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At least 649 records · Page 36

The FastEddy® Resident-GPU Accelerated Large-Eddy Simulation Framework: Moist Dynamics Extension, Validation and Sensitivities of Modeling Non-Precipitating Shallow Cumulus Clouds

Herein we describe the moist dynamics formulation implemented within the graphics processing unit-resident large-eddy simulation FastEddy® model, which includes a simple saturation adjustment scheme for condensation and evaporation processes. Two LES model intercomparison exercises for non-precipitating shallow cumulus clouds are simulated in order to validate this model extension, including a static forcing and a time-dependent forcing case. Overall, we find our dynamical, thermodynamical and microphysical quantities, along with turbulence variability and fluxes, to be commensurate with the corresponding model intercomparison results. In addition, sensitivities to specific model settings are investigated. Among these settings, it is shown that boundary layer and cloud layer structure and characteristics are sensitive to use of higher-order advection schemes impacting the vertical distribution of cloud content and associated turbulence statistics. Increasing the timescale of the saturation scheme leads to enhanced liquid water presence and decreases vertical velocity variance within the cloud deck. In some cases, these sensitivities agree with the model-to-model variability reported in the intercomparison exercises, highlighting the important role of specific model implementation choices in the context of shallow cumulus convection simulations. These analyses and findings also provide the basis for future extensions and applications of FastEddy® for modeling moist convection and precipitation scenarios.

54 ENVIRONMENTAL SCIENCES↗

Optimization of key energy and performance metrics for drug product manufacturing

During the development of pharmaceutical manufacturing processes, detailed systems-based analysis and optimization are required to control and regulate critical quality attributes within specific ranges, to maintain product performance. As discussions on carbon footprint, sustainability, and energy efficiency are gaining prominence, the development and utilization of these concepts in pharmaceutical manufacturing are seldom reported, which limits the potential of pharmaceutical industry in maximizing key energy and performance metrics. Based on an integrated modeling and techno-economic analysis framework previously developed by the authors, this study presents the development of a combined sensitivity analysis and optimization approach to minimize energy consumption while maintaining product quality and meeting operational constraints in a pharmaceutical process. The optimal input process conditions identified were validated against experiments and good agreement resulted between simulated and experimental data. Here, the results also allowed for a comparison of the capital and operational costs for batch and continuous manufacturing schemes under nominal and optimized conditions. Using the nominal batch operations as a basis, the optimized batch operation results in a 71.7% reduction of energy consumption, whereas the optimized continuous case results in an energy saving of 83.3%.

59 BASIC BIOLOGICAL SCIENCES↗

Status of the Mu2e experiment at Fermilab

The Mu2e experiment aims to improve, by four orders of magnitude, current sensitivity in the search for the charged-lepton flavor violating (cLFV) neutrino-less conversion of a negative muon into an electron. The conversion process will be identified by a distinctive signature of a mono-energetic electron with energy slightly below the muon rest mass. In the Standard Model this process has a negligible rate. However, in many Beyond the Standard Model scenarios its rate is within the reach of Mu2e sensitivity. In this paper, we explain the Mu2e design guidelines and summarize the status of the experiment.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Effects of Wire Diameter and Filament Size on the Processing Window of Bi-2212 Round Wire

High engineering critical current density (J E of 1300 A/mm 2 at 4.2 K and 15 T) in Bi-2212 round wire has been achieved through a partial melt, overpressure heat treatment process. J E varies strongly with processing conditions, particularly the maximum heat treatment temperature (T max ). Increasing T max results in longer time in the melt (defined as the time between when Bi-2212 melts on heating and when Bi-2212 begins to form on cooling), more bridging between the filaments, lower J E , and higher ac losses. A wide processing window with a large range of T max that has a nearly constant J E is desired for processing large coils with large thermal mass and significant thermal time constants that may make precise control over the desired temperature – time profiles uncertain. Accordingly, we wanted to explore broadening the T max window by controlling the Bi-2212 powder melting or wire architecture design. In this work, we report on studies of the performance variation with T max for two production wires with a filling factor of about 20% and 85 × 18 filaments where filament size was varied by changing the wire diameter, a process which also shortens the distance between filaments. We found that wires with smaller filament diameter (9 to 11 μm) showed a peak J E at the low end of T max and also a J E that was more sensitive to T max . A J E – T max plot showed a plateau J E (4.2 K, 5 T) of ~1100 A/mm 2 between T max of 886 and 894 °C for 1.0 and 1.2 mm wires, where J E is less sensitive to the wire diameter and T max . This J E plateau range is a preferred processing window for achieving high J E in coils.

36 MATERIALS SCIENCE↗

Exploring the Nucleon Structure via Deep Electroproduction Processes

Understanding the internal structure of the nucleon is a fundamental goal of modern physics, which aims at a comprehensive framework describing the internal dynamics of quarks and gluons. Among other structure functions, Generalized Parton Distributions (GPDs) offer a powerful framework for describing the nucleon dynamics by correlating the longitudinal momentum and the transverse position of its internal partons. Such a correlation provides a three-dimensional picture of the nucleon and enables access to fundamental properties, including the internal pressure distributions and the parton’s angular momentum contribution to the nucleon's total spin, thereby playing a central role in resolving the nucleon spin puzzle. At the Thomas Jefferson National Facility (JLab), polarized electron beam experiments allow for probing GPDs through the measurement of hard exclusive processes. Among the cleanest experimental channels, we find the electro-production of a real photon through the Deeply Virtual Compton Scattering (DVCS) mechanism. The first data-taking period of the CLAS12 program, taking place in 2018, allowed for unique DVCS Beam Spin Asymmetry (BSA) measurements in the phase space covered by a 10.6 GeV polarized electron beam impinging on an unpolarized liquid hydrogen target. Although detecting all final-state particles ensures exclusivity of the process, conservation laws indicate that it is not mandatory. I adopt an approach omitting the direct detection of the recoil proton, providing a simplified yet effective event selection strategy that boosts statistics and gives access to a larger phase space sensitive to the underlying GPD dynamics through BSA and cross section measurements. The Double DVCS (DDVCS) process promises a dedicated mapping of GPDs. Contributing to the electro-production of a lepton pair cross-section, the DDVCS reaction extends DVCS by allowing the final-state photon to be virtual, enriching the kinematic phase space and providing unique access to the internal correlations encoded by GPDs. A feasibility study is conducted to assess the potential of future DDVCS measurements at Jefferson Lab and the future Electron-Ion Collider (EIC). While Jefferson Lab will provide DDVCS measurements in the valence region through the SoLID$\mu$ and $\mu$CLAS12 experimental projects, in the long term, the EIC will provide complementary measurements in the sea region, both accessing unprecedented information about GPDs in a phase space region otherwise inaccessible. Taken together, these investigations demonstrate both the current capabilities and future opportunities for probing GPDs through exclusive processes. The experimental analysis of DVCS at CLAS12 provides precise measurements within an established framework, while the phenomenological study of DDVCS opens the door to richer and more comprehensive explorations with future detectors and facilities.

Alvarado, Juan [Université Paris-Saclay: Gif-sur-Y↗

Time-resolved probing of laser-induced nanostructuring processes in liquids

Laser synthesis and processing of colloids (LSPC) in liquids has gained widespread applications in producing nanomaterials of different classes of solids. While the technical processes in different cases of ablation, fragmentation or colloidal fusion may look macroscopically different in each application, the underlying fundamental mechanisms are always the same cascade of laser interaction with matter, non-thermal or thermal energy deposition, phase transitions, and the subsequent structure formation processes. Disentangling these mechanisms represents a veritable challenge, as ultrafast and structurally sensitive experimental methods are required. This review presents a discussion of how state-of-the-art experimental protocols using ultrafast lasers and sensitive structural probes, such as electrons or X-rays are able to address this challenge. In particular, it is possible to investigate LSPC on single objects using single probe pulses and avoid accumulation effects in a heterogeneous sample. The presented results capture structure formation with femtosecond and atomic scale resolution. Ultrafast time-resolved probing approaches are key to revealing the transient states and pathways that govern material transformation in LSPC.

X-ray scattering↗

Surface Reconstruction of Halide Perovskites During Post-treatment

Postfabrication surface treatment strategies have been instrumental to the stability and performance improvements of halide perovskite photovoltaics in recent years. However, a consensus understanding of the complex reconstruction processes occurring at the surface is still lacking. Here, we combined complementary surface-sensitive and depth-resolved techniques to investigate the mechanistic reconstruction of the perovskite surface at the microscale level. We observed a reconstruction toward a more PbI 2 -rich top surface induced by the commonly used solvent isopropyl alcohol (IPA). We discuss several implications of this reconstruction on the surface thermodynamics and energetics. Particularly, our observations suggest that IPA assists in the adsorption process of organic ammonium salts to the surface to enhance their defect passivation effects.

14 SOLAR ENERGY↗

Fast and sensitive measurements of sub-3 nm particles using Condensation Particle Counters For Atmospheric Rapid Measurements (CPC FARM)

New particle formation (NPF) is the atmospheric process whereby gas molecules react and nucleate to form detectable particles. NPF has a strong impact on Earth's radiative balance as it produces roughly half of global cloud condensation nuclei. However, the time resolution and sensitivity of current instrumentation are inadequate in measuring the size distribution of sub-3 nm particles, the particles critical for understanding NPF. Here we present the Condensation Particle Counters For Atmospheric Rapid Measurements (CPC FARM), a method to measure the concentrations of freshly nucleated particles. The CPC FARM consists of five CPCs operating in parallel, each configured to operate at different detectable particle sizes between 1–3 nm. This study explores two methods to calculate the size distribution from the differential measurements across the CPC channels. The performance of both inversion methods was tested against the size distribution measured by a pair of stepping particle mobility sizers (SMPSs) during an ambient air sampling study in Pittsburgh, PA. Observational results indicate that the CPC FARM is more accurate with higher time resolution and sensitivity in the sub-3 nm range compared to the SMPS.

Cheng, Darren [Carnegie Mellon Univ., Pittsburgh, ↗

DUNE experiment physics

The Deep Underground Neutrino Experiment (DUNE) will feature a 40-kton liquid argon TPC detector situated a mile below the surface at the Sanford Underground Research Facility. A new broadband high-intensity neutrino source and Near Detector complex will be located at Fermilab, 1300 kilometers away. This arrangement will provide unprecedented sensitivity in the search for neutrino CP violation, determination of the neutrino mass ordering, and precision measurements of neutrino mixing parameters. The underground Far Detector also allows for low background, low threshold observations of supernova neutrinos, with a unique sensitivity to the electron neutrino flux. Further, DUNE will conduct a wide range of searches for physics beyond the Standard Model, including baryon number violation, rare scattering processes, and non-standard flavor transitions. In this poster, we review DUNE's extensive physics program and show updated sensitivities.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Ammonia Permeation Through Inorganic Membranes

Moisture probes are used in the tritium facility to measure the moisture content of the gas stream. When tritium reacts with nitrogen to form ammonia, the ammonia gas damages the sensitive moisture probe. The gas stream tested during this experiment for moisture probe protection is composed of nitrogen and argon gas in conjunction with ammonia and water vapor. The gas stream is filtered through an inorganic membrane due to the high reactivity of tritium and a residual gas analyzer (RGA) is used to measure the ammonia and water vapor in the gas stream, as well as the permeability of nitrogen and argon through the inorganic membranes. The membranes tested were boron nitride and silver. The permeability was compared for each membrane at different pressures and flow rates. Fourier-transformed infrared spectroscopy (FT-IR) was used to compare the membranes before and after ammonia permeation. Ammonia gas is a byproduct formed from tritium gas reacting with nitrogen in the gas stream, similar to the Haber Process which occurs when hydrogen reacts with nitrogen [2]. The corrosive nature of ammonia damages metals and sensitive instruments such as moisture probes. Moisture probes are essential in various gas and liquid processes for measuring the moisture content of a gas. Membrane research has found that graphene oxide membranes successfully uptake ammonia from the gas stream at a humidity of approximately 30% at which point the pores pin closed, preventing gas permeation. Further research is being conducted to find an inorganic membrane that will prevent ammonia permeation thus circumventing damage to the sensitive moisture probe. The permeation measurements for argon and nitrogen gas and water and ammonia vapor were measured at various pressures of 800, 1000, 1200, 1500, 1800, and 2000 torr. The permeability average (PA) was calculated for each filter using a Barrer calculation. The average permeations for each filter were then compared. The gas composition was measured using the RGA Nitrogen was permeated through the membranes after ammonia permeation and a FT-IR spectrum was obtained. Boron Nitride: As the nitrogen pressure increased, the permeability of the membrane decreased from 800-1200 torr and remained relatively unchanged from 1200-2000 torr. The membrane exhibited a slight decrease in argon permeability from 800-1200 torr and a slight increase from 1500-2000 torr. The boron nitride membrane when permeated with ammonia and nitrogen prevented less ammonia permeation compared to the blank filter. The boron nitride filter demonstrated a decrease in permeability after ammonia permeation. Silver Membrane: When permeated with nitrogen alone, the membrane permeability decreased from 800 torr to 1200 torr. The permeability of the membrane showed little difference as pressure increased from 1200 torr. When permeated with argon, the same phenomenon occurred but on a much smaller scale. When compared to the blank and the boron nitride membranes the silver membrane exhibited significantly lower permeability. This may be in part due to the coating on the silver membrane and differences in pore size of the membranes. During permeation with ammonium hydroxide vapor and nitrogen, the partial pressure of the ammonia increased as compared to the blank membrane. The permeability before and after permeation with ammonia and nitrogen were compared. Permeability values suggested that after being permeated with the ammonia that the permeability for lower pressures increased slightly. There was no significant change in the FT-IR spectrums before and after permeation. Future work: Continue testing various inorganic membranes for ammonia permeation. Further research chemical separation of ammonia from the gas stream, which may prove difficult due to the high reactivity of tritium.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Understanding and controlling the fundamental photochemistry of protonic solar energy conversion (Final Scientific/Technical Report)

The selectivity and activity of most fuel-forming reactions are tunable by the concentration of electrons, holes, protons, and/or hydroxides. That is one reason why traditional solar energy conversion processes are used to drive these reactions, where light directly increases the concentration of electrons and holes. We, instead, took a different approach, using light to increase the concentration of protons and/or hydroxides. For this, we leveraged photophysical and solid-state physics theories, techniques, and design strategies previously developed for the study of traditional solar energy conversion processes. We designed and fabricated several materials platforms based on molecular photoacid and photobase dyes coupled with ion-exchange polymer membranes and assessed their fundamental photoelectrochemistry. We demonstrated control over built-in electric potentials, photovoltages, proton-transfer kinetics, and efficiency limits to our approach. Understanding the basic science of these dye-sensitized protonic membranes and their photochemical mechanisms is of use to the DOE-relevant processes of solar photochemical fuel formation, solar photodialytic desalination, and solar cells. Moreover, functional materials that we developed from this project may be of use to several broad-reaching fields and may provide the foundation for a completely new, inexpensive, and robust solar energy conversion technology.

14 SOLAR ENERGY↗

Metal-to-Ligand Charge-Transfer Spectrum of a Ru-Bipyridine-Sensitized TiO 2 Cluster from Embedded Multiconfigurational Excited-State Theory

Understanding optical properties of the dye molecule in dye-sensitized solar cells (DSSCs) from first-principles quantum mechanics can contribute to improving the efficiency of such devices. While density functional theory (DFT) and time-dependent DFT have been pivotal in simulating optoelectronic properties of photoanodes used in DSSCs at the atomic scale, questions remain regarding DFT’s adequacy and accuracy to furnish critical information needed to understand the various excited-state processes involved. In this work, we simulate the absorption spectra of a dye-sensitized solar cell analogue, comprised of a Ru-bipyridine (Ru-bpy) dye molecule and a small TiO2 cluster via DFT and via an accurate embedded correlated wavefunction (CW) theory. We generated CW spectra for the adsorbed Ru-bpy dye via a recently introduced capped density functional embedding theory or capped-DFET (to generate the embedding potential that accounts for the interaction of the molecule and the TiO 2 cluster). We then combined capped-DFET with the accurate but expensive multiconfigurational complete active space second-order perturbation theory (CASPT2)—embedded CASPT2. Because the CW theory is conducted on only a portion of the total system in the presence of an embedding potential that describes that portion’s interaction with its environment, we efficiently obtain CW-quality predictions that reflect local properties of the entire system. Specifically, for example, with capped-DFET and embedded CW theory, we can simulate accurately a plethora of metal-to-ligand charge-transfer excited properties at a manageable computational cost. Here, we predict detailed electronic spectra within the visible region, featuring the lowest three singlet and triplet excited states, along with predictions of the singlets’ lifetimes. We illustrated these results using a Jablonski diagram that show the relative energy position of the singlet and longer-lived triplet excited states and analyzed and proposed relaxation paths for the excited state corresponding to the most intense but short-lived absorption (interconversion, intersystem crossing, fluorescence, and phosphorescence) that may lead to longer-lived excited states necessary for efficient charge separation required to generate current in solar cells.

14 SOLAR ENERGY↗

An antibody-free platform for multiplexed, sensitive quantification of protein biomarkers in complex biomatrices

Sensitive, multiplexed protein quantification remains challenging despite recent advancements in LC-MS assays for targeted protein biomarker quantification. High-sensitivity protein biomarker measurements usually require immuno-affinity enrichment of target protein; a process which is highly dependent on capture reagent and limited in capability to measure multiple analytes. Herein, we report a novel antibody-free platform, which measures multiple biomarkers from complex matrices employing a strategically optimized solid-phase extraction cleanup and orthogonal multidimensional LC-MS. Eight human protein biomarkers with different specifications were spiked into canine plasma as a model investigation system. The developed strategy achieved the desired sensitivity, robustness, and throughput via the following steps: (1) post digestion mixed-mode cation exchange-reverse phase SPE enrichment cleaned up the sample initially; (2) rapid, high-pH peptide fractionation further eliminated background components efficiently while selectively enriched signature peptides (SP) to provide sufficient sensitivity for multiple targets; and (3) trapping-micro-LC-MS analysis delivered high sensitivity comparable to a nano-LC-MS method but with much better robustness and throughput for the final analysis. Compared with a conventional LC-MS assay with direct protein digestion and limited clean-up, analysis with this antibody-free platform improved the LLOQ by 1–2 orders of magnitude for the eight protein biomarkers, reaching as low as 5 ng/mL in plasma, with feasible robustness and throughput. In conclusion, this platform was applied for the quantification of biomarkers of respiratory conditions in patients with various lung diseases, demonstrating real-world applicability.

59 BASIC BIOLOGICAL SCIENCES↗

Development of direct ink write radially graded alumina/zirconia

Functionally graded materials (FGMs) are of interest in multiple fields, yet many materials combinations are limited by coefficient of thermal expansion (CTE) mismatch. Here, a radially graded alumina/yttria-doped zirconia (Al 2 O 3 /8YZ) FGM is used to demonstrate processing strategies to mitigate CTE and sintering behavior differences between these oxides. FGM materials are especially sensitive to ink stability during printing, as all components (in this case, Al 2 O 3 and 8YZ) must be stabilized in the same dispersant or additive solution. Thus, this system is also ideal to demonstrate ink optimization best practices. Materials were characterized throughout processing to correlate the effects of common additives on both the ceramic particle suspensions and final sintered components. Aggregation observed in the initial additive-containing suspensions were present in the sintered component. The differences in sintering onset temperature and shrinkage rate resulted in internal stresses within the sintered component, which ultimately caused mechanical failure of the component under low stress. In conclusion, a processing strategy was recommended to mitigate the sintering behavior mismatch of alumina and 8 wt% yttria-stabilized zirconia.

Lamm, Benjamin W. [Oak Ridge National Laboratory (↗

Characterization of the image plate multi-scan response to mono-energetic x-rays

Image plates (IPs), or phosphor storage screens, are a technology employed frequently in inertial confinement fusion (ICF) and high energy density plasma (HEDP) diagnostics because of their sensitivity to many types of radiation, including, x rays, protons, alphas, beta particles, and neutrons. Prior studies characterizing IPs are predicated on the signal level remaining below the scanner saturation threshold. Since the scanning process removes some signal from the IP via photostimulated luminescence, repeatedly scanning an IP can bring the signal level below the scanner saturation threshold. This process, in turn, raises concerns about the signal response of IPs after an arbitrary number of scans and whether such a process yields, for example, a constant ratio of signal between the nth and n + 1st scan. Here, the sensitivity of IPs is investigated when scanned multiple times. It is demonstrated that the ratio of signal decay is not a constant with the number of scans and that the signal decay depends on the x-ray energy. As such, repeatedly scanning an IP with a mixture of signal types (e.g., x ray, neutron, and protons) enables ICF and HEDP diagnostics employing IPs to better isolate a particular signal type.

Instruments & Instrumentation↗

Sensitivity of Thermal Predictions to Uncertain Surface Tension Data in Laser Additive Manufacturing

To understand the process-microstructure relationships in additive manufacturing (AM), it is necessary to predict the solidification characteristics in the melt pool. This study investigates the influence of Marangoni driven fluid flow on the predicted melt pool geometry and solidification conditions using a continuum finite volume model. A calibrated laser absorptivity was determined by comparing the model predictions (neglecting fluid flow) against melt pool dimensions obtained from single laser melt experiments on a nickel super alloy 625 (IN625) plate. Using this calibrated efficiency, predicted melt pool geometries agree well with experiments across a range of process conditions. When fluid mechanics is considered, a surface tension gradient recommended for IN625 tends to overpredict the influence of convective heat transfer, but the use of an intermediate value reported from experimental measurements of a similar nickel super alloy produces excellent experimental agreement. Despite its significant effect on the melt pool geometry predictions, fluid flow was found to have a small effect on the predicted solidification conditions compared to processing conditions. We find that this result suggests that under certain circumstances, a model only considering conductive heat transfer is sufficient for approximating process-microstructure relationships in laser AM. Extending the model to multiple laser passes further showed that fluid flow also has a small effect on the solidification conditions compared to the transient variations in the process. Furthermore, limitations of the current model and areas of improvement, including uncertainties associated with the phenomenological model inputs are discussed.

36 MATERIALS SCIENCE↗

Climate and multiple dimensions of plant diversity regulate ecosystem carbon exchange along an elevational gradient

The impacts of warming on communities and ecosystems are predicted to be significant in mountain ecosystems because physiological processes, including rates of carbon (C) cycling, are often more temperature-sensitive in colder environments. Plant biodiversity can also influence C exchange, yet few studies integrate how biotic and abiotic factors may directly or interactively impact ecosystem Cflux. Here, we examine the link between simultaneous changes in multiple dimensions of plant diversity and peak growing season ecosystem C uptake across a climatic gradient in the Rocky Mountains, Colorado, USA. We found that taxonomic diversity (species richness), functional diversity (functional evenness), and phylogenetic diversity (mean pairwise distance) were significantly and positively related to peak growing sea-son ecosystem C uptake (i.e., net ecosystem exchange) when considered independently. However, when abiotic and biotic factors were integrated in a structural equation model, only plant phylogenetic diversity was significantly related to C uptake. In addition, we found that actual evapotranspiration (AET - a measure that integrates precipitation and temperature) affected ecosystem C exchange indirectly via its impact on the three dimensions of plant diversity that we examined. These findings highlight complex relation-ships among key measures of biodiversity and ecosystem C uptake in a rapidly warming ecosystem, and the possible mechanisms that underlie relationships between biodiversity and ecosystem functioning. They also point to the need for integrating multiple dimensions of biodiversity into studies of community and ecosystem ecology.

54 ENVIRONMENTAL SCIENCES↗

Improving the picture of atomic structure in nonoriented polymer domains using the pair distribution function: A study of polyamide 6

Abstract Investigations of the atomic structures within polyamides started over 80 years ago and continue today. These weakly ordered materials diffract X‐rays poorly and typically require postprocessing to obtain idealized samples for structural studies. An important goal remains to develop techniques to study the local structure in its natural state, with atomic resolution, and with sensitivity to subtle changes due to synthesis conditions or other technologically relevant processing procedures. Here, we compare the structures of as‐produced, nonoriented polyamide 6 ([C 6 H 11 NO] n ) from both hydrolytic and anionic processes. A total scattering pair distribution function approach is used to elucidate information about the atomic bonding, molecular conformation, chain packing, crystallite size, and ratio of ordered to disordered domain content. The results are compared with those from standard analytical methods.

Terban, Maxwell W.↗