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DOE OSTI2013

Temporal Variability of Aerosol Properties during TCAP: Impact on Radiative Forcing

Ground-based remote sensing and in situ observations of aerosol microphysical and optical properties have been collected during summertime (June-August, 2012) as part of the Two-Column Aerosol Project (TCAP; http://campaign.arm.gov/tcap/), which was supported by the U.S. Department of Energy’s (DOE’s) Atmospheric Radiation Measurement (ARM) Program (http://www.arm.gov/). The overall goal of the TCAP field campaign is to study the evolution of optical and microphysical properties of atmospheric aerosol transported from North America to the Atlantic and their impact on the radiation energy budget. During TCAP, the ground-based ARM Mobile Facility (AMF) was deployed on Cape Cod, an arm-shaped peninsula situated on the easternmost portion of Massachusetts (along the east coast of the United States) and that is generally downwind of large metropolitan areas. The AMF site was equipped with numerous instruments for sampling aerosol, cloud and radiative properties, including a Multi-Filter Rotating Shadowband Radiometer (MFRSR), a Scanning Mobility Particle Sizer (SMPS), an Aerodynamic Particle Sizer (APS), and a three-wavelength nephelometer. In this study we present an analysis of diurnal and day-to-day variability of the column and near-surface aerosol properties obtained from remote sensing (MFRSR data) and ground-based in situ measurements (SMPS, APS, and nephelometer data). In particular, we show that the observed diurnal variability of the MFRSR aerosol optical depth is strong and comparable with that obtained previously from the AERONET climatology in Mexico City, which has a larger aerosol loading. Moreover, we illustrate how the variability of aerosol properties impacts the direct aerosol radiative forcing at different time scales.

aerosol microphysical and optical properties↗

DOE OSTI2025

Spatial and Temporal Variability of Vertical Velocity under Shallow Cumulus

Vertical velocity distribution below cloud is one of the key determinants of cloud life cycle, but observations of this variable are extremely sparse in space. Doppler lidar retrievals and large-eddy simulations at the U.S. Department of Energy’s Atmospheric Radiation Measurement User Facility Southern Great Plains site are used to determine whether vertical velocity statistics from temporally dense profiles at a single location can be substituted for spatial vertical velocity statistics. We show that even a small number (five) of widely distributed [ O (1°) latitude/longitude spacing] lidars is sufficient sampling to reconstruct domainwide spatial vertical velocity variance, but not higher moments of the vertical velocity distribution. Spatial and temporal vertical velocity variances in the Doppler lidar observations are nearly interchangeable as long as the spatial variance is temporally averaged and the temporal variance is averaged across lidars. This is true even though the dominant spatial scales of vertical velocity variability are ≲ 3 km, more than an order of magnitude smaller than the spacing between the lidars. Further, in the limit where the temporal variance does not vary across a spatial domain (e.g., if the meteorological and surface forcing of the atmospheric turbulence is homogeneous across the domain) and the domain-mean vertical velocity is zero, the commonly available retrieval of temporal vertical velocity variance at one site is equivalent to the spatial variance over the domain. We use an updraft parcel model to show that substituting temporal for spatial vertical velocity statistics will have a relatively minor effect on cloud droplet number concentrations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Limitations of Bin and Bulk Microphysics in Reproducing the Observed Spatial Structure of Light Precipitation

Abstract Coarse-gridded atmospheric models often account for subgrid-scale variability by specifying probability distribution functions (PDFs) of process rate inputs such as cloud and rainwater mixing ratios ( q c and q r , respectively). PDF parameters can be obtained from numerous sources: in situ observations, ground- or space-based remote sensing, or fine-scale modeling such as large-eddy simulation (LES). LES is appealing to constrain PDFs because it generates large sample sizes, can simulate a variety of cloud regimes/case studies, and is not subject to the ambiguities of observations. However, despite the appeal of using model output for parameterization development, it has not been demonstrated that LES satisfactorily reproduces the observed spatial structure of microphysical fields. In this study, the structure of observed and modeled microphysical fields are compared by applying bifractal analysis, an approach that quantifies variability across spatial scales, to simulations of a drizzling stratocumulus field that span a range of domain sizes, drop concentrations (a proxy for mesoscale organization), and microphysics schemes (bulk and bin). Simulated q c closely matches observed estimates of bifractal parameters that measure smoothness and intermittency. There are major discrepancies between observed and simulated q r properties, though, with bulk simulated q r consistently displaying the bifractal properties of observed clouds (smooth, minimally intermittent) rather than rain while bin simulations produce q r that is appropriately intermittent but too smooth. These results suggest fundamental limitations of bulk and bin schemes to realistically represent higher-order statistics of the observed rain structure.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

Oxidation of Organics in the Defense Waste Processing Facility Condensate

Defense Waste Processing Facility (DWPF): The state of South Carolina currently holds 35 million gallons of radioactive waste in 51 underground tanks. DWPF was built in an effort to convert the waste into a more stable form. It turns the sludge waste from the tanks into glass, which will keep the waste stable for 10,000 years. Currently, DWPF uses formic acid in its flowsheet and there is one major problem associated with its use: it decomposes into hydrogen, a flammable gas. Glycolic acid, however, has been found as a possible alternative that performs similarly to formic acid but does not directly form hydrogen. One of the main issues with the glycolic acid flowsheet is the potential for there to be glycolate and other organics in DWPF's Recycle Collection Tank (RCT). These organics could lead to hydrogen generation later in the downstream evaporators and must be destroyed in the RCT in order for glycolic acid to be a suitable replacement for formic acid. Oxidants can be added to the RCT to destroy the organics. Two oxidizers, permanganate and Fenton's reagent (iron catalyzed hydrogen peroxide), are possible candidates. Find optimum processing conditions for the oxidation of organic species in a typical RCT simulant. A reactor served as a small-scale version of the RCT. During each run, an RCT simulant with 8 added organics, including glycolate, was created in the reactor. Either permanganate or peroxide was slowly added for each run through a syringe pump. Each experiment lasts 6 hours and a total of 23 runs are scheduled. Variables of Interest: Oxidizer (Permanganate or Peroxide); Temperature (15 deg. C to 50 deg. C); Oxidant addition time (10 mins to 2 hours); Amount of oxidant (1 x to 1.5 x stoichiometric requirements); Solution pH (3 to 13); Glycolate concentration (125 to 250 mg/kg). Offgas Analyzers: Mass spectrometer and FTIR spectrometer. Samples: pulled at 7 different times throughout the run to determine the amount of organic and inorganic carbon and concentrations of various organics through ion chromatography (IC). Only 3 of the runs have been completed at this point, all with permanganate. Based on the first 3 runs, permanganate seems to oxide the majority of the organics and the run at pH 8 and 32.5 deg. C had the most effective oxidation. The rest of the runs will need to be performed to determine the best oxidant and optimum values of the other variables of interest. Once the experiment is completed, DWPF will select one of the oxidants. Testing will continue to determine its performance during foam-over and other non-ideal conditions. Finally, the oxidant will be tested with actual radioactive waste to confirm its effectiveness.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2019

Understanding the Significance of Biochemistry in the Storage, Handling, Purification, and Sampling of Amphiphilic Mycolactone

Mycolactone, the amphiphilic macrolide toxin secreted by Mycobacterium ulcerans , plays a significant role in the pathology and manifestations of Buruli ulcer (BU). Consequently, it follows that the toxin is a suitable target for the development of diagnostics and therapeutics for this disease. Yet, several challenges have deterred such development. For one, the lipophilic nature of the toxin makes it difficult to handle and store and contributes to variability associated with laboratory experimentation and purification yields. In this manuscript, we have attempted to incorporate our understanding of the lipophilicity of mycolactone in order to define the optimal methods for the storage, handling, and purification of this toxin. We present a systematic correlation of variability associated with measurement techniques (thin-layer chromatography (TLC), mass spectrometry (MS), and UV-Vis spectrometry), storage conditions, choice of solvents, as well as the impact of each of these on toxin function as assessed by cellular cytotoxicity. We also compared natural mycolactone extracted from bacterial culture with synthesized toxins in laboratory (solvents, buffers) and physiologically relevant (serum) matrices. Our results point to the greater stability of mycolactone in organic, as well as detergent-containing, solvents, regardless of the container material (plastic, glass, or silanized tubes). They also highlight the presence of toxin in samples that may be undetectable by any one technique, suggesting that each detection approach captures different configurations of the molecule with varying specificity and sensitivity. Most importantly, our results demonstrate for the very first time that amphiphilic mycolactone associates with host lipoproteins in serum, and that this association will likely impact our ability to study, diagnose, and treat Buruli ulcers in patients.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2011

SWIFT X-RAY OBSERVATIONS OF CLASSICAL NOVAE. II. THE SUPER SOFT SOURCE SAMPLE

The Swift gamma-ray burst satellite is an excellent facility for studying novae. Its rapid response time and sensitive X-ray detector provides an unparalleled opportunity to investigate the previously poorly sampled evolution of novae in the X-ray regime. This paper presents Swift observations of 52 Galactic/Magellanic Cloud novae. We included the X-Ray Telescope (0.3-10 keV) instrument count rates and the UltraViolet and Optical Telescope (1700-8000 A) filter photometry. Also included in the analysis are the publicly available pointed observations of 10 additional novae the X-ray archives. This is the largest X-ray sample of Galactic/Magellanic Cloud novae yet assembled and consists of 26 novae with Super Soft X-ray emission, 19 from Swift observations. The data set shows that the faster novae have an early hard X-ray phase that is usually missing in slower novae. The Super Soft X-ray phase occurs earlier and does not last as long in fast novae compared to slower novae. All the Swift novae with sufficient observations show that novae are highly variable with rapid variability and different periodicities. In the majority of cases, nuclear burning ceases less than three years after the outburst begins. Previous relationships, such as the nuclear burning duration versus t{sub 2} or the expansion velocity of the eject and nuclear burning duration versus the orbital period, are shown to be poorly correlated with the full sample indicating that additional factors beyond the white dwarf mass and binary separation play important roles in the evolution of a nova outburst. Finally, we confirm two optical phenomena that are correlated with strong, soft X-ray emission which can be used to further increase the efficiency of X-ray campaigns.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2016

Prospective Validation of a High Dimensional Shape Model for Organ Motion in Intact Cervical Cancer

Purpose: Validated models are needed to justify strategies to define planning target volumes (PTVs) for intact cervical cancer used in clinical practice. Our objective was to independently validate a previously published shape model, using data collected prospectively from clinical trials. Methods and Materials: We analyzed 42 patients with intact cervical cancer treated with daily fractionated pelvic intensity modulated radiation therapy and concurrent chemotherapy in one of 2 prospective clinical trials. We collected online cone beam computed tomography (CBCT) scans before each fraction. Clinical target volume (CTV) structures from the planning computed tomography scan were cast onto each CBCT scan after rigid registration and manually redrawn to account for organ motion and deformation. We applied the 95% isodose cloud from the planning computed tomography scan to each CBCT scan and computed any CTV outside the 95% isodose cloud. The primary aim was to determine the proportion of CTVs that were encompassed within the 95% isodose volume. A 1-sample t test was used to test the hypothesis that the probability of complete coverage was different from 95%. We used mixed-effects logistic regression to assess effects of time and patient variability. Results: The 95% isodose line completely encompassed 92.3% of all CTVs (95% confidence interval, 88.3%-96.4%), not significantly different from the 95% probability anticipated a priori (P=.19). The overall proportion of missed CTVs was small: the grand mean of covered CTVs was 99.9%, and 95.2% of misses were located in the anterior body of the uterus. Time did not affect coverage probability (P=.71). Conclusions: With the clinical implementation of a previously proposed PTV definition strategy based on a shape model for intact cervical cancer, the probability of CTV coverage was high and the volume of CTV missed was low. This PTV expansion strategy is acceptable for clinical trials and practice; however, we recommend daily image guidance to avoid systematic large misses in select patients.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

DOE OSTI2024

Ensemble variational Fokker-Planck methods for data assimilation

Particle flow filters solve Bayesian inference problems by smoothly transforming a set of particles into samples from the posterior distribution. Particles move in state space under the flow of an McKean-Vlasov-Itˆo process. This work introduces the Variational Fokker-Planck (VFP) framework for data assimilation, a general approach that includes previously known particle flow filters as special cases. The McKean-Vlasov-Itˆo process that transforms particles is defined via an optimal drift that depends on the selected diffusion term. It is established that the underlying probability density - sampled by the ensemble of particles - converges to the Bayesian posterior probability density. For a finite number of particles the optimal drift contains a regularization term that nudges particles toward becoming independent random variables. Based on this analysis, we derive computationally-feasible approximate regularization approaches that penalize the mutual information between pairs of particles, and avoid particle collapse. Moreover, the diffusion plays a role akin to a particle rejuvenation approach that aims to alleviate particle collapse. The VFP framework is very flexible. Different assumptions on prior and intermediate probability distributions can be used to implement the optimal drift, and localization and covariance shrinkage can be applied to alleviate the curse of dimensionality. A robust implicit-explicit method is discussed for the efficient integration of stiff McKean- Vlasov-Itˆo processes. Here, the effectiveness of the VFP framework is demonstrated on three progressively more challenging test problems, namely the Lorenz ’63, Lorenz ’96 and the quasi-geostrophic equations.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2022

Representing Socio‐Economic Uncertainty in Human System Models

Abstract Socio‐economic development pathways and their implications for the environment are highly uncertain, and energy transitions will involve complex interactions among sectors. Here, traditional Monte Carlo analysis is paired with scenario discovery techniques to provide a richer portrait of these complexities. Modeled uncertain input variables include costs of advanced energy technologies, energy efficiency trends, fossil fuel resource availability, elasticities of substitution for labor, capital, and energy across economic sectors, population growth, and labor and capital productivity. The sampled values are simulated through a multi‐sector, multi‐region, recursively dynamic model of the world economy to explore a range of possible future outcomes. We find that many patterns of energy and technology development are possible for various long‐term environmental pathways and that sectoral output for most sectors is little affected through 2050 by the long‐term temperature target, but with tight constraints on emissions, emission intensities must fall much more rapidly. Scenario discovery techniques are applied to the large uncertainty ensembles to explore if there are prevailing storylines behind outcomes of interest. An illustrative investigation focused on different levels of economic growth shows many combinations of pathways and no single storyline emerging for a given economic outcome. This method can be extended to other outcomes of interest, exploring the nature of scenarios with both tail and median outcomes. Sampling from a Monte Carlo generated ensemble provides a rich set of scenarios to investigate, and potentially aids in avoiding heuristic biases in less structured scenario approaches.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2022

Evaluating changes in growth and pigmentation of Cladosporium cladosporioides and Paecilomyces variotii in response to gamma and ultraviolet irradiation

Abstract Melanin-containing fungi (black molds) have the capacity to thrive under extreme environmental conditions such as the elevated radiation levels inside the former Chernobyl reactors. These fungi have been hypothesized to grow toward and use gamma radiation as an energy source, but the literature does not clearly address which energies of the electromagnetic spectrum, if any, positively affect fungal growth. The goal of this work was to characterize the response of non-melanized and melanized fungi to two distinct electromagnetic wavelengths, i.e., ultraviolet (UV) and gamma ray, keeping absorption and other potentially confounding variables constant. Exposure to UV or gamma radiation induced significant changes in fungi pigmentation, but not growth rate of Cladosporium cladosporioides and Paecilomyces variotii . Specifically, increased pigmentation of both fungi was observed in samples exposed to UV, while decreased pigmentation was observed for gamma-irradiated samples. These results provide new insights into the role of electromagnetic energies on growth of fungi and provide an impetus to examine additional energies and types of radiation to develop a fundamental understanding of this phenomenon.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2024

Spatial patterns of historical crop yields reveal soil health attributes in US Midwest fields

Abstract Attaining high crop yields and increasing carbon storage in agricultural soils, while avoiding negative environmental impacts on water quality, soil erosion, and biodiversity, requires accurate and precise management of crop inputs and management practices. The long-term analysis of spatial and temporal patterns of crop yields provides insights on how yields vary in a field, with parts of field constantly producing either high yields or low yields and other parts that fluctuate from one year to the next. The concept of yield stability has shown to be informative on how plants translate the effects of environmental conditions (e.g., soil, climate, topography) across the field and over the years in the final yield, and as a valuable layer in developing prescription maps of variable fertilizer rate inputs. Using known relationships between soil health and crop yields, we hypothesize that areas with measured constantly low yield will return low carbon to the soil affecting its heath. On this premises, yield stability zones (YSZ) provide an effective and practical integrative measure of the small-scale variability of soil health on a field relative basis. We tested this hypothesis by measuring various metrics of soil health from commercial farmers’ fields in the north central Midwest of the USA in samples replicated across YSZ, using a soil test suite commonly used by producers and stakeholders active in agricultural carbon credits markets. We found that the use of YSZ allowed us to successfully partition field-relative soil organic carbon (SOC) and soil health metrics into statistically distinct regions. Low and stable (LS) yield zones were statistically lower in normalized SOC when compared to high and stable (HS) and unstable (US) yield zones. The drivers of the yield differences within a field are a series of factors ranging from climate, topography and soil. LS zones occur in areas of compacted soil layers or shallow soils (edge of the field) on steeper slopes. The US zones occurring with high water flow accumulation, were more dependent on topography and rainfall. The differences in the components of the overall soil health score (SHS) between these YSZ increased with sample depth suggesting a deeper topsoil in the US and HS zones, driven by the accumulation of water, nutrients, and carbon downslope. Comparison of the field management provided initial evidence that zero tillage reduces the magnitude of the variance in SOC and soil health metrics between the YSZ.

Fowler, Ames↗

DOE OSTI2017

A practical approach to the sensitivity analysis for kinetic Monte Carlo simulation of heterogeneous catalysis

Lattice kinetic Monte Carlo simulations have become a vital tool for predictive quality atomistic understanding of complex surface chemical reaction kinetics over a wide range of reaction conditions. In order to expand their practical value in terms of giving guidelines for atomic level design of catalytic systems, it is very desirable to readily evaluate a sensitivity analysis for a given model. The result of such a sensitivity analysis quantitatively expresses the dependency of the turnover frequency, being the main output variable, on the rate constants entering the model. In the past the application of sensitivity analysis, such as Degree of Rate Control, has been hampered by its exuberant computational effort required to accurately sample numerical derivatives of a property that is obtained from a stochastic simulation method. Here in this study we present an efficient and robust three stage approach that is capable of reliably evaluating the sensitivity measures for stiff microkinetic models as we demonstrate using CO oxidation on RuO 2 (110) as a prototypical reaction. In a first step, we utilize the Fisher Information Matrix for filtering out elementary processes which only yield negligible sensitivity. Then we employ an estimator based on linear response theory for calculating the sensitivity measure for non-critical conditions which covers the majority of cases. Finally we adopt a method for sampling coupled finite differences for evaluating the sensitivity measure of lattice based models. This allows efficient evaluation even in critical regions near a second order phase transition that are hitherto difficult to control. The combined approach leads to significant computational savings over straightforward numerical derivatives and should aid in accelerating the nano scale design of heterogeneous catalysts.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2012

Disentangling instrumental features of the 130 GeV Fermi line

We study the instrumental features of photons from the peak observed at E{sub γ} = 130 GeV in the spectrum of Fermi-LAT data. We use the sPlots algorithm to reconstruct — seperately for the photons in the peak and for background photons — the distributions of quantities such as incident angles, the recorded time, features of the spacecraft position, the zenith angles, the conversion type and details of the energy and direction reconstruction. The presence of a striking feature or cluster in such a variable would suggest an instrumental cause for the peak. In the publically available data, we find several suggestive features which may inform further studies by instrumental experts, though the size of the signal sample is too small to draw statistically significant conclusions.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2014

The Personal Human Oral Microbiome Obscures the Effects of Treatment on Periodontal Disease

Periodontitis is a progressive disease of the periodontium with a complex, polymicrobial etiology. Recent Next-Generation Sequencing (NGS) studies of the microbial diversity associated with periodontitis have revealed strong, community-level differences in bacterial assemblages associated with healthy or diseased periodontal sites. In this study, we used NGS approaches to characterize changes in periodontal pocket bacterial diversity after standard periodontal treatment. Despite consistent changes in the abundance of certain taxa in individuals whose condition improved with treatment, posttreatment samples retained the highest similarity to pre-treatment samples from the same individual. Deeper phylogenetic analysis of periodontal pathogen-containing genera Prevotella and Fusobacterium found both unexpected diversity and differential treatment response among species. Our results highlight how understanding interpersonal variability among microbiomes is necessary for determining how polymicrobial diseases respond to treatment and disturbance.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2025

Tailoring Nitinol for elastocaloric application

This study focuses on tailoring commercial Nitinol, the most commonly used elastocaloric material, for near-room-temperature cooling applications. Short heat treatments near 500 °C were used to fine-tune the material’s transition temperature, resulting in austenite finish temperatures ranging from 6.0 to 25.5°C and altered superelastic and elastocaloric properties. Plateau stresses decreased while temperature changes rose from 21.5°C up to 27.9°C at 6% strain. Significant variability in the Nitinol response when testing below its austenite finish temperature was observed. In conclusion, the effect of mechanical cycling on transition temperatures was also evaluated, demonstrating an increase for all the samples.

Efficiency↗

DOE OSTI2023

Microbarograph - ESRL Hi-Res Microbarograph, Troutdale - Raw Data

High-precision barometers (Paroscientific 6000-16B-IS) are combined with Nishiyama-Bedard Quad Disk pressure probes, measuring pressure (mb) at the surface, nominally 2 m above ground level. Data are sampled at 20 Hz for potential studies of turbulence. The sensors' high accuracy makes them useful for determining horizontal pressure gradients and their relation to wind ramp events, as well as the temporal variability of pressure associated with mountain wakes and waves. **Note different ASCII file formats for Goldendale (z04) and Walla Walla (z09) sites.**

17 WIND ENERGY↗

DOE OSTI2023

Microbarograph - ESRL Hi-Res Microbarograph, Bonneville - Raw Data

17 WIND ENERGY↗

DOE OSTI2023

Microbarograph - ESRL Hi-Res Microbarograph, Goldendale - Raw Data

17 WIND ENERGY↗