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At least 415 records · Page 23

Perspective: Maintaining surface-phase purity is key to efficient open air fabricated cuprous oxide solar cells

Electrochemically deposited Cu{sub 2}O solar cells are receiving growing attention owing to a recent doubling in efficiency. This was enabled by the controlled chemical environment used in depositing doped ZnO layers by atomic layer deposition, which is not well suited to large-scale industrial production. While open air fabrication with atmospheric pressure spatial atomic layer deposition overcomes this limitation, we find that this approach is limited by an inability to remove the detrimental CuO layer that forms on the Cu{sub 2}O surface. Herein, we propose strategies for achieving efficiencies in atmospherically processed cells that are equivalent to the high values achieved in vacuum processed cells.

36 MATERIALS SCIENCE↗

Selective deposition of a crystalline Si film by a chemical sputtering process in a high pressure hydrogen plasma

The selective deposition of Si films was demonstrated using a chemical sputtering process induced by a high pressure hydrogen plasma at 52.6 kPa (400 Torr). In this chemical sputtering process, the initial deposition rate (R{sub d}) is dependent upon the substrate type. At the initial stage of Si film formation, R{sub d} on glass substrates increased with elapsed time and reached to a constant value. In contrast, R{sub d} on Si substrates remained constant during the deposition. The selective deposition of Si films can be achieved by adjusting the substrate temperature (T{sub sub}) and hydrogen concentration (C{sub H2}) in the process atmosphere. For any given deposition time, it was found that an optimum C{sub H2} exists for a given T{sub sub} to realize the selective deposition of a Si film, and the optimum T{sub sub} value tends to increase with decreasing C{sub H2}. According to electron diffraction patterns obtained from the samples, the selectively prepared Si films showed epitaxial-like growth, although the Si films contained many defects. It was revealed by Raman scattering spectroscopy that some of the defects in the Si films were platelet defects induced by excess hydrogen incorporated during Si film formation. Raman spectrum also suggested that Si related radicals (SiH{sub 2}, SiH, Si) with high reactivity contribute to the Si film formation. Simple model was derived as the guideline for achieving the selective growth.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Detecting outliers in streaming time series data from ARM distributed sensors

The Atmospheric Radiation Measurement (ARM) Data Center at ORNL collects data from a number of permanent and mobile facilities around the globe. The data is then ingested to create high level scientific products. High frequency streaming measurements from sensors and radar instruments at ARM sites require high degree of accuracy to enable rigorous study of atmospheric processes. Outliers in collected data are common due to instrument failure or extreme weather events. Thus, it is critical to identify and flag them. We employed multiple univariate, multivariate and time series techniques for outlier detection methods and studied their effectiveness. First, we examined Pearson correlation coefficient which is used to measure the pairwise correlations between variables. Singular Spectrum Analysis (SSA) was applied to detect outliers by removing the anticipated annual and seasonal cycles from the signal to accentuate anomalies. K-means was applied for multivariate examination of data from collection of sensors to identify any deviation from expected and known patterns and identify abnormal observation. The Pearson correlation coefficient, SSA and K-means methods were later combined together in a framework to detect outliers through a range of checks. We applied the developed method to data from meteorological sensors at ARM Southern Great Plains site and validated against existing database of known data quality issues.

Lu, Yuping↗

Application of automated iterative target detection for standoff hyperspectral imaging

The utility of hyperspectral imaging (HSI) has been well established for a wide array of applications but has generated a need for automated screening of high volumes of large HSI cubes. We report two important automated algorithms for more efficient standoff processing: atmospheric correction and target detection. The atmospheric correction method is based on a fast asymmetric least squares approach that is applied on a pixel-by-pixel basis. Here, the correction can be applied to entire images without manually identifying regions of interest and utilizes only in-scene information, no ancillary modeling of the atmosphere is required. An iterative target detection approach is also introduced which demonstrates faster speeds relative to moving window approaches. The target detection algorithm classifies each pixel as true target detections, near target detections, clutter, and no-calls. The algorithms were tested on forty images of twenty-two solid mineral targets placed at a 14-meter standoff distance allowing general observations on expected detection performance for a variety of minerals. In addition to identifying anomalous pixels, the inclusion of “no-calls” reduced the number of false detections significantly.

47 OTHER INSTRUMENTATION↗

Direct observation of anisotropic growth of water films on minerals driven by defects and surface tension

Knowledge of the occurrences of water films on minerals is critical for global biogeochemical and atmospheric processes, including element cycling and ice nucleation. The underlying mechanisms controlling water film growth are, however, misunderstood. Using infrared nanospectroscopy, amplitude-modulated atomic force microscopy, and molecular simulations, we show how water films grow from water vapor on hydrophilic mineral nanoparticles. We imaged films with up to four water layers that grow anisotropically over a single face. Growth usually begins from the near edges of a face where defects preferentially capture water vapor. Thicker films produced by condensation cooling completely engulf nanoparticles and form thicker menisci over defects. The high surface tension of water smooths film surfaces and produces films of inhomogeneous thickness. Nanoscale topography and film surface energy thereby control anisotropic distributions and thicknesses of water films on hydrophilic mineral nanoparticles.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Analysis of the dependence of surfatron acceleration of electrons by an electromagnetic wave in space plasma on the particle momentum along the wave front

Based on the numerical solution of the nonlinear nonstationary second-order equation for the wave phase on the particle trajectory, the dynamics of surfatron acceleration of electrons by an electromagnetic wave propagating across the external magnetic field in space plasma is analyzed as a function of the electron momentum along the wave front. Numerical calculations show that, for strongly relativistic initial values of the electron momentum component along the wave front g{sub y}(0) (the other parameters of the problem being the same), electrons are trapped into the regime of ultrarelativistic surfatron acceleration within a certain interval of the initial wave phase Ψ(0) on the particle trajectory. It is assumed in the calculations that vertical bar Ψ(0) vertical bar ≤ π. For strongly relativistic values of g{sub y}(0), electrons are immediately trapped by the wave for 19% of the initial values of the phase Ψ(0) (favorable phases). For the rest of the values of Ψ(0), trapping does not occur even at long times. This circumstance substantially simplifies estimations of the wave damping due to particle acceleration in subsequent calculations. The dynamics of the relativistic factor and the components of the electron velocity and momentum under surfatron acceleration is also analyzed. The obtained results are of interest for the development of modern concepts of possible mechanisms of generation of ultrarelativistic particle fluxes in relatively calm space plasma, as well as for correct interpretation of observational data on the fluxes of such particles and explanation of possible reasons for the deviation of ultrarelativistic particle spectra detected in the heliosphere from the standard power-law scalings and the relation of these variations to space weather and large-scale atmospheric processes similar to tropical cyclones.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

HIGRAD/FIRETEC

This is the public-facing repository for the LANL-developed and maintained HIGRAD/FIRETEC software, a CFD software designed to simulate the coupled fire-atmospheric processes at a landscape-scale of resolution. Distribution is possible under OSS license O5086.

Josephson, Alexander [Los Alamos National Laborato↗

Characterizing the Spatial Scales of Extreme Daily Precipitation in the United States

The spatial extent of an extreme precipitation event can be important for a basin’s hydrologic response and subsequent flood risk, and may yield insights into underlying atmospheric processes. Using a relaxed moving-neighborhood approach, we develop indicator semivariograms based on precipitation records from the Global Historical Climatology Network–Daily (GHCN-D) station network to directly quantify the climatological length scales of extreme daily precipitation over the United States during 1965–2014. We find that the length scales of extreme (90th percentile) daily precipitation events vary both regionally and seasonally. Over the eastern half of the United States, daily extreme precipitation length scales reach 400 km during the winter months, but are approximately half as large during the summer months. The Northwest region, on the other hand, exhibits little seasonal variation, with extreme precipitation length scales of approximately 150 km throughout the year. By leveraging in situ station measurements, our study avoids some of the uncertainties associated with satellite or interpolated precipitation data, and provides the longest climatological assessment of length scales of extreme daily precipitation over the United States to date. Although the length scales that we calculate can be sensitive to station density, neighborhood size, and neighborhood relaxation, we find that the interregional and interseasonal differences in length scales are relatively robust. Our method could be extended to quantify changes in the spatial extent of extreme daily precipitation in the recent past, and to investigate the underlying causes of any changes that are detected.

Touma, Danielle↗

The Dependence of Mean Climate State on Shortwave Absorption by Water Vapor

Abstract State-of-the-art climate models exhibit significant spread in the climatological value of atmospheric shortwave absorption (SWA). This study investigates both the possible causes and climatic impacts of this SWA intermodel spread. The intermodel spread of global-mean SWA largely originates from the intermodel difference in water vapor shortwave absorptivity. Hence, we alter the water vapor shortwave absorptivity in the Community Earth System Model, version 1, with the Community Atmosphere Model, version 4 (CESM1-CAM4). Increasing the water vapor shortwave absorptivity leads to a reduction in global-mean precipitation and a La Niña–like cooling over the tropical Pacific. The global-mean atmospheric energy budget suggests that the precipitation is suppressed as a way to compensate for the increased SWA. The precipitation reduction is driven by the weakened surface winds, stabilized planetary boundary layer, and surface cooling. The La Niña–like cooling over the tropical Pacific is attributed to the zonal asymmetry of climatological evaporative damping efficiency and the low cloud enhancement over the eastern basin. Complementary fixed SSTs simulations suggest that the latter is more fundamental and that it primarily arises from atmospheric processes. Consistent with our experiments, the CMIP5/6 models with a higher global-mean SWA tend to produce tropical Pacific toward a more La Niña–like mean state, highlighting the possible role of water vapor shortwave absorptivity for shaping the mean-state climate patterns.

Kim, Hanjun↗

Satellite Sounder Observations of Contrasting Tropospheric Moisture Transport Regimes: Saharan Air Layers, Hadley Cells, and Atmospheric Rivers

This paper examines the performance of satellite sounder atmospheric vertical moisture proles (AVMP) under tropospheric conditions encompassing moisture contrasts driven by convection and advection transport mechanisms, specifically Atlantic Ocean Saharan air layers (SALs) and Pacific Ocean moisture conveyer belts (MCBs) commonly referred to as atmospheric rivers (ARs), both of these being mesoscale to synoptic meteorological phenomena within the vicinity of subtropical Hadley subsidence zones. Operational AVMP environmental data records retrieved from the Suomi National Polar-orbiting Partnership (SNPP) NOAA-Unique Combined Atmospheric Processing System (NUCAPS) are collocated with dedicated radiosonde observations (RAOBs) obtained from ocean-based intensive field campaigns; these RAOBs provide uniquely independent correlative truth data not assimilated into numerical weather prediction models for satellite sounder validation over open ocean. Using these marine-based data, we empirically assess the performance of the operational NUCAPS AVMP product for detecting and resolving these tropospheric moisture features over otherwise RAOB-sparse regions.

54 ENVIRONMENTAL SCIENCES↗

Assessing Adaptive Mesh Refinement (AMR) in a Forced Shallow-Water Model with Moisture

Two forced shallow-water flow scenarios are explored in a 2D fourth-order finite-volume dynamical core with adaptive mesh refinement (AMR) to investigate AMR’s ability to track and resolve complex evolving features. Traditional shallow-water test cases are mainly characterized by large-scale smooth flows that do not effectively test the multiscale abilities of variable-resolution and AMR models to resolve sharp gradients and small-scale flow filaments. Therefore, adding forcing mechanisms to the shallow-water system to model key atmospheric processes adds complexity and creates small-scale phenomena. These can serve as foci for dynamic grid refinement while remaining simple enough to study the numerical design of a model’s dynamical core. The first shallow-water flow scenario represents a strengthening, tropical cyclone–like, vortex that is driven by a Betts–Miller-like convection scheme. The second shallow-water test is built upon a barotropically unstable jet with an added Kessler-like warm rain scheme that leads to precipitating frontal zones. The key feature of both tests is that there is significant sensitivity to the model grid while converging (structurally) at high resolution. Both test cases are investigated for a series of uniform resolutions and a variety of AMR tagging criteria. The AMR simulations demonstrate that grid refinement can resolve local features without requiring global high-resolution meshes. However, the results are sensitive to the refinement criteria. Criteria that trigger refinement early in a simulation reproduce the uniform-resolution reference solutions most reliably. Finally, in contrast, AMR criteria that delay refinement for several days require careful tuning of the AMR thresholds to improve results compared with uniform-resolution simulations.

54 ENVIRONMENTAL SCIENCES↗

Assimilation of a Coordinated Fleet of Uncrewed Aircraft System Observations in Complex Terrain: EnKF System Design and Preliminary Assessment

Abstract Uncrewed aircraft system (UAS) observations collected during the 2018 Lower Atmospheric Process Studies at Elevation—a Remotely Piloted Aircraft Team Experiment (LAPSE-RATE) field campaign were assimilated into a high-resolution configuration of the Weather Research and Forecasting Model using an ensemble Kalman filter. The benefit of UAS observations was assessed for a terrain-driven (drainage and upvalley) flow event that occurred within Colorado’s San Luis Valley (SLV) using independent observations. The analysis and prediction of the strength, depth, and horizontal extent of drainage flow from the Saguache Canyon and the subsequent transition to upvalley and up-canyon flow were improved relative to that obtained both without data assimilation (benchmark) and when only surface observations were assimilated. Assimilation of UAS observations greatly improved the analyses of vertical variations in temperature, relative humidity, and winds at multiple locations in the northern portion of the SLV, with reductions in both bias and the root-mean-square error of roughly 40% for each variable relative to the benchmark run. Despite these noted improvements, some biases remain that were tied to measurement error and/or the impact of the boundary layer parameterization on vertically spreading the observations, both of which require further exploration. The results presented here highlight how observations obtained with a fleet of profiling UAS improve limited-area, high-resolution analyses and short-term forecasts in complex terrain.

54 ENVIRONMENTAL SCIENCES↗

Persistent, “Mysterious” Seismoacoustic Signals Reported in Oklahoma State during 2019

Here, we report on the source of seismoacoustic pulses that were observed across the state of Oklahoma (OK) during summer of 2019, and the subject of national media coverage and speculation. Seismic network data collected across four U.S. states and interviews with witnesses to the pulse’s effect on residential structures demonstrate that they were triggered by routine ammunition disposal operations conducted by McAlester Army Ammunition Plant (McAAP). During these operations, conventional explosives destroy obsolete munitions stored in pits through a controlled sequence of electronically timed shots that occur over tens of minutes. Despite noise-abatement efforts that reduce coupling of acoustic energy with air, some lower frequency, subaudible (infrasonic) sound radiates from these shots as discrete pulses. We use nine months of blast log documents, seismic network records, analyst picks, and physical modeling to demonstrate that seismic stations as far as 640 km from McAAP sample these pulses, which record seasonal patterns in stratospheric and tropospheric winds, as well as the dynamic formation of waveguides and shadow zones. Digital short-term average to long-term average detectors that we augment with dynamic thresholds and time-binning operations identify these pulses with a fair probability, when compared with visual observations. Our analyses thereby provide estimates of observation rates for both partial and full sequences of these pulses, as well as single shots. We suggest that disposal operations can exploit existing, composite seismic networks to predict where residents are likely to witness blasting. Crucially, our data also show that dense seismic networks can record multiscale atmospheric processes in the absence of infrasound arrays.

58 GEOSCIENCES↗

Improving the Representation of Soluble Iron in Climate Models

Mineral dust produced in the arid and semi-arid regions of the world is the dominant source of iron (Fe) in atmospheric aerosol inputs to the open ocean. The bioavailable Fe fraction of atmospheric dust is thought to regulate and occasionally limit the primary productivity in large oceanic regions, which influences the CO2 uptake from the atmosphere affecting the Earth’s climate. Because Fe bioavailability cannot be directly measured, it is assumed that the dissolved Fe or highly reactive Fe in the dust is bioavailable. The fraction of soluble Fe in dust is mainly controlled by: (1) the mineral composition of the soils and the emitted dust from the source areas; (2) the atmospheric processing that converts the Fe in Fe-bearing minerals into highly soluble forms of Fe. The project has mainly focused on constraining the mineral composition of dust aerosols (1), a previously neglected, yet a key issue to constrain the deposition of soluble iron. Deriving aerosol mineral composition requires global knowledge of the soil mineral content, which is available from poorly constrained global atlases. In addition, the mineral content of the emitted aerosol differs from that of the parent soil. Measurements of soil mineral fractions are based upon wet sedimentation (or ’wet sieving’) techniques that disturb the soil sample, breaking aggregates that are found in the original, undispersed soil that is subject to wind erosion. Wet sieving alters the soil size distribution, replacing aggregates that are potentially mobilized as aerosols with a collection of smaller particles. A major challenge is to derive the size-distributed mineral fractions of the emitted dust based upon their fractions measured from wet-sieved soils. Finally, representations of dust mineral composition need to account for mixtures of minerals. Examination of individual particles shows that iron, an element that is central to many climate processes, is often found as trace impurities of iron oxide attached to aggregates of other minerals. This is another challenge that has been tackled by the project. The project has produced a major step forward on our understanding of the key processes needed to predict the mineral composition of dust aerosols by connecting theory, modeling and observations. The project has produced novel semi-empirical and theoretical methods to estimate the emitted size distribution and mineral composition of dust aerosols. These methods account for soil aggregates that are potentially emitted from the original undisturbed soil but are destroyed during wet sieving. The methods construct the emitted size distribution of individual minerals building upon brittle fragmentation theory, reconstructions of wet-sieved soil mineral size distributions, and/or characteristic mineral size distributions estimated from observations at times of high concentration. Based on an unprecedented evaluation with a new global compilation of observations produced with the project support, we showed that the new methods remedy some key deficiencies compared to the previous state-of-the-art. This includes the correct representation of Fe-bearing phyllosilicates at silt sizes, where they are abundant according to observations. In addition, the quartz fraction of silt particles is in better agreement with measured values. In addition, we represent an additional class of iron oxide aerosol that is a small impurity embedded within other minerals, allowing it to travel farther than in its pure crystalline state. We assume that these impurities are least frequent in soils rich in iron oxides (as a result of the assumed effect of weathering that creates pure iron oxide crystals). The mineral composition of dust is also important to other interaction with climate - through shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, and the heterogeneous formation of sulfates and nitrates - and to its impacts upon human health. Despite the importance of mineral composition, models have typically assumed that soil dust aerosols have globally uniform composition. The results of this project will allow an improved estimation of the dust effects upon climate and health.

54 ENVIRONMENTAL SCIENCES↗

Earth System Model Improvement Pipeline via Uncertainty Attribution and Active Learning

Primary focal area: 2 (Predictive Modeling via AI): We develop methods to formally quantify uncertainties in Earth System models for the land-atmosphere coupled system. Science Challenge: Earth system models still have significant biases in historical predictions of the intensity and frequency of water cycling extremes (e.g., droughts and flood events), leading to low confidence in future projections. Uncertainties arise from incomplete understanding of land and atmospheric processes, and insufficient observational constraints on model parameters. Many observations, including those from key DOE investments such as ARM and AmeriFlux, are used to evaluate model performance but have not been used to formally quantify model uncertainty because of the expense of running ESM simulations. An efficient pipeline engaging cutting-edge machine learning (ML) and uncertainty quantification (UQ) methods is needed to improve the predictive understanding of water cycle extremes in the Earth system.

54 ENVIRONMENTAL SCIENCES↗

Semi-automated Design of Artificial Intelligence Earth Systems Models

Prediction and observation of water cycles at various scales involve not only patterns isolated in space and time, but also modeling of complex spatio-temporal relationships across multiple domains. For instance, evapotranspiration (ET) and leaf area indexes (LAI) are two parameters that are needed to accurately model and understand land-atmosphere processes. Accurate assessments of ET and LAI are critical for understanding hydrological processes, deforestation, crop yield, and irrigation impacts. However, ET estimates for global simulations are available at very coarse spatial resolution. They are usually derived from satellite data based on broad plant functional types (PFTs), which fail to capture fine-scale variations because of changes in vegetation type across the globe. Similarly LAI estimates have typically been derived from vegetation indices at global scales or estimated locally using physical models, both of which suffer from a range of uncertainties that impact model sensitivity. The new era of AI model development for Earth systems (ES) calls for data-driven methods that provide domain scientists with uncertainty-aware estimations of biophysical parameters such as ET and LAI in a generalizable, interpretable, and discoverable manner.

54 ENVIRONMENTAL SCIENCES↗

The Usage of Observing System Simulation Experiments and Reinforcement Learning to Optimize Experimental Design and Operation

Various organizations regularly conduct field campaigns across the globe designed to probe and improve atmospheric process understanding. However, these campaigns are mostly designed ad-hoc, and rely on anecdotes and knowledge of what was successful in previous campaigns. Such ad-hoc experiment design results in sub-optimal instrument siting and operation strategies. Inadequate targeted data collection of extreme weather is a major limitation to Earth and Environmental Systems Science Division (EESSD)’s goals of data model integration (4.5.3), which limits the knowledge gained through the collected observations, holding back significant advances in predictability. While advances in instrument design are always chipping away at these limitations, we are not optimally utilizing the instrumentation we currently possess.

54 ENVIRONMENTAL SCIENCES↗

LDRD 2022 Annual Report: Laboratory Directed Research and Development Program Activities

Each year, Brookhaven National Laboratory (BNL) is required to provide a report of its completed Laboratory Directed Research and Development Program (LDRD) projects to the Department of Energy (DOE) Office of Scientific and Technical Information in accordance with DOE Order 413.2C Chg1 (MinChg) dated August 2, 2018. This report provides a detailed look at the scientific and technical activities for each of the LDRD projects funded by BNL in FY 2022, in fulfillment of that requirement. In FY 2022, the BNL LDRD Program funded 70 projects, 30 of which were new starts, at a total cost of $17.2M. The investments that BNL makes in its LDRD program support the Laboratory’s strategic goals. BNL has identified seven scientific initiatives that define the Laboratory’s scientific future and that will enable it to realize its overall vision. This requires simultaneous excellence in all aspects of BNL’s work – from science and operations, to external partnerships with the local, state, and national communities, and beyond. This is enabled by safe, efficient, and secure operations; by an unwavering commitment to a diverse, equitable, and inclusive environment, including workforce development, both with staff and reaching out to the community; and by a strong focus on renewed infrastructure. The seven scientific initiatives are: 1) Nuclear Physics: uncover the structure of visible matter by constructing and operating the Electron-Ion Collider at BNL to maintain international leadership in nuclear physics for decades; 2) Clean Energy and Climate: support a net-zero U.S. economy through fundamental research in basic energy and climate sciences to revolutionize grid-scale storage, renewable integration, and the study of atmospheric processes with a new facility to improve climate predictability; 3) Quantum Information Science and Technology: discover new quantum materials to enhance quantum computers and develop an entanglement sharing quantum network as a prototype for the first quantum internet; 4) Discovery Science Driven by the Human-AI Facility Integration: revolutionize the operation of experiments across the sciences at user facilities and in core programs; 5) High Energy Physics: understand the origin of space and time with the ATLAS high luminosity upgrade at CERN and the future Long Baseline Neutrino Facility/Deep Underground Neutrino Experiment; 6) Isotope Production: accelerate and expand isotope production to ensure the security of the Nation’s supply; 7) Accelerator Science and Technology: harness the cross-cutting accelerator science expertise at BNL to develop new facilities, improve and expand its user facilities, and promote the use of accelerators in industry. The funded projects support BNL’s seven scientific initiatives and priority programs as well as new areas of research and competencies at the Laboratory that are consistent with the Laboratory’s vision and mission. In total, these LDRD investments supported 43 postdoctoral researchers in whole or in part and resulted in 138 publications and 7 awards. This Program Activities Report represents the future of BNL science; it is an impressive body of exploratory work that investigates many scientific and technical directions in support of the DOE and BNL missions.

99 GENERAL AND MISCELLANEOUS↗