Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “NUCLEATION”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic

Abstract. Atmospheric ice nucleation impacts the hydrological cycle and climate by modifying the radiative properties of clouds. To improve our predictive understanding of ice formation, ambient ice-nucleating particles (INPs) need to be collected and characterized. Measurements of INPs at lower latitudes in a remote marine region are scarce. The Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign, in the region of the Azores islands, provided the opportunity to collect particles in the marine boundary layer (MBL) and free troposphere (FT) by aircraft during the campaign's summer and winter intensive operation period. The particle population in samples collected was examined by scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy. The identified INPs were analyzed by scanning electron microscopy with energy-dispersive X-ray analysis. We observed differences in the particle population characteristics in terms of particle diversity, mixing state, and organic volume fraction between seasons, mostly due to dry intrusion events during winter, as well as between the sampling locations of the MBL and FT. These differences are also reflected in the temperature and humidity conditions under which water uptake, immersion freezing (IMF), and deposition ice nucleation (DIN) proceed. Identified INPs reflect typical particle types within the particle population on the samples and include sea salt, sea salt with sulfates, and mineral dust, all associated with organic matter, as well as carbonaceous particles. IMF and DIN kinetics are analyzed with respect to heterogeneous ice nucleation rate coefficients, Jhet, and ice nucleation active site density, ns, as a function of the water criterion Δaw. DIN is also analyzed in terms of contact angles following classical nucleation theory. Derived MBL IMF kinetics agree with previous ACE-ENA ground-site INP measurements. FT particle samples show greater ice nucleation propensity compared to MBL particle samples. This study emphasizes that the types of INPs can vary seasonally and with altitude depending on sampling location, thereby showing different ice nucleation propensities, which is crucial information when representing mixed-phase cloud and cirrus cloud microphysics in models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Quantifying and Modeling the Impact of Phase State on the Ice Nucleation Abilities of 2-Methyltetrols as a Key Component of Secondary Organic Aerosol Derived from Isoprene Epoxydiols

Organic aerosols (OAs) may serve as ice-nucleating particles (INPs), impacting the formation and properties of cirrus clouds when their phase state and viscosity are in the semisolid to glassy range. However, there is a lack of direct parameterization between aerosol viscosity and their ice nucleation capabilities. In this study, we experimentally measured the ice nucleation rate of 2-methyltetrols (2-MT) aerosols, a key component of isoprene-epoxydiol-derived secondary organic aerosols (IEPOX-SOA), at different viscosities. These results demonstrate that the phase state has a significant impact on the ice nucleation abilities of OA under typical cirrus cloud conditions, with the ice nucleation rate increasing by 2 to 3 orders of magnitude when the phase state changes from liquid to semisolid. An innovative parametric model based on classical nucleation theory was developed to directly quantify the impact of viscosity on the heterogeneous nucleation rate. This model accurately represents our laboratory measurement and can be implemented into climate models due to its simple, equation-based form. Based on data collected from the ACRIDICON-CHUVA field campaign, our model predicts that the INP concentration from IEPOX-SOA can reach the magnitude of 1 to tens per liter in the cirrus cloud region impacted by the Amazon rainforest, consistent with recent field observations and estimations. This novel parameterization framework can also be applied in regional and global climate models to further improve representations of cirrus cloud formation and associated climate impacts.

2-methyltetrol↗
DOE OSTI2025

Strontium‐Enriched Barite for Enhanced PbSO 4 Nucleation in Lead‐Acid Batteries

Abstract Barite (BaSO 4 ) crystals are an important additive in lead acid batteries due to their ability to promote the controlled nucleation and growth of anglesite (PbSO 4 ) during battery cycling. This is due to BaSO 4 ’s isostructural match with PbSO 4 , which facilitates epitaxial nucleation. However, BaSO 4 ’s efficacy as a nucleation promoter is limited by lattice mismatches between the two phases of 1–5%. Here, strontium‐enriched barite, (Ba,Sr)SO 4 , is synthesized to produce a nucleating promoter that displays an improved lattice match with PbSO 4 . Nucleation of PbSO 4 from Pb‐rich sulfuric acid solutions on strontium‐free and strontium‐enriched barite (up to 17 mol% Sr) is investigated using in‐situ atomic force microscopy and optical microscopy. At low strontium concentrations, PbSO 4 forms by the Stranski–Krastanov growth pathway (monolayer + island formation), with most nucleation occurring on edges and surface defects. At higher concentrations, the layer‐by‐layer growth mechanism known as Frank van‐der‐Merwe growth is observed, which allows for facile growth of continuous PbSO 4 films across the BaSO 4 surface. These films are successfully re‐dissolved on exposure to Pb‐free sulfuric acid. The results show that strontium incorporation fundamentally alters the mechanism of PbSO 4 nucleation on BaSO 4 , and thus provides a potential avenue for creating improved nucleation promoters in lead‐acid batteries.

Campbell, Colin T. [Pacific Northwest National Lab↗
DOE OSTI2026

Why Seeding Works When Nucleation Barriers Vanish

Crystallization is a process governed by the interplay between nucleation and growth. While crystalline seeds are known to reduce nucleation barriers and accelerate crystallization under nucleation-limited conditions, their influence when nucleation is not the limiting step remains poorly understood. This creates a mechanistic puzzle in systems where nucleation barriers are already negligible, yet seeding still accelerates crystallization. Here, the synthesis of zeolites is a quintessential example of growth-limited crystallization in which seeds accelerate the process despite negligible homogeneous nucleation barriers. Using coarse-grained molecular dynamics simulations─validated across two zeolites and the unrelated case of ice crystallization─we establish that growth-limited crystallization produces many small, misoriented crystallites whose slow coarsening into larger domains controls the emergence of X-ray-detectable crystallinity. Local crystalline order, structural coherence, and X-ray detectability are therefore kinetically decoupled milestones: the first can be reached rapidly while the latter two lag significantly. Seeds resolve this lag by imposing a common orientational registry on nascent crystallites, enabling their coherent coalescence into large seed-bound domains. This early coherence-building step produces a crystallite-size asymmetry that accelerates subsequent coarsening, advancing the onset of X-ray-detectable crystallinity without necessarily increasing the nucleated fraction. We conclude that under growth-limited conditions, the apparent induction period observed in powder X-ray diffraction reflects the time required to build long-range coherence, not the time to form crystalline material. Accordingly, seeds function not primarily by reducing nucleation barriers but by enforcing spatial coherence, thereby shortening the time required to develop long-range order detectable by X-ray diffraction.

Growth-Limited Crystallization↗
DOE OSTI2018

Forward flux sampling calculation of homogeneous nucleation rates from aqueous NaCl solutions

We used molecular dynamics simulations and the path sampling technique known as forward flux sampling to study homogeneous nucleation of NaCl crystals from supersaturated aqueous solutions at 298 K and 1 bar. Nucleation rates were obtained for a range of salt concentrations for the Joung-Cheatham NaCl force field combined with the Extended Simple Point Charge (SPC/E) water model. The calculated nucleation rates are significantly lower than the available experimental measurements. The estimates for the nucleation rates in this work do not rely on classical nucleation theory, but the pathways observed in the simulations suggest that the nucleation process is better described by classical nucleation theory than an alternative interpretation based on Ostwald’s step rule, in contrast to some prior simulations of related models. In addition to the size of NaCl nucleus, we find that the crystallinity of a nascent cluster plays an important role in the nucleation process. Nuclei with high crystallinity were found to have higher growth probability and longer lifetimes, possibly because they are less exposed to hydration water.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Cooperative actin filament nucleation by the Arp2/3 complex and formins maintains the homeostatic cortical array in Arabidopsis epidermal cells

Abstract Precise control over how and where actin filaments are created leads to the construction of unique cytoskeletal arrays within a common cytoplasm. Actin filament nucleators are key players in this activity and include the conserved actin-related protein 2/3 (Arp2/3) complex as well as a large family of formins. In some eukaryotic cells, these nucleators compete for a common pool of actin monomers and loss of one favors the activity of the other. To test whether this mechanism is conserved, we combined the ability to image single filament dynamics in the homeostatic cortical actin array of living Arabidopsis (Arabidopsis thaliana) epidermal cells with genetic and/or small molecule inhibitor approaches to stably or acutely disrupt nucleator activity. We found that Arp2/3 mutants or acute CK-666 treatment markedly reduced the frequency of side-branched nucleation events as well as overall actin filament abundance. We also confirmed that plant formins contribute to side-branched filament nucleation in vivo. Surprisingly, simultaneous inhibition of both classes of nucleator increased overall actin filament abundance and enhanced the frequency of de novo nucleation events by an unknown mechanism. Collectively, our findings suggest that multiple actin nucleation mechanisms cooperate to generate and maintain the homeostatic cortical array of plant epidermal cells.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2015

A comprehensive laboratory study on the immersion freezing behavior of illite NX particles. A comparison of 17 ice nucleation measurement techniques

Immersion freezing is the most relevant heterogeneous ice nucleation mechanism through which ice crystals are formed in mixed-phase clouds. In recent years, an increasing number of laboratory experiments utilizing a variety of instruments have examined immersion freezing activity of atmospherically relevant ice-nucleating particles. However, an intercomparison of these laboratory results is a difficult task because investigators have used different ice nucleation (IN) measurement methods to produce these results. A remaining challenge is to explore the sensitivity and accuracy of these techniques and to understand how the IN results are potentially influenced or biased by experimental parameters associated with these techniques. Within the framework of INUIT (Ice Nuclei Research Unit), we distributed an illite-rich sample (illite NX) as a representative surrogate for atmospheric mineral dust particles to investigators to perform immersion freezing experiments using different IN measurement methods and to obtain IN data as a function of particle concentration, temperature ( T ), cooling rate and nucleation time. A total of 17 measurement methods were involved in the data intercomparison. Experiments with seven instruments started with the test sample pre-suspended in water before cooling, while 10 other instruments employed water vapor condensation onto dry-dispersed particles followed by immersion freezing. The resulting comprehensive immersion freezing data set was evaluated using the ice nucleation active surface-site density, n s , to develop a representative n s ( T ) spectrum that spans a wide temperature range (-37 °C < T < -11 °C) and covers 9 orders of magnitude in n s . In general, the 17 immersion freezing measurement techniques deviate, within a range of about 8 °C in terms of temperature, by 3 orders of magnitude with respect to n s . In addition, we show evidence that the immersion freezing efficiency expressed in n s of illite NX particles is relatively independent of droplet size, particle mass in suspension, particle size and cooling rate during freezing. A strong temperature dependence and weak time and size dependence of the immersion freezing efficiency of illite-rich clay mineral particles enabled the n s parameterization solely as a function of temperature. We also characterized the n s ( T ) spectra and identified a section with a steep slope between -20 and -27 °C, where a large fraction of active sites of our test dust may trigger immersion freezing. This slope was followed by a region with a gentler slope at temperatures below -27 °C. While the agreement between different instruments was reasonable below ~ -27 °C, there seemed to be a different trend in the temperature-dependent ice nucleation activity from the suspension and dry-dispersed particle measurements for this mineral dust, in particular at higher temperatures. For instance, the ice nucleation activity expressed in n s was smaller for the average of the wet suspended samples and higher for the average of the dry-dispersed aerosol samples between about -27 and -18 °C. Only instruments making measurements with wet suspended samples were able to measure ice nucleation above -18 °C. A possible explanation for the deviation between -27 and -18 °C is discussed. Multiple exponential distribution fits in both linear and log space for both specific surface area-based n s ( T ) and geometric surface area-based n s ( T ) are provided. These new fits, constrained by using identical reference samples, will help to compare IN measurement methods that are not included in the present study and IN data from future IN instruments.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Complex plant-derived organic aerosol as ice-nucleating particles – more than the sums of their parts?

Quantifying the impact of complex organic particles on the formation of ice crystals in clouds remains challenging, mostly due to the vast number of different sources ranging from sea spray to agricultural areas. In particular, there are many open questions regarding the ice nucleation properties of organic particles released from terrestrial sources such as decaying plant material. In this work, we present results from laboratory studies investigating the immersion freezing properties of individual organic compounds commonly found in plant tissue and complex organic aerosol particles from vegetated environments, without specifically investigating the contribution from biological particles, which may contribute to the overall ice nucleation efficiency observed at high temperatures. To characterize the ice nucleation properties of plant-related aerosol samples for temperatures between 242 and 267 K, we used the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud chamber and the Ice Nucleation SpEctrometer of the Karlsruhe Institute of Technology (INSEKT), which is a droplet freezing assay. Individual plant components (polysaccharides, lignin, soy and rice protein) were mostly less ice active, or similarly ice active, compared to microcrystalline cellulose, which has been suggested by recent studies to be a proxy for quantifying the primary cloud ice formation caused by particles originating from vegetation. In contrast, samples from ambient sources with a complex organic matter composition (agricultural soils and leaf litter) were either similarly ice active or up to 2 orders of magnitude more ice active than cellulose. Of all individual organic plant components, only carnauba wax (i.e., lipids) showed a similarly high ice nucleation activity as that of the samples from vegetated environments over a temperature range between 245 and 252 K. Hence, based on our experimental results, we suggest considering cellulose as being representative for the average ice nucleation activity of plant-derived particles, whereas lignin and plant proteins tend to provide a lower limit. In contrast, complex biogenic particles may exhibit ice nucleation activities which are up to 2 orders of magnitude higher than observed for cellulose, making ambient plant-derived particles a potentially important contributor to the population of ice-nucleating particles in the troposphere, even though major uncertainties regarding their transport to cloud altitude remain.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Ice nucleation measurements from DRUM impactors during TRACER campaign in the Houston TX region from July to September 2022

During TRACER, three Davis Rotating Uniform size-cut Monitors (DRUM; DRUMAir 4-DRUM) were used to collect aerosols for ice nucleation measurements in the Brooks laboratory at Texas A&M University. The three instruments were located at AMF1 in La Porte, Ancillary site in Guy (ANC), and onboard the Texas A&M Rapid Onsite Atmospheric Measurements Van (ROAM-V). ROAM-V was deployed to capture airmasses behind (maritime) and ahead (continental) of the passage of the sea-breeze front through Houston. On select sampling days, ROAM-V sampled in the morning/mid-day on the coast and then transited to a second inland site for the afternoon/evening. The suite of instruments deployed on ROAM-V included a Condensation Particle Counter (CPC; GRIMM Model 5.403 CPC), Scanning Mobility Particle Sizer (SMPS; TSI 3750 detector, TSI 3082 classifier, TSI 3088 neutralizer, TSI 3081A Differential Mobility Analyzer), Cloud Condensation Nuclei counter (Droplet Measurement Technologies CCN Counter), micro pulse lidar (Droplet Measurement Technologies Micro Pulse LiDAR (miniMPL)), and one of the Davis Rotating Uniform size-cut Monitors (DRUM; DRUMAir 4-DRUM). Before sampling at each location, the latitude and longitude were recorded using the GPS on the phone application “My Altitude”. Each DRUM sampler was operated at a flow rate of 23 LPM. Each DRUM has four stages where the aerodynamic diameter size cuts are as follows: stage 1 larger than 3 μm, stage 2 from 3 to 1.2 μm, stage 3 from 1.2 to 0.34 μm, and stage 4 from 0.34 to 0.15 μm. Pretreated aluminum foil was used as a substrate on all stages. At AMF1 and ANC sites, the DRUMs were operated on the shared aerosol inlet, with generous support of the DOE ARM site staff. These instruments rotated 24 mm per day and only contained aluminum foil substrates. Substrates were changed weekly and transported to Texas A&M for storage in -80C freezer until analysis. The DRUM onboard ROAM-V was operated at a faster rotation rate of 150 mm per day to clearly separate the multiple deployment locations for ROAM-V. For the ROAM-V DRUM, substrates were changed every deployment and transported to Texas A&M for storage in -80C freezer until analysis. At Texas A&M, ice nucleation experiments were conducted to measure the ice nucleation temperature of the ambient aerosol samples collected from the three DRUMs using our previously established procedures (Alsante et al., 2023; Fornea et al., 2009; Matthews et al., 2023). For ice nucleation, only samples collected on stage 3 were analyzed, given that these are the most relevant size (1.2 to 0.34 μm diameter) for potential ice nucleating particles. For the AMF1 and ANC sites, we cut and analyzed 2 mm (2-hour) samples. We analyzed the time periods of the AMF1 site instrument when the ROAM-V was deployed. A 72-hour period from July 11th at 23:49 through July 15th at 1:49 was analyzed from the ANC site instrument. For the ROAM-V instrument, we separated the daily samples by site location. Between 1- and 6-hour independent samples were analyzed at each location. We also cut the ROAM-V samples in half to allow for compositional analysis of the aerosol on the other half of the substrate. All viable samples from the ROAM-V were analyzed. Analysis was done using a custom-built ice nucleation apparatus, recently updated to include an array of 16 individual samples (Matthews et al., 2023). On our experimental setup, we used 100 μL of Ultra-High-Performance Liquid Chromatography (UHPLC) water (Sigma Aldrich, >99.9% purity) to wash off the aerosol from the DRUM substrate. Then, we micropipetted 2 μL droplet samples into each of the 16 wells of the array, using hydrophobically coated microscope slides. Experiments would cycle 28 times from 10 C to -40C over a 20-hour period. During analysis of the TRACER samples, nine experiments were conducted with UHPLC water process blanks that followed an identical preparation procedure. The average freezing temperature and standard deviation for these process blanks is -27.7±2.4 C. This data was collected for ARM Field Campaign AFC07023 and supported by DOE ASR grant DE-SC0021047. For any further questions, please feel free to contact the instrument PI, Sarah D. Brooks, sbrooks@tamu.edu. Alsante, A. N., Thornton, D. C., & Brooks, S. D. (2023). Ice nucleation catalyzed by the photosynthesis enzyme RuBisCO and other abundant biomolecules. Communications Earth & Environment, 4(1), 51. Fornea, A. P., Brooks, S. D., Dooley, J. B., & Saha, A. (2009). Heterogeneous freezing of ice on atmospheric aerosols containing ash, soot, and soil. Journal of Geophysical Research: Atmospheres, 114(D13). DOI:10.1029/2009JD011958 Matthews, B. H., Alsante, A. N., & Brooks, S. D. (2023). Pollen Emissions of Subpollen Particles and Ice Nucleating Particles. ACS Earth and Space Chemistry.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1997

Colloids and Nucleation

The objectives of the work funded under this grant were to develop a microphotographic technique and use it to monitor the nucleation and growth of crystals of hard colloidal spheres. Special attention is given to the possible need for microgravity studies in future experiments. A number of persons have been involved in this work. A masters student, Keith Davis, began the project and developed a sheet illumination apparatus and an image processing system for detection and analysis. His work on a segmentation program for image processing was sufficient for his master's research and has been published. A post doctoral student Bernie Olivier and a graduate student Yueming He, who originally suggested the sheet illumination, were funded by another source but along with Keith made photographic series of several samples (that had been made by Keith Davis). Data extraction has been done by Keith, Bernie, Yueming and two undergraduates employed on the grant. Results are published in Langmuir. These results describe the sheet lighting technique as one which illuminates not only the Bragg scattering crystal, but all the crystals. Thus, accurate crystal counts can be made for nucleation rate measurements. The strange crystal length scale reduction, observed in small angle light scattering (SALS) studies, following the initial nucleation and growth period, has been observed directly. The Bragg scattering (and dark) crystal size decreases in the crossover region. This could be an effect due to gravitational forces or due to over- compression of the crystal during growth. Direct observations indicate a complex morphology for the resulting hard sphere crystals. The crystal edges are fairly sharp but the crystals have a large degree of internal structure. This structure is a result of (unstable) growth and not aggregation. As yet unpublished work compares growth exponents data with data obtained by SALS. The nucleation rate density is determined over a broad volume fraction range (0.505 to 0.575) and compared to classical nucleation rate calculations. The experimental nucleation rate density varies with volume fraction more slowly than expected theoretically. Gravity may influence nucleation because crystal nuclei are more dense than the surrounding fluid and may be gravitationally convected. The largest observed crystal size was near volume fraction 0.52. Near the freezing point, crystals should grow to large size because nuclei are sparse and there is plenty of room to grow without contacting other crystals. Near melting the opposite is true, with crystals growing into one another shortly after nucleation. The maximum crystal size seen near 0.52 volume fraction suggests that gravitational stresses are limiting crystal growth near freezing.

Ackerson, Bruce↗
DOE OSTI2023

Surface Functional Groups Affect Iron (Hydr)oxide Heterogeneous Nucleation: Implications for Membrane Scaling

Because of its favorable thermodynamics and fast kinetics, heterogeneous solid nucleation on membranes triggers early-stage mineral scaling. Iron (hydr)oxide, a typical membrane scale, initially forms as nanoparticles that interact with surface functional groups on membranes, but these nanoscale phenomena are difficult to observe in real time. In this study, we utilized in situ grazing incidence small angle X-ray scattering and ex situ atomic force microscopy to examine the heterogeneous nucleation of iron (hydr)oxide on surface functional groups commonly used in membranes, including hydroxyl (OH), carboxyl (COOH), and fluoro (F) groups. We found that, compared to nucleation on hydrophilic OH- and COOH-surfaces, the high hydrophobicity of an F-modified surface significantly reduced the extents of both heterogeneously and homogeneously formed iron (hydr)oxide nucleation. Moreover, on the OH-surface, the high functional group density of 0.76 nmol/cm 2 caused faster heterogeneous nucleation than that on a COOH-surface, with a density of 0.28 ± 0.04 nmol/cm 2 . The F-surface also had the highest heterogeneous nucleation energy barrier (26 ± 0.6 kJ/mol), followed by COOH- (23 ±0.8 kJ/mol) and OH- (20 ± 0.9 kJ/mol) surfaces. The kinetic and thermodynamic information provided here will help us better predict the rates and extents of early-stage scaling of iron (hydr)oxide nanoparticles in membrane processes. Finally, this work provides both kinetic and thermodynamic information about iron (hydr)oxide nucleation controlled by membrane-related functional groups (OH, COOH, and F).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Electric Field’s Dueling Effects through Dehydration and Ion Separation in Driving NaCl Nucleation at Charged Nanoconfined Interfaces

Investigating nucleation in charged nanoconfined environments under electric fields is crucial for many scientific and engineering applications. Here we study the nucleation of NaCl from aqueous solution near charged surfaces using machine-learning-augmented enhanced sampling molecular dynamics simulations. Our simulations successfully drive phase transitions between the liquid and solid phases of NaCl. The solid phase is stabilized under electric fields, particularly at an intermediate surface charge density. We examine which physical characteristics drive the nucleation of NaCl from aqueous solutions and find that the removal of solvent water from Cl– at the solid precursor surface plays a more critical role than the accumulation of ions. Our simulations reveal the competing effects of electric fields on nucleation processes: they facilitate the removal of water, promoting nucleation, but also promote the separation of ion pairs, thereby hindering nucleation. Here, this work provides a framework for studying nucleation processes in nanoconfined environments under electric fields and provides physical insights for the design of electrochemistry materials.

Electric fields↗
DOE OSTI2019

Engineering Nucleation Kinetics of Graphite Nodules in Inoculated Cast Iron for Reducing Porosity

Inoculation of cast iron with spherical graphite (SGI) controls nucleation kinetics of graphite nodules and is used for improving casting performance and eliminating solidification micro-porosity. In this study, thermodynamic simulations were used to design inoculants. Thermal and chemical stability of different potential heterogeneous nuclei formed in the melt above the liquidus temperature and in the mushy zone during solidification was predicted. Several inoculation treatments of SGI were performed in laboratory heats. An automated SEM/EDX analysis was applied to examine the graphite nodule size distribution and the family of the non-metallic inclusions in the experimental castings. The data were used to reconstruct a relative graphite nodule nucleation rate in the castings. It was shown that the graphite nodule nucleation kinetics in the castings were significantly different from those predicted by classical nucleation models. In inoculated SGI, the observed bi-modal distribution of graphite nodules was related to a continuous nucleation that occurred towards the end of solidification. The origin of the continuous nucleation and the possibility of engineering graphite nodules nucleation kinetics to control SGI casting soundness by inoculation are discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Crack nucleation from non-metallic inclusions in aluminum alloys described by peridynamics simulations

Conventional engineering methods oftentimes have challenges in the quantification of crack nucleation processes from manufacturing defects that are relevant for engineering component lifing. In this work, we present peridynamic simulation framework for the description of the crack nucleation process from cluster of non-metallic inclusions in aluminum alloys. Our non-local simulation framework characterizes crack nucleation process as multiple micro-crack nucleation events from individual inclusions, and eventually one micro-crack dominates. We define individual stages of the crack nucleation process, i.e., nucleation, micro-crack, technical, and crack initiation, that allow a quantification and meta model development of both the individual stages and the entire crack nucleation process.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Statistical evaluation of microscale stress conditions leading to void nucleation in the weak shock regime

Here, we investigate the heterogeneity of the stress state driven by anisotropic deformation response at the single crystal level through five statistical volume element (SVE) calculations of polycrystalline BCC tantalum. This work focuses on grain boundaries as a prominent material defect type prone to void nucleation based upon experimental observations of predominantly intergranular void nucleation in this material. The SVEs are constructed to be statistically representative of larger volumes of material and are meshed such that mean and standard deviation of grain size and orientation information is reconstructed. The computational meshes feature hexahedral (brick) elements and smooth conformal grain boundaries where significant stress concentration is known to occur, a tail effect of interest in the extreme events process of dynamic ductile damage. An existing micromechanical crystallographic plasticity model shown to capture the single crystal behavior of BCC tantalum well is used to perform the polycrystal calculations. The model includes representation of the non-Schmid effect of non-planar screw dislocation kinetics in tantalum. A three-dimensional stress state time profile predicted by damage modeling of a flyer plate impact experiment is applied as boundary conditions to each SVE. Resulting grain boundary stress state statistics are strongly non-Gaussian. Significant structural evolution is observed within the compressive hold before unloading into tension in the stress profile. Strong angular dependence of grain boundary traction magnitude with shock direction is observed. Non-Schmid effects continue to suggest their influence on propensity of microstructural defect types to nucleate voids. A general void nucleation criterion is proposed using probability theory. The general framework is specified to polycrystalline BCC tantalum in the weak shock regime to include the SVE calculations and literature molecular dynamics calculations of grain boundary void nucleation strength. Probability density functions (PDFs) are used to describe the interaction between the local stress state heterogeneity and the distributed grain boundary void nucleation strength state. A causation entropy maximization procedure removes the requirement for ad hoc selection of a PDF functional form and provides a rigorous procedure for data-based PDF determination. The resulting physically informed PDF describes the spatial appearance frequency of nucleated voids as a function of applied macroscale pressure. Lower length scale physics are thus packaged in a precise and computationally efficient way to provide computational plasticity insight to macroscale dynamic ductile damage models.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Effects of Mg-Al-O-Mn-S inclusion on the nucleation of acicular ferrite in magnesium-containing low-carbon steel

Highlights: • We redefine the mechanism of AF nucleation from Gibbs free energy of nucleation. • Complex inclusions present a better ability of inducing AF formation due to the Mn-depleted zone. • The lattice misfit and the thermal strain are calculated in this study. - Abstract: The effects of inclusion size and chemical composition on acicular ferrite (AF) nucleation and possible nucleation mechanisms were discussed. With the use of low-carbon structure steel containing 13 ppm Mg, the chemical composition and size of inclusions were quantified by scanning electron microscopy combined with an energy dispersive spectroscopy system. Results showed that the complex inclusions MgO-MnS and MgO-Al{sub 2}O{sub 3}-MnS are the most effective inclusions for inducing AF nucleation in Mg-containing A36, and their probabilities of AF nucleation are 35.8% and 41.4%, respectively. Moreover, the inclusion size in the range of 1–2 μm exhibits the most remarkable ability to induce AF formation. AF nucleates at the interface of MgO and MgO-Al{sub 2}O{sub 3} because of the low lattice misfit with AF. Complex inclusions, such as MgO-MnS and MgO-Al{sub 2}O{sub 3}-MnS, present a better ability of inducing AF formation than that of MnS due to the Mn-depleted zone.

36 MATERIALS SCIENCE↗
DOE OSTI2022

High-fidelity pool boiling simulations on multiple nucleation sites using interface capturing method

Boiling has proved to be one of the most efficient means for heat transfer and is a very important phenomenon during severe accident scenarios in light water reactors. High-fidelity pool boiling simulations can provide a numerical database for improving mechanistic boiling models by allowing for specific evaluation of interactions among bubbles. Previously published pool boiling simulations investigated two nucleation sites in which bubble growth at one site suppressed nucleation at the other site. Based on previous study results, more complicated interface-capturing simulations on pool boiling were conducted using PHASTA code with locally refined unstructured mesh. First, different boundary conditions (BCs) were assessed to support robustness and reproducibility of the boiling model. Then, a scale study was conducted at a larger domain with nine nucleation sites where either nine or four nucleation sites are activated. Involving more nucleation sites increased the complexity of bubble interactions from surrounding sites. Finally, bubble departure behavior influenced by wall heat flux was investigated. In this work, when heat flux was increased, the order of bubble departure changed, but diagonal bubbles always departed after one another. The departure time interval between the first and second bubble reduced as heat flux increased. The corresponding frequency was almost linearly proportional to the heat flux. In addition, bubble departure behavior was found to be greatly influenced by the nucleation site pattern. Multiple nucleation sites resulted in superimposed inhibitive effects from surrounding sites to each bubble, which extensively delayed the departure. This new observation was not discussed in previously published works. The work presented here provides new insight on the fundamental understanding of boiling phenomena, contributes to the development of a 3D multiphase computational fluid dynamics (M-CFD) model, and provides a more comprehensive database for data-driven pool boiling studies.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2018

The Role of Organic Aerosol in Atmospheric Ice Nucleation: A Review

Predicting the formation of ice crystals in the atmosphere presents one of the great challenges in physical sciences with important implications for the chemistry and composition of the Earth’s atmosphere, the hydrological cycle, and climate. Among atmospheric ice formation processes, heterogeneous ice nucleation proceeds on aerosol particles ranging from a few nanometers to micrometers in size, commonly referred to as ice nucleating particles (INPs). Research over the last two decades has demonstrated that organic matter (OM) is ubiquitous in the atmosphere, present as organic aerosol (OA) particles or as coatings on other particle types. While it is well understood that mineral dust particles can induce ice nucleation under atmospheric conditions, it is currently not clear how much OA particles including pollution aerosol and secondary organic aerosol (SOA) contributes to the ambient INP population. The physicochemical properties of OM make predicting how OM interacts with water vapor leading ultimately to ice crystals challenging. This review focuses on the role of OM in INPs, summarizing and highlighting recent advances in our understanding of the ice nucleation process gained from theoretical, laboratory, and field studies. Examination of ice residuals and INPs with analytical techniques demonstrates that OM participates in atmospheric ice crystal formation. Molecular dynamic simulations provide insight into the microscopic processes that initiate ice nucleation. The amorphous phase state of OM in the supercooled and metastable regime is identified as a key factor in assessing the particles’ nucleation pathways and rates. A theoretical model is advanced, based on particle water activity, to holistically predict amorphous phase changes and ice nucleation rates of particles coated by OM. The goal of this review is to synthesize our current understanding and propose future research directions needed to fully evaluate how OA particles contribute to INPs in the atmosphere.

54 ENVIRONMENTAL SCIENCES↗