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DOE OSTI2019

ASSESMENT OF IMPURITIES IN NP METAL USING DOUBLE-FOCUSING SF-ICP-MS

In the transmutation process, minor actinides such as neptunium, americium and curium obtained from spent nuclear fuel are incorporated into new fuel that can be placed into a fast reactor, where these elements fission into products with shorter half-lives which reduces the health and safety hazards [1]. In order to better understand the all the involved processes, fundamental physical properties of actinides should be investigated, and for that reason, high-purity materials need to be produced. One of the main challenges in characterizing these materials is the lack of pure metal available for study, and lack of analytical methods to determine the purity. Trans-uranic elements are challenging to study because of the need to be handled in specialized facilities, safeguards concerns and they are not easily purchased and/or produced. High-purity Np metal is being produced at the Materials and Fuels Complex (MFC) of Idaho National Laboratory (INL), in a process of direct oxide reduction developed by Squires and Lessing [2], with a target purity of 99.999%. The goal of this research is to develop methods to determine the impurities in the Np metal, with detection limits low enough to achieve this purity level. In this work, we have used several ICP-MS and ICP OES techniques, but the focus was the method development using a recently acquired Double-Focusing Sector Field Inductively Coupled Plasma Mass Spectrometer (SF-ICP-MS). To produce the Np metal, approximately 20 g of the neptunium oxide powder was calcined at 800 oC for 6 h in a magnesium oxide crucible, which is placed inside a stainless steel crucible, that goes into the Hot Uniaxial Press (HUP) furnace insert. After the calcining step, the Np oxide was mixed with approximately 9 g of calcium metal and 100 g of ultra-dry calcium chloride. The HUP furnace was heated in a ramp rate of 50 oC min -1 up to 1000 oC. When the reaction mixture reached 850 oC, a tantalum stirrer was activated at 100 rpm. After the tantalum stirrer was removed and the mixture cooled overnight, the MgO crucible was opened with a hammer and chisel to retrieve the Np metal button at the bottom of the reaction mixture [2]. Prior to the dissolution process, the surface contaminants of the sample were removed. The Np button was washed in 10 mL of ultra-pure water for 1 min, with a faint reaction observed on the surface, indicating the presence of Ca metal. The water-washed sample was placed in a tube with 2 M HCl for only 3 s, as a vigorous reaction in the button surface was observed. The leachates were saved for further analysis. The sample was then rinsed with ultra-pure water and air-dried prior to dissolution. The cleaned sample was placed in a PTFE beaker and 25 mL of 6 M HCl and 150 µL of 24 M HF were added. After 10 minutes of reaction, the beaker was placed on a hot plate for 1 h and 30 min, followed by the addition of 1 mL of 16 M HNO3 and allowed to react for a further 1 h and 20 min. The sample was removed from heat and 10 mL of HNO3 16 M was added to react with the HCl. The beaker was covered and left for overnight reaction, producing a solution with approximately 20 mL of final volume. A Quadrupole Inductively Coupled Plasma Mass Spectrometer (Q-ICP-MS, Perkin Elmer ELAN DRC II Q-ICP-MS) was used to obtain qualitative mass spectra for the dissolution blank, each of the leachates and the dissolved sample. In the water leachate spectrum mainly Ca and Mg were observed, while the acid wash had a similar peak pattern to the one observed for the Np metal sample, indicating that the process not only removed surface contamination, but also reacted with the sample itself. In the Np material spectrum, Ta and actinides were identified as candidates for major contaminants, as the most intense peaks corresponded to the mass-to-charge ratios of these elements. Minor contaminants included Al, Au, Ca, Cr, Fe, I, Na, Nb, Pb, Sn, Ti, Tl, V, Y. The presence of impurities in the material could have originated from several sources, such as the materials used for the casting process, the use of impure NpO2 or contamination of reagents and materials used for the analysis. Some of the isotopes listed as potential contaminants are susceptible to spectral interferences, so Double-Focusing SF-ICP-MS (Nu Instruments Attom ES HR-ICP-MS) was used for the quantitative analysis. For each isotope determined, several items were evaluated: raw signal of a blank solution, sensitivity and determination coefficient of calibration curves, possibility of interferences and comparison of results obtained for at least two resolving powers (RP): 300 and 4000. The evaluation of the signal in a blank solution can indicate if a spectral interference from the plasma gas and/or the solvent was successfully resolved (commonly observed for 52Cr+/40Ar12C+, for example). It is important to highlight that a signal reduction is expected when a higher RP is used, as the ion beam transmission is decreased by the use of na

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Assessment of Impurities in Neptunium Metal Using Double-Focusing SF-ICP-MS

In the transmutation process, minor actinides such as neptunium, americium and curium obtained from spent nuclear fuel are incorporated into new fuel that can be placed into a fast reactor, where these elements fission into products with shorter half-lives which reduces the health and safety hazards. In order to better understand the all the involved processes, fundamental physical properties of actinides should be investigated, and for that reason, high-purity materials need to be produced. One of the main challenges in characterizing these materials is the lack of pure metal available for study, and lack of analytical methods to determine the purity. Trans-uranic elements are challenging to study because of the need to be handled in specialized facilities, safeguards concerns and they are not easily purchased and/or produced. High-purity Np metal is being produced at the Materials and Fuels Complex (MFC) of Idaho National Laboratory (INL), in a process of direct oxide reduction developed by Squires and Lessing, with a target purity of 99.999%. The goal of this research is to develop methods to determine the impurities in the Np metal, with detection limits low enough to achieve this purity level. In this work, we have used several ICP-MS and ICP OES techniques, but the focus was the method development using a recently acquired Double-Focusing Sector Field Inductively Coupled Plasma Mass Spectrometer (SF-ICP-MS). To produce the Np metal, approximately 20 g of the neptunium oxide powder was calcined at 800 oC for 6 h in a magnesium oxide crucible, which is placed inside a stainless steel crucible, that goes into the Hot Uniaxial Press (HUP) furnace insert. After the calcining step, the Np oxide was mixed with approximately 9 g of calcium metal and 100 g of ultra-dry calcium chloride. The HUP furnace was heated in a ramp rate of 50 oC min -1 up to 1000 oC. When the reaction mixture reached 850 oC, a tantalum stirrer was activated at 100 rpm. After the tantalum stirrer was removed and the mixture cooled overnight, the MgO crucible was opened with a hammer and chisel to retrieve the Np metal button at the bottom of the reaction mixture. Prior to the dissolution process, the surface contaminants of the sample were removed. The Np button was washed in 10 mL of ultra-pure water for 1 min, with a faint reaction observed on the surface, indicating the presence of Ca metal. The water-washed sample was placed in a tube with 2 M HCl for only 3 s, as a vigorous reaction in the button surface was observed. The leachates were saved for further analysis. The sample was then rinsed with ultra-pure water and air-dried prior to dissolution. The cleaned sample was placed in a PTFE beaker and 25 mL of 6 M HCl and 150 µL of 24 M HF were added. After 10 minutes of reaction, the beaker was placed on a hot plate for 1 h and 30 min, followed by the addition of 1 mL of 16 M HNO3 and allowed to react for a further 1 h and 20 min. The sample was removed from heat and 10 mL of HNO3 16 M was added to react with the HCl. The beaker was covered and left for overnight reaction, producing a solution with approximately 20 mL of final volume. A Quadrupole Inductively Coupled Plasma Mass Spectrometer (Q-ICP-MS, Perkin Elmer ELAN DRC II Q-ICP-MS) was used to obtain qualitative mass spectra for the dissolution blank, each of the leachates and the dissolved sample. In the water leachate spectrum mainly Ca and Mg were observed, while the acid wash had a similar peak pattern to the one observed for the Np metal sample, indicating that the process not only removed surface contamination, but also reacted with the sample itself. In the Np material spectrum, Ta and actinides were identified as candidates for major contaminants, as the most intense peaks corresponded to the mass-to-charge ratios of these elements. Minor contaminants included Al, Au, Ca, Cr, Fe, I, Na, Nb, Pb, Sn, Ti, Tl, V, Y. The presence of impurities in the material could have originated from several sources, such as the materials used for the casting process, the use of impure NpO2 or contamination of reagents and materials used for the analysis. Some of the isotopes listed as potential contaminants are susceptible to spectral interferences, so Double-Focusing SF-ICP-MS (Nu Instruments Attom ES HR-ICP-MS) was used for the quantitative analysis. For each isotope determined, several items were evaluated: raw signal of a blank solution, sensitivity and determination coefficient of calibration curves, possibility of interferences and comparison of results obtained for at least two resolving powers (RP): 300 and 4000. The evaluation of the signal in a blank solution can indicate if a spectral interference from the plasma gas and/or the solvent was successfully resolved (commonly observed for 52Cr+/40Ar12C+, for example). It is important to highlight that a signal reduction is expected when a higher RP is used, as the ion beam transmission is decreased by the use of narrower slits

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRSDate not supplied

Transitioning TEMPO Data for Air Quality Management Applications at the NASA SPoRT Center

The TEMPO mission has been observing air pollutants every hour during the daytime across its Field of Regard (FoR) covering greater North America since First Light on August 2, 2023. The highly anticipated public release of TEMPO data occurred on May 20, 2024, consisting of level 2 and level 3 trace gas data products of nitrogen dioxide, formaldehyde, and ozone. The NASA SPoRT Center is developing value-added products and tools to support the TEMPO mission and Early Adopters program with special attention on stakeholder from air agencies. One component of our work is focused on evaluating the TEMPO products over stakeholder target areas using Pandora and surface monitor observations to characterize the uncertainties and develop best practices for processing and analyzing TEMPO data. Methods for oversampling TEMPO data to 1 km resolution are being applied over the target areas to resolve fine-scale emission sources and pollutant gradients. Machine learning techniques using TEMPO, surface monitor, and model data to estimate surface-level nitrogen dioxide concentrations are being developed over the target areas. A SPoRT viewer for TEMPO has been launched for providing visualizations of the TEMPO products and an ArcGIS dashboard is being designed for enabling air agency stakeholders to efficiently analyze TEMPO data. Training materials including user guides are being developed to ensure the effective and sustained use of TEMPO data at our stakeholder agencies. One major goal of our TEMPO initiatives at SPoRT is to better enable the inclusion of TEMPO data in air quality management applications such as exceptional event demonstrations through our close engagement with stakeholders. This talk will provide an update on our SPoRT activities and showcase use cases of TEMPO data for monitoring different emission sources including wildland fire smoke.

Air Quality↗

DOE OSTI2016

Structural and Magnetic Properties of Mn{sub 1−x}Zn{sub x}Fe{sub 2}O{sub 4} Ferrite Nanoparticles

In this work, solid solutions of Mn{sub 1−x}Zn{sub x}Fe{sub 2}O{sub 4} (where x = 0.0, 0.2, 0.4, 0.6, 0.8, and 1.0) ferrite nanoparticles were synthesized using the novel combustion method. A powder X-ray diffraction study confirms the formation of spinel-structured Mn{sub 1−x}Zn{sub x}Fe{sub 2}O{sub 4}. Unusual increases in the lattice constant were observed from 8.358 to 8.435 Å for Zn substitution. Raman spectra show the change in local environment of tetrahedral and octahedral symmetry. Field emission scanning electron microscopy images show that the prepared samples are nanosized and there is not much difference observed in surface morphology. A magnetic study reveals that the prepared samples exhibit superparamagnetic properties with negligible coercivity and the saturation magnetizations initially increase from 31.12 emu g{sup −1} (x = 0) to 35.48 emu g{sup −1} (x = 0.2) and then decrease for further Zn substitution at 300 K. The zero-field-cooled and field-cooled magnetization studies confirm the superparamagnetic nature of prepared samples, and the observed blocking temperature decreases from 146.05 to 32.3 K. At 20 K, the measured hysteresis loop shows the coercivity and it gradually decreases from 810 to 152 Oe. The obtained results suggest that the prepared superparamagnetic Mn{sub 1−x}Zn{sub x}Fe{sub 2}O{sub 4} ferrite nanoparticles are a promising candidate material for biomedical applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS2014

On the Evaluation of Global Sea-Salt Aerosol Models at Coastal/Orographic Sites

Sea-salt aerosol global models are typically evaluated against concentration observations at coastal stations that are unaffected by local surf conditions and thus considered representative of open ocean conditions. Despite recent improvements in sea-salt source functions, studies still show significant model errors in specific regions. Using a multiscale model, we investigated the effect of high model resolution (0.1deg x 0.1deg vs. 1deg x 1.4deg) upon sea-salt patterns in four stations from the University of Miami Network: Baring Head, Chatam Island, and Invercargill in New Zealand, and Marion Island in the sub-antarctic Indian Ocean. Normalized biases improved from +63.7% to +3.3% and correlation increased from 0.52 to 0.84. The representation of sea/land interfaces, mesoscale circulations, and precipitation with the higher resolution model played a major role in the simulation of annual concentration trends. Our results recommend caution when comparing or constraining global models using surface concentration observations from coastal stations.

sea-salt aerosol↗

DOE OSTI2019

Evaluation of the WRF lake module (v1.0) and its improvements at a deep reservoir

Large lakes and reservoirs play important roles in modulating regional hydrological cycles and climate; however, their representations in coupled models remain uncertain. The existing lake module in the Weather Research and Forecasting (WRF) system (hereafter WRF-Lake), although widely used, did not accurately predict temperature profiles in deep lakes mainly due to its poor lake surface property parameterizations and underestimation of heat transfer between lake layers. We therefore revised WRF-Lake by improving its (1) numerical discretization scheme; (2) surface property parameterization; (3) diffusivity parameterization for deep lakes; and (4) convection scheme, the outcome of which became WRF-rLake (i.e., revised lake model). We evaluated the off-line WRF-rLake by comparing simulated and measured water temperature at the Nuozhadu Reservoir, a deep reservoir in southwestern China. WRF-rLake performs better than its predecessor by reducing the root-mean-square error (RMSE) against observed lake surface temperatures (LSTs) from 1.4 to 1.1°C and consistently improving simulated vertical temperature profiles. We also evaluated the sensitivity of simulated water temperature and surface energy fluxes to various modeled lake processes. We found (1) large changes in surface energy balance fluxes (up to 60 W m -2 ) associated with the improved surface property parameterization and (2) that the simulated lake thermal structure depends strongly on the light extinction coefficient and vertical diffusivity. Although currently only evaluated at the Nuozhadu Reservoir, we expect that these model parameterization and structural improvements could be general and therefore recommend further testing at other deep lakes and reservoirs.

58 GEOSCIENCES↗

DOE OSTI2020

Observations Regarding Face Shield Designs Using Commonly Available Materials

A Sandia COVID-19 LDRD effort, the Sandia E-PiPEline Team, systematically evaluated design options for face shields constructed from commonly available materials (CAMs). This study is not focused on face shields for medical applications, and as such, has excluded labeling and flammability considerations suggested by the FDA. Design options for face shields were analyzed with subject matter expert input considering the design's effectiveness (seal around face), reusability (compatibility with solvents, degree of inertness), producibility (ability to obtain materials, build time), cost, and comfort (fit around head, contact surface interface). Observations for the design of face shields using CAMS are provided here.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2016

The effect of inhibitor sodium nitrate on pitting corrosion of dissimilar material weldment joint of stainless steel AISI 304 and mild steel SS 400

This study experimentally evaluated the effect of Sodium Nitrate inhibitor (NaNO{sub 3}) of 0.1%, 0.3%, and 0.5% on NaCl 3.5% toward pitting corrosion of dissimilar metal welding joint between stainless steel AISI 304 and mild steel SS 400. Electrochemical corrosion was tested using potentiodynamic polarization. Further the Scanning Electron Microscope (SEM) conducted to analyze the specimen. Chemical composition analysis used Energy Dispersive X-ray Spectrometry (EDS). The highest efficiency of sodium nitrate for ER 308 attained 63.8% and 64.89%for ER 309L. The specimen surface which observed through SEM showed decrease of pitting corrosion respectively with the addition of sodium nitrate content as inhibitor.

36 MATERIALS SCIENCE↗

NASA NTRS1995

New upper limits on the local metagalactic ionizing radiation density

We have obtained H-alpha observations with the Maryland-Caltech Fabry-Perot Spectrometer attached to the Cassegrain focus of the 1.5 m telescope at Palomer Observatory in order to set limits on the number of ionizing photons from the local metagalactic radiation field. We have observed the SW component of the Haynes-Giovanelli cloud H I 1225+01, an intergalactic cloud which should be optimum for measuring the metagalactic flux because it is nearly opaque to ionizing photons, it does not appear to be significantly shielded from the metagalactic radiation field, and the limits on embedded or nearby ionizing sources are unusually low. For the area of the cloud with an H I column density greater than 10(exp 19)/sq cm we set a 2 sigma limit of 1.1 x 10(exp -19) ergs/sq cm/s/sq arcsec (20 mR) for the surface brightness of diffuse H-alpha. This implies a 2 sigma upper limit on the incident one-sided ionizing flux of Phi(sub ex) is less than 3 x 10(exp 4)/sq cm/s. For a radiation field of the form J(sub nu) is approximately nu(exp -1.4), this yields a firm 2 sigma upper limit on the local metagalactic photoionization rate of Gamma is less than 2 x 10(exp -13)/s, and an upper limit for the radiation field J(sub nu) at the Lyman limit of J(sub nu0) is less than 8 x 10(exp -23) ergs/sq cm/Hz/sr. We discuss previous efforts to constrain the metagalactic ionizing flux using H-alpha surface brightness observations and also other methods, and conclude that our result places the firmest upper limit on this flux. We also observed the 7 min diameter region centered on 3C 273 in which H-alpha emission at a velocity of approximately 1700 km/s was initially reported by Williams and Schommer. In agreement with T. B. Williams (private communication) we find the initial detection was spurious. We obtain a 2 sigma upper limit of 1.8 x 10(exp -19) ergs/sq cm/s/sq arcsec (32 mR) for the mean surface brightness of diffuse H-alpha, about a factor of 6 below the published value.

Vogel, Stuart N.↗

NASA NTRS2019

Quantifying Water Storage Change and Land Subsidence Induced by Reservoir Impoundment Using GRACE, Landsat, and GPS Data

The construction of hydropower dams is a common strategy to support a country's increasing need for electricity and river water management for industry and agriculture. Although the hydrological and geophysical impacts of water relocation are usually assessed prior to impoundment, their accuracy is generally limited due to the lack of in situ observations, especially in a remote area. This study presents a workflow to quantify the terrestrial water storage change (TWS) and land subsidence induced by a reservoir's water impoundment using multiple satellite observations (GRACE, Landsat), land surface models (CABLE, GLDAS, NCEP, ECMWF), and GPS data. The study site is the Bakun Dam, located in Sarawak, Malaysia, which is the largest hydropower dam in Southeast Asia. Commencing operation in late 2010, the dam induced a change of water mass and lake surface area that was clearly observed by GRACE and Landsat observations, respectively. During the 17-month impounding period (from August 2010 to December 2011), GRACE observed a dramatic increase of approximately 200 mm equivalent water height, while Landsat detected an increased lake extent of around 600 km2. In this paper, a forward model is developed to determine the increased water surface level corresponding to GRACE observations, estimated to be about 120 m. In contrast to GRACE, the TWS derived from land surface models cannot capture the increased TWS, due to the lack of reservoir routing algorithms in the models. In addition, the land subsidence was calculated using the disk load model constructed based on the GRACE-derived lake level and Landsat-derived lake extent; the result is validated with the GPS data from BIN1 station, located at the western coast of Borneo. The commencement stage of the Bakun Dam induces the large-scale land subsidence, which causes the GPS-BIN1 station to subside by ~9 mm, and move toward the Bakun Lake by ~4 mm. Computation of the surface displacements directly from GRACE spherical harmonic coefficient data fails to capture the subsidence feature, mainly due to the truncation error. Overall, this study demonstrates that evaluating GRACE in conjunction with Landsat, LSMs, and GPS data allows the exploitation of the gravity signal at a much smaller spatial scale than its intrinsic resolution. Benefiting from global coverage, the newly developed satellite-based algorithm is a valuable tool for assessing the impacts of reservoir operation on hydrological and geophysical changes from local to regional scales.

Natthachet Tangdamrongsub↗

DOE OSTI2016

Ti 3 C 2 T x (MXene)–polyacrylamide nanocomposite films

Polymer nanocomposite films are of great interest due to their enhanced properties over base polymers. By incorporating 2D titanium carbide a representative of a new family of 2D materials, MXenes, as nanofillers into a water soluble polyacrylamide (PAM) matrix, the resulting films benefit from the flexibility, robustness, and processability of PAM, as well as the conductivity and mechanical properties of MXene fillers. We report on manufacturing and characterization of MXene-PAM nanocomposite films. Dimethylsulfoxide (DMSO) intercalation in-between the Ti 3 C 2 -based MXene layers led to full delamination of the MXene layers and hence a uniform dispersion of hydrophilic MXene nanosheets in aqueous PAM solutions was achieved. Moreover, the polymer composite solutions of up to 75 wt.% MXene loading were sonicated and cast onto large Teflon trays and dried at room temperature to produce shiny black films. The observation of reduced 0002 peaks of Ti 3 C 2 T x phase in X-ray diffraction patterns and TEM images indicate the presence of well dispersed nanoflakes. The as-prepared composite films are flexible and the conductivity was increased significantly to 3 x 10 -3 S cm -1 for 6 wt. % MXene-PAM films. With high MXene loading, some non-uniformity between the top and bottom surfaces was observed. This could be due to the segregation of MXene layers in composite films during drying. Finally, the power law dependence of conductivity above the percolation threshold is presented through detailed conductivity measurements.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2023

Theoretical assessments of Pd–PdO phase transformation and its impacts on H 2 O 2 synthesis and decomposition pathways

The direct synthesis of H 2 O 2 from O 2 and H 2 provides a green pathway to produce H 2 O 2 , a popular industrial oxidant. Here, in this study, we theoretically investigate the effects of Pd oxidation states, coordination environments, and particle sizes on primary H 2 O 2 selectivities, assessed by calculating the ratio of rate constants for the formation of H 2 O 2 (via OOH* reduction; k O–H ) and the decomposition of OOH* (via O–O cleavage; k O–O ). For Pd metals, the k O–H /k O–O ratio decreased from 10 -4 for Pd(111) to 10 -10 for the Pd 13 cluster at 300 K, indicating poorer H 2 O 2 selectivity as Pd particle size decreases and low primary selectivities for H 2 O 2 overall. As the oxygen chemical potential increases and metals form surface and bulk oxides, the perturbation of Pd–Pd ensemble sites by lattice O atoms results in selectivities that become dramatically higher than unity. For instance, at 300 K, the k O–H /k O–O ratio increases significantly from 10 -4 to 10 9 to 10 16 as Pd(111) oxidizes to Pd 5 O 4 /Pd(111) and to PdO(100), respectively. In contrast, such selectivity enhancements are not observed for surface and bulk oxides that persistently contain rows of more metallic, undercoordinated Pd–Pd ensemble sites, such as PdO(101)/Pd(100) and PdO(101). These Pd–Pd ensembles are also absent when smaller Pd nanoparticles fully oxidize, indicating that smaller PdO clusters can be more selective for H 2 O 2 synthesis. These trends for primary H 2 O 2 selectivities were found to inversely correlate with trends for H 2 O 2 decomposition rates via O–O bond cleavage, demonstrating that catalysts with high primary H 2 O 2 selectivity can also hinder H 2 O 2 decomposition. Ab initio thermodynamic calculations are used to estimate the thermodynamically favored phase among Pd, PdO/Pd and PdO in O 2 , H 2 O 2 /H 2 O, and O 2 /H 2 environments. These results are combined to show that smaller Pd nanoparticles are more prone to be oxidized at lower oxygen chemical potentials, upon which they become more selective than larger Pd particles for H 2 O 2 synthesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2014

Controlling the number of graphene sheets exfoliated from graphite by designed normal loading and frictional motion

We use molecular dynamics to study the exfoliation of patterned nanometer-sized graphite under various normal loading conditions for friction-induced exfoliation. Using highly ordered pyrolytic graphite (HOPG) as well as both amorphous and crystalline SiO{sub 2} substrate as example systems, we show that the exfoliation process is attributed to the corrugation of the HOPG surface and the atomistic roughness of the substrate when they contact under normal loading. The critical normal strain, at which the exfoliation occurs, is higher on a crystalline substrate than on an amorphous substrate. This effect is related to the atomistic flatness and stiffness of the crystalline surface. We observe that an increase of the van der Waals interaction between the graphite and the substrate results in a decrease of the critical normal strain for exfoliation. We find that the magnitude of the normal strain can effectively control the number of exfoliated graphene layers. This mechanism suggests a promising approach of applying designed normal loading while sliding to pattern controlled number of graphene layers or other two-dimensional materials on a substrate surface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS2007

The Global Precipitation Climatology Project (GPCP): Results, Status and Future

The Global Precipitation Climatology Project (GPCP) is one of a number of long-term, satellite-based, global analyses routinely produced under the auspices of the World Climate Research Program (WCRP) and its Global Energy and Watercycle EXperiment (GEWEX) program. The research quality analyses are produced a few months after real-time through the efforts of scientists at various national agencies and universities in the U.S., Europe and Japan. The primary product is a monthly analysis of surface precipitation that is globally complete and spans the period 1979-present. There are also pentad analyses for the same period and a daily analysis for the 1997-present period. Although generated with somewhat different data sets and analysis schemes, the pentad and daily data sets are forced to agree with the primary monthly analysis on a grid box by grid box basis. The primary input data sets are from low-orbit passive microwave observations, geostationary infrared observations and surface raingauge information. Examples of research with the data sets are discussed, focusing on tropical (25N-25s) rainfall variations and possible long-term changes in the 28-year (1979-2006) monthly dataset. Techniques are used to discriminate among the variations due to ENSO, volcanic events and possible long-term changes for rainfall over both land and ocean. The impact of the two major volcanic eruptions over the past 25 years is estimated to be about a 5% maximum reduction in tropical rainfall during each event. Although the global change of precipitation in the data set is near zero, a small upward linear change over tropical ocean (0.06 mm/day/l0yr) and a slight downward linear change over tropical land (-0.03 mm/day/l0yr) are examined to understand the impact of the inhomogeneity in the data record and the length of the data set. These positive changes correspond to about a 5% increase (ocean) and 3% increase (ocean plus land) during this time period. Relations between variations in surface temperature and precipitation are analyzed on seasonal to inter-decadal time scales. A new, version 3 of GPCP is being planned to incorporate new satellite information (e.g., TRMM) and provide higher spatial and temporal resolution for at least part of the data record. The goals and plans for that GPCP re-processing will be outlined.

Adler, Robert F.↗

NASA NTRS2011

Retrospective Analog Year Analyses Using NASA Satellite Data to Improve USDA's World Agricultural Supply and Demand Estimates

The USDA World Agricultural Outlook Board (WAOB) is responsible for monitoring weather and climate impacts on domestic and foreign crop development. One of WAOB's primary goals is to determine the net cumulative effect of weather and climate anomalies on final crop yields. To this end, a broad array of information is consulted, including maps, charts, and time series of recent weather, climate, and crop observations; numerical output from weather and crop models; and reports from the press, USDA attach s, and foreign governments. The resulting agricultural weather assessments are published in the Weekly Weather and Crop Bulletin, to keep farmers, policy makers, and commercial agricultural interests informed of weather and climate impacts on agriculture. Because both the amount and timing of precipitation significantly affect crop yields, WAOB often uses precipitation time series to identify growing seasons with similar weather patterns and help estimate crop yields for the current growing season, based on observed yields in analog years. Historically, these analog years are visually identified; however, the qualitative nature of this method sometimes precludes the definitive identification of the best analog year. Thus, one goal of this study is to derive a more rigorous, statistical approach for identifying analog years, based on a modified coefficient of determination, termed the analog index (AI). A second goal is to compare the performance of AI for time series derived from surface-based observations vs. satellite-based measurements (NASA TRMM and other data).

Teng, William↗

DOE OSTI2020

Tuning Fermi Levels in Intrinsic Antiferromagnetic Topological Insulators MnBi 2 Te 4 and MnBi 4 Te 7 by Defect Engineering and Chemical Doping

MnBi 2 Te 4 and MnBi 4 Te 7 are intrinsic antiferromagnetic topological insulators, offering a promising materials platform for realizing exotic topological quantum states. However, high densities of intrinsic defects in these materials not only cause bulk metallic conductivity, preventing the measurement of quantum transport in surface states, but may also affect magnetism and topological properties. In this paper, systematic density functional theory calculations reveal specific material chemistry and growth conditions that determine the defect formation and dopant incorporation in MnBi 2 Te 4 and MnBi 4 Te 7 . The large strain induced by the internal heterostructure promotes the formation of large-size-mismatched antisite defects and substitutional dopants. The results here show that the abundance of antisite defects is responsible for the observed n-type metallic conductivity. Additionally, a Te-rich growth condition is predicted to reduce the bulk free electron density, which is confirmed by experimental synthesis and transport measurements in MnBi 2 Te 4 . Furthermore, Na doping is proposed to be an effective acceptor dopant to pin the Fermi level within the bulk band gap to enable the observation of surface quantum transport. The defect engineering and doping strategies proposed here should stimulate further studies for improving synthesis and for manipulating magnetic and topological properties in MnBi 2 Te 4 , MnBi 4 Te 7 , and related magnetic topological insulators.

36 MATERIALS SCIENCE↗

NASA NTRS2018

Multidecadal Changes in Lower Stratospheric Ozone: Variability Vs. Trends

As upper stratospheric ozone appears to be recovering as a result of decreasing chlorine loading following the implementation of the Montreal Protocol and its amendments and in agreement with model projections, several recent studies report an apparent decline of ozone concentrations in the lower stratosphere in the last two decades, particularly in the extratropics. Our previous work as well as at least two other studies provide evidence that this decline results from transport changes rather than an intensification of chemical depletion. It remains unclear whether these changes represent long-term internal variability or are a consequence of a climate forcing. Here we perform free-running ensembles of the recent past (1980-2016) using the Goddard Earth Observing System Model (GEOS) at the cubed sphere C180 (approximately half degree) resolution. Two suites of 10-member ensembles are performed, one in which observed sea surface temperature (SSTs) are fully prescribed, and the other in which the linear SST trend over the recent past is removed so as to only retain internal variability. We evaluate the trends in both ozone as well as two idealized tracers with prescribed uniform loss that are used to isolate the role of transport from chemistry and emissions. Probability-distribution-functions of the trends in both ozone and idealized tracers are compared among ensemble members and with observed trends in order to evaluate the likelihood of recent observed declines in lower stratospheric ozone, relative to large internal variability. Moreover, comparisons among simulations with and without imposed SST trends indicate the extent to which dynamically-driven ozone trends reflect forced trends or internal variability in lower stratospheric dynamics.

Wargan, Krzysztof↗

NASA NTRS1987

4-D display of satellite cloud images

A technique has been developed to display GOES satellite cloud images in perspective over a topographical map. Cloud heights are estimated using temperatures from an infrared (IR) satellite image, surface temperature observations, and a climatological model of vertical temperature profiles. Cloud levels are discriminated from each other and from the ground using a pattern recognition algorithm based on the brightness variance technique of Coakley and Bretherton. The cloud regions found by the pattern recognizer are rendered in three-dimensional perspective over a topographical map by an efficient remap of the visible image. The visible shades are mixed with an artificial shade based on the geometry of the cloud-top surface, in order to enhance the texture of the cloud top.

Hibbard, William L.↗