer covering the UV-NIR to monitor their physicochemical processes and to obtain reliable aerosol information for various applications. During the 2019 pre-monsoon season over northern Thailand, we deployed a ground-based SMART–s (Spectral Measurements for Atmospheric Radiative Transfer–spectroradiometer) instrument, which is an extended-range Pandora with reliable radiometric calibration in the 330–820 nm range, to retrieve remotely sensed chemical and aerosol properties for the first time near biomass burning sources. The high spectral resolution (∼ 1.0 nm full width half maximum with ∼ 3.7 × oversampling) of sun and sky measurements from SMART–s provides several key trace gases (e.g., O 3 , NO 2 , and H 2 O) and aerosol properties covering the UV where significant light absorption occurs by the carbonaceous particles. During the measurement period, highly correlated total column amounts of NO 2 and aerosol optical thickness (т aer ) retrieved from SMART–s (correlation coefficient, R=0.74) indicated their common emissions from biomass burning events. The SMART–s retrievals of the spectral single scattering albedo (ω 0 ) of smoke aerosols showed an abrupt decrease in the UV, which is an important parameter dictating photochemical processes in the atmosphere. The values of ω 0 and column precipitable water vapor (H 2 O) gradually increase with the mixing of biomass burning smoke particles and higher water vapor concentrations when approaching the monsoon season. The retrieved ω 0 and weighted mean radius of fine-mode aerosols from SMART–s showed positive correlations with the H 2 O (R=0.81 for ω 0 at 330 nm and 0.56 for the volume-weighted mean radius), whereas the real part of the refractive index of fine-mode aerosol (n f ) showed negative correlations (R = -0.61 at 330 nm), which suggest that aerosol aging processes including hygroscopic growth (e.g., humidification and cloud processing) can be a major factor affecting the temporal trends of aerosol optical properties. Retrieved n f and ω 0 were closer to those of the water droplet (i.e., n f of about 1.33 and ω 0 of about 1.0) under lower amounts of NO 2 during the measurement period; considering that the NO 2 amounts in the smoke may indicate the aging of the plume after emission due to its short lifetime, the tendency is also consistent with active hygroscopic processes of the aerosols over this area. Retrieved UV aerosol properties from SMART–s generally support the assumed smoke aerosol models (i.e., the spectral shape of aerosol absorption) used in NASA's current satellite algorithms, and their spectral ω 0 retrievals from ground and satellites showed good agreements (R = 0.73–0.79). However, temporal and spectral variabilities in the aerosol absorption properties in the UV emphasize the importance of a realistic optical model of aerosols for further improvements in satellite retrievals.

biomass burning↗
DOE OSTI2018

Line shape parameters of air-broadened water vapor transitions in the nu(1) and nu(3) spectral region

A Bruker IFS-120HR Fourier transform spectrometer located at the Pacific Northwest Laboratory (PNNL) in Richland, Washington was used to record a series of spectra of pure H2O and air-broadened H2O in the regions of the ¦1 and ¦3 bands (3450-4000 cm-1) at different pressures, mperatures and volume mixing ratios of H2O in air. 18 high-resolution, high signal- to-noise (S/N) ratio absorption spectra were recorded at T = 268, 296 and 353 K using two temperature-controlled absorption cells with path lengths of 9.906(1) and 19.95(1) cm. The resolution of the spectra recorded with the 9.906 cm and 19.95 cm absorption cells was 0.006 and 0.008 cm-1, respectively. A multispectrum nonlinear least squares fitting technique was employed to fit all the eighteen spectra simultaneously to retrieve 313 accurate line positions, 315 intensities, 229 Lorentz air-broadened half- width and 213 air-shift coefficients and their temperature dependences (136 for air-broadened width and 128 for air-shift coefficients, respectively). Room temperature self-broadened half-width coefficients for 209 transitions and self-shift coefficients for 106 transitions were also measured. Line mixing coefficients were experimentally determined for isolated sets of 10 transition pairs for H2O-air and 8 transition pairs for H2O-H2O using the off-diagonal relaxation matrix element formalism, and 85 quadratic speed dependence parameters were measured. Modified Complex Robert-Bonamy (MCRB) calculations of self-, and air-broadened (from N2- and O2-broadening) half-width and air-shift coefficients, and temperature dependence exponents of air-broadened half-width coefficients are made. The measurements and calculations are compared with each other and with similar parameters reported in the literature.

H2O, spectral line shapes, air-broadening, tempera↗
DOE OSTI2021

Time-resolved absorption spectroscopic characterization of ultrafast laser-produced plasmas under varying background pressures

Time-resolved tunable laser absorption spectroscopy is used to characterize the physical properties of ultrafast laser-produced plasmas. The plasmas were produced from an Inconel target, with = 0.4 wt. % Al, using ~ 35 fs, ~800 nm laser pulses at varying Ar background pressures from 1-100 Torr. The absorption spectrum of atomic Al is measured with high spectral and temporal resolution when the probe laser is stepped across the selected Al transition at 394.4 nm. Spectral fitting is used to infer linewidths, kinetic temperature, Al column density, and pressure broadening coefficient. The late time physical properties of plasmas are compared for various pressure levels. Our studies highlight that a significant lower state population exists even at early times of ultrafast laser-produced plasma evolution and lower state population persistence decreases with increasing ambient pressure. We also show that the fundamental optical properties, such as pressure-broadening, can be measured using ultrafast laser-produced plasmas combined with laser absorption spectroscopy.

laser absorption spectroscopy, laser produced plas↗
DOE OSTI2014

Positive temperature variation of the bandgap energy in the single-crystalline chalcopyrite semiconductor AgInS{sub 2}

Optical absorption spectra have been measured on the single-crystalline chalcopyrite semiconductor AgInS{sub 2} using polarized light at T = 10–300 K. The bandgap energy E{sub g} of AgInS{sub 2} shows unusual temperature dependence at low temperatures. The resultant temperature coefficient ∂E{sub g}/∂T is found to be positive at T < 130 K and negative above 130 K. This result has been successfully explained by considering the effects of thermal expansion and electron–phonon interaction. The free-exciton emission of photoluminescence spectra also indicates positive temperature dependence of the peak energies at low temperatures. The exciton binding energy of AgInS{sub 2} is determined to be 26.4 meV.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Chemical Kinetics for the Oxidation of Californium(III) Ions with Select Radiation-Induced Inorganic Radicals (Cl 2 •– and SO 4 •– )

Despite the availability of transuranic elements increasing in recent years, our understanding of their most basic and inherent radiation chemistry is limited and yet essential for accurate interpretation of their physical and chemical properties. Here, in this work, we explore the transient interactions between trivalent californium ions (Cf 3+ ) and select inorganic radicals arising from the radiolytic decomposition of common anions and functional group constituents, specifically the dichlorine (Cl 2 •- ) and sulfate (SO 4 •- ) radical anions. Chemical kinetics, as measured by integrated electron pulse radiolysis and transient absorption spectroscopy techniques, are presented for the reactions of these two oxidizing radicals with Cf 3+ ions. The derived and ionic strength corrected second-order rate coefficients (k) for these radiation-induced processes are k(Cf 3+ + Cl 2 •- ) = (8.28 ± 0.61) × 10 5 M -1 s -1 and k(Cf 3+ + SO 4 •- ) = (9.50 ± 0.43) × 10 8 M -1 s -1 under ambient temperature conditions (22 ± 1 °C).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Adsorption of Rare Earth Elements onto DNA-Functionalized Mesoporous Carbon

The recovery and separation of rare earth elements (REEs) are of national importance owing to the specific usages, high demand, and low supply of these elements. In this research, we have investigated the adsorption of rare earth elements onto DNA-functionalized mesoporous carbons with a BET surface area of 605 m2/g and a median mesopore width of 48 Å. Additionally, three types of single-stranded DNA, one with 100 base units of thymine, another with 20 units of thymine, and the third, a 2000 unit long DNA from salmon milt were grafted on the carboxylated mesoporous carbon surface. All of the DNA-functionalized mesoporous carbons demonstrated higher adsorption of REEs compared to pristine mesoporous carbon and DNA grafted with 100 units of thymine demonstrated slightly higher adsorbed amounts compared to others. Pure neodymium (Nd(III)) adsorption in the aqueous phase demonstrated an adsorbed amount of 110.4 mg/g with respect to the initial concentration of 500 mg/g. A pH variation study with pure Nd(III) demonstrated that the adsorbed amount is higher at elevated pH compared to that at lower pH, thereby suggesting possible recovery at lower pH. Adsorption of a mixture of 16 REEs, including Sc, Lu, Tm, Yb, Er, Ho, Tb, Dy, Y, Eu, Gd, Sm, Ce, Nd, Pr, and La revealed that the adsorbed amount increased with an increase in the atomic weight and metallic radii of elements within the lanthanides. The calculation of the distribution coefficients for all of the equilibrium adsorption amounts suggested that adsorption is more effective in the lower concentration region. The Nd L3-edge X-ray absorption near edge structure (XANES) confirmed a 3+ oxidation state of Nd in the adsorbed phase. The extended X-ray absorption fine structure (EXAFS) confirmed the local atomic structure relaxation of Nd complexes in the adsorbed phase and shortening of the Nd–O bond distance by about 0.03–0.04 Å, which may be associated with their local complexation at the carbon surface.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Spatiotemporal Observation of Quasi-Ballistic Transport of Electrons in Graphene

We report spatiotemporal observations of room-temperature quasi-ballistic electron transport in graphene, which is achieved by utilizing a four-layer van der Waals heterostructure to generate free charge carriers. The heterostructure is formed by sandwiching a MoS 2 and MoSe 2 heterobilayer between two graphene monolayers. Transient absorption measurements reveal that the electrons and holes separated by the type-II interface between MoS 2 and MoSe 2 can transfer to the two graphene layers, respectively. Transient absorption microscopy measurements, with high spatial and temporal resolution, reveal that while the holes in one graphene layer undergo a classical diffusion process with a large diffusion coefficient of 65 cm 2 s –1 and a charge mobility of 5000 cm 2 V –1 s –1 , the electrons in the other graphene layer exhibit a quasi-ballistic transport feature, with a ballistic transport time of 20 ps and a speed of 22 km s –1 , respectively. The different in-plane transport properties confirm that electrons and holes move independently of each other as charge carriers. Furthermore, the optical generation of ballistic charge carriers suggests potential applications for such van der Waals heterostructures as optoelectronic materials.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
NASA NTRS1988

The use of a helicopter mounted ranging scatterometer for estimation of extinction and scattering properties of forest canopies-II: Experimental results for high-density aspen

An analytic expression is derived that describes the backscatter power from a semi-infinite plane parallel homogeneous canopy as a function of distance from an airborne radar. This model is fitted to observed data for a high-density aspen canopy by a modification of a technique developed by Tyapkin (1960). This inversion of the model provides unbiased estimates of the canopy extinction and backscattering parameters. An active radar calibrator located underneath the canopy provides an independent method of determining the volume extinction coefficient. The results reported indicate that the coefficients change throughout the year. A comparison of these coefficients with Eom and Funk's (1984) disk model, using measured canopy properties, shows that at C-band frequency, only a part of the scattering and absorption can be attributed to the canopy leaves.

Pitts, David E.↗

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