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NASA NTRS1994

Ionospheric projections of magnetospheric regions under low and high solar wind pressure conditions

The projection of magnetospheric regions into the dayside ionosphere as determined by particle precipitation characteristics was studied for dependence on solar wind parameters. It was found that the solar wind kinetic pressure p dramatically affected the map of magnetospheric projections. Under the constraint that p greater than or equal 4 nPa(yielding (p) = 5.9 nPa), the area of the cusp (magnetic latitude times magnetic local time extent) was 4.83 degree-hours; whereas under the constraint that p greater than or equal 2 nPa (yielding (p) = 1.5 nPa), the cusp area was only 1.01 degree-hours. The ionospheric footprint of the low-latitude boundary layer was similarly affected. Various possible correlations of p with other solar wind variables, including n, v, and absolute value of B(sub z), proved unable to account for the pressure effect. Because one criterion for identifying the cusp is high fluxes, the effect of nv was investigated with particular care, both in examples and statistically. Again, p itself had by far the most striking effect. Thus we concluded that some physical mechanism is needed to account for the pressure effect. One possibility is that increased direct solar wind plasma penetration of the magnetopause occurs under high-p conditions in the manner suggested by various proponents of impulsive penetration models. An alternative, which we find promising, is that, regardless of the original interplanetary magnetic field (IMF) strength, a high-p solar wind leads to a large compression factor for the magnetosheath field, which is the field actually in contact with the magnetosphere. From this latter viewpoint, the chief effect of high particle pressure is simply to enhance the effectiveness of the interaction of the IMF with the magnetosphere.

Newell, Patrick T.↗

NASA NTRS2005

Partially-Averaged Navier Stokes Model for Turbulence: Implementation and Validation

Partially-averaged Navier Stokes (PANS) is a suite of turbulence closure models of various modeled-to-resolved scale ratios ranging from Reynolds-averaged Navier Stokes (RANS) to Navier-Stokes (direct numerical simulations). The objective of PANS, like hybrid models, is to resolve large scale structures at reasonable computational expense. The modeled-to-resolved scale ratio or the level of physical resolution in PANS is quantified by two parameters: the unresolved-to-total ratios of kinetic energy (f(sub k)) and dissipation (f(sub epsilon)). The unresolved-scale stress is modeled with the Boussinesq approximation and modeled transport equations are solved for the unresolved kinetic energy and dissipation. In this paper, we first present a brief discussion of the PANS philosophy followed by a description of the implementation procedure and finally perform preliminary evaluation in benchmark problems.

Girimaji, Sharath S.↗

NASA NTRS2007

Multi-Scale Modeling of Magnetospheric Reconnection

One of the major challenges in modeling the magnetospheric magnetic reconnection is to quantify the interaction between large-scale global magnetospheric dynamics and microphysical processes in diffusion regions near reconnection sites. There is still considerable debate as to what degree microphysical processes on kinetic scales affect the global evolution and how important it is to substitute numerical dissipation and/or ad hoc anomalous resistivity by a physically motivated model of dissipation. Comparative studies of magnetic reconnection in small scale geometries demonstrated that MHD simulations that included non-ideal processes in terms of a resistive term $\eta J$ did not produce the fast reconnection rates observed in kinetic simulations. For a broad range of physical parameters in collisionless magnetospheric plasma, the primary mechanism controlling the dissipation in the vicinity of the reconnection site is non-gyrotropic effects with spatial scales comparable with the particle Larmor radius. We utilize the global MHD code BATSRUS and incorporate nongyrotropic effects in diffusion regions in terms of corrections to the induction equation. We developed an algorithm to search for magnetotail reconnection sites, specifically where the magnetic field components perpendicular to the local current direction approaches zero and form an X-type configuration. Spatial scales of the diffusion region and magnitude of the reconnection electric field are calculated selfconsistently using MHD plasma and field parameters in the vicinity of the reconnection site. The location of the reconnection sites is updated during the simulations. To clarify the role of nongyrotropic effects in diffusion region on the global magnetospheric dynamic we perform simulations with steady southward IMF driving of the magnetosphere. Ideal MHD simulations with magnetic reconnection supported by numerical resistivity produce steady configuration with almost stationary near-earth neutral line (NENL). Simulations with non-gyrotropic corrections demonstrate dynamic quasi-periodic response to the steady driving condition. The loading/unloading cycle in non-gyrotropic MHD results has a non-stationary reconnection site in the magnetotail, with the retreating during the stretching phase and then a new NENL forming in the resulting thin plasma sheet. We expect that this model will lead to improved representations of space weather event in the magnetosphere.

Kuznetsova, M. M.↗

NASA NTRS1978

A study of the atmospheric energetics of a six-layer operational forecast model

Verification data for twice-daily analyses of horizontal wind and temperature are compared with 00, 12, 24, 36, 60, and 84 hour forecasts prepared for winter 1975-76 from a six-layer operational forecast model; the comparison focuses on certain energy components in the forecast fields. Significant losses (15 to 20%) of zonal available potential energy and zonal kinetic energy appear beyond the 36-hour forecasts; the zonal kinetic energy loss is associated with a large increase in this parameter during the first 12-hour forecast period, due to a downward and northward movement of the mean jet-stream core. In addition, energy losses in the eddy potential and kinetic energy components are noted in the initialization procedure.

Hauser, R. K.↗

DOE OSTI2025

Data-Driven Tailoring Optimization of Thermoset Polymers Using Ultrasonics and Machine Learning

Thermoset polymers are highly demanded for their structural robustness, thermal stability, and chemical resistance. Tailoring the properties of these polymers for high-performance applications is often preferred to designing brand-new polymers. However, the traditional destructive techniques used to characterize their properties as a function of manufacturing parameters are expensive and time-consuming. A novel non-destructive, data-driven method leveraging ultrasonics and machine learning techniques to tailor the properties of thermosets as a function of the manufacturing parameters is demonstrated. Thermoset epoxy samples with varying curing temperatures (15–40 °C) and curing agent amounts (±40%) were manufactured and tested. Their curing kinetics were monitored by determining the sound speed in the material in real time, while the longitudinal modulus of the samples was determined post-cure. Machine learning models were developed using a k-nearest neighbors algorithm. These models were implemented to predict the curing and final elastic properties using the manufacturing parameters, i.e., stoichiometry and curing temperature, and vice versa. Understanding and modeling how these parameters affect the cure kinetics and final properties will allow for efficient and reliable optimization of thermoset tailoring and manufacturing.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Suppressing the enhancement of stimulated Raman scattering in inhomogeneous plasmas by tuning the modulation frequency of a broadband laser

The stimulated Raman scattering (SRS) instability can inhibit the performance of laser driven inertial confinement fusion (ICF) implosions by scattering light into unwanted directions or by generating hot electrons that preheat the target fuel. In principle, ICF target designs can avoid parameter regimes conducive to large, linear SRS gains. In practice, kinetic inflation—the nonlinear enhancement of SRS due to electron trapping in the excited plasma wave—makes this difficult. Here we show that laser bandwidth in the form of frequency modulation can either decrease or increase the inflationary SRS (iSRS) threshold in inhomogeneous plasmas depending on the maximum chirp of the laser pulse. The threshold, mapped out by a series of particle-in-cell simulations, exhibits a minimum when the frequency change within the pulse cancels the spatial detuning due to density inhomogeneities along the trajectory of the scattered light. In conclusion, by tuning the pump laser parameters away from this minimum, the iSRS threshold can be larger than at zero bandwidth, providing a path to mitigating kinetic inflation in ignition relevant plasmas.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Additive friction stir deposition of SS316: Effect of process parameters on microstructure evolution

Solid state nature of additive friction stir deposition (AFSD) additive manufacturing process is very advantageous in terms of defect formation and microstructural refinement in the material. Current study presents the process optimization, microstructural evolution and kinetics of recrystallization for AFSD deposited low stacking fault energy material - SS316. As deposited microstructure shows equiaxed ultra fine grains with an average grain size of ~5.0 ± 0.5 μm. Shear deformation at high temperature during processing leads to the operation of restoration mechanisms. Observation of necklace type microstructure in the as deposited SS316 is attributed to discontinuous dynamic recrystallization during processing. Recrystallization kinetics of the AFSD SS316 is characterized using Johnson-Mehl-Avarami-Kolmogorov (JMAK) model. Deformation – thermal cycling during AFSD process resulted in inconsistent recrystallization kinetics. Variation in strain, strain rate and temperature during processing with processing parameters result in varying microstructure and tool wear. Further, high strength-ductility combination and sustained work hardening in as deposited SS316 appear to arise from transformation and twinning during deformation, leading to the formation of hierarchical twins and martensitic phase after deformation.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Generation and Study of Am(IV) by Temperature-Controlled Electron Pulse Radiolysis

Used nuclear fuel (UNF) separation techniques that strive to separate radiotoxic americium (Am) from trivalent lanthanide fission products through oxidation state control have increased research efforts surrounding Am(V) and Am(VI). However, equivalent knowledge of the tetravalent state, Am(IV), has remained elusive, particularly in conditions more representative of UNF reprocessing, i.e., in concentrated nitric acid (HNO3). With this in mind, we have used electron pulse radiolysis to study the radiation-induced redox reaction of Am(III) with the oxidizing nitrate radical (NO3?) in 6 M HNO3: Am(III) + NO3? ? Am(IV) + NO3? . These experiments enabled us to observe the growth and decay of Am(IV) in a concentrated acidic solution for the first time. The transient Am(IV) species was found to have a lifetime of ~16 µs?sufficiently long-lived to play a critical mechanistic role in UNF reprocessing systems. Additionally, we performed the first-ever temperature-dependent kinetics study of an actinide element, elucidating unprecedented Arrhenius and Eyring activation parameters for the reaction of Am(III) with NO3?. This new knowledge provides much-needed molecular-level insights into the radiation-induced behavior of Am.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

NASA NTRS1980

Solar-pumped gas laser development

A survey of gas properties through detailed kinetic models led to the identification of critical gas parameters for use in choosing appropriate gas combinations for solar pumped lasers. Broadband photoabsorption in the visible or near UV range is required to excite large volumes of gas and to insure good solar absorption efficiency. The photoexcitation density is independent of the absorption bandwidth. The state excited must be a metastable state which is not quenched by the parent gas. The emission bandwidth must be less than 10 A to insure lasing threshold over reasonable gain lengths. The system should show a high degree of chemical reversibility and an insensitivity to increasing temperature. Other properties such as good quantum efficiency and kinetic efficiency are also implied. Although photoexcitation of electronic vibrational transitions is considered as a possible system if the emission bands sufficiently narrow, it appears that photodissociation into atomic metastables is more likely to result in a successful solar pumped laser system.

Wilson, J. W.↗

DOE OSTI2022

A learned closure method applied to phase mixing in a turbulent gradient-driven gyrokinetic system in simple geometry

We present a new method for formulating closures that learn from kinetic simulation data. We apply this method to phase mixing in a simple gyrokinetic turbulent system – temperature-gradient-driven turbulence in an unsheared slab. The closure, called the learned multi-mode (LMM) closure, is constructed by, first, extracting an optimal basis from a nonlinear kinetic simulation using singular value decomposition. Subsequent nonlinear fluid simulations are projected onto this basis and the results are used to formulate the closure. We compare the closure with other closures schemes over a broad range of the relevant two-dimensional parameter space (collisionality and gradient drive). We find that the turbulent kinetic system produces phase-mixing rates much lower than the linear expectations, which the LMM closure is capable of capturing. We also compare radial heat fluxes. A Hammett–Perkins closure, generalized to include collisional effects, is quite successful throughout the parameter space, producing ${\sim }14\,\%$ root-mean-square (r.m.s.) error. The LMM closure is also very effective: when trained at three (two) points (in a 35 point parameter grid), the LMM closure produces $8\,\%$ ( $12\,\%$ ) r.m.s. errors. The LMM procedure can be readily generalized to other closure problems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2025

Internally Catalyzed Hydrogen Atom Transfer (I-CHAT)—A New Class of Reactions in Combustion Chemistry

The current paradigm of low-T combustion and autoignition of hydrocarbons is based on the sequential two-step oxygenation of fuel radicals. The key chain-branching occurs when the second oxygenation adduct (OOQOOH) is isomerized releasing an OH radical and a key ketohydroperoxide (KHP) intermediate. The subsequent homolytic dissociation of relatively weak O–O bonds in KHP generates two more radicals in the oxidation chain leading to ignition. Based on the recently introduced intramolecular “catalytic hydrogen atom transfer” mechanism (J. Phys. Chem. 2024, 128, 2169), abbreviated here as I-CHAT, we have identified a novel unimolecular decomposition channel for KHPs to form their classical isomers—enol hydroperoxides (EHP). The uncertainty in the contribution of enols is typically due to the high computed barriers for conventional (“direct”) keto–enol tautomerization. Remarkably, the I-CHAT dramatically reduces such barriers. The novel mechanism can be regarded as an intramolecular version of the intermolecular relay transfer of H-atoms mediated by an external molecule following the general classification of such processes (Catal. Rev.-Sci. Eng. 2014, 56, 403). Here, we present a detailed mechanistic and kinetic analysis of the I-CHAT-facilitated pathways applied to n-hexane, n-heptane, and n-pentane models as prototype molecules for gasoline, diesel, and hybrid rocket fuels. We particularly examined the formation kinetics and subsequent dissociation of the γ-enol-hydroperoxide isomer of the most abundant pentane-derived isomer γ-C5-KHP observed experimentally. To gain molecular-level insight into the I-CHAT catalysis, we have also explored the role of the internal catalyst moieties using truncated models. All applied models demonstrated a significant reduction in the isomerization barriers, primarily due to the decreased ring strain in transition states. In addition, the longer-range and sequential H-migration processes were also identified and illustrated via a combined double keto–enol conversion of heptane-2,6-diketo-4-hydroperoxide as a potential chain-branching model. To assess the possible impact of the I-CHAT channels on global fuel combustion characteristics, we performed a detailed kinetic analysis of the isomerization and decomposition of γ-C5-KHP comparing I-CHAT with key alternative reactions—direct dissociation and Korcek channels. Calculated rate parameters were implemented into a modified version of the n-pentane kinetic model developed earlier using RMG automated model generation tools (ACS Omega, 2023, 8, 4908). Simulations of ignition delay times revealed the significant effect of the new pathways, suggesting an important role of the I-CHAT pathways in the low-T combustion of large alkanes.

Biochemistry & Molecular Biology↗

DOE OSTI2025

Pyridine Catalysis of Anhydride Hydrolysis within Carbodiimide‐Driven Reaction Networks

Carbodiimide-fueled reaction networks offer a versatile platform for nonequilibrium chemical systems. Typically, the carbodiimide converts a carboxylic acid to its anhydride, called “activation,” which subsequently undergoes hydrolysis, called “deactivation.” Here, we investigate pyridines with variable nucleophilicity as catalysts to control deactivation (pyridine, 4-methylpyridine, 4-methoxypyridine, and 4-dimethylaminopyridine). Reactions have been monitored by NMR spectroscopy. Although this reaction network is simple, determination of well-defined rate constants from kinetic modeling is challenging because of correlation between the parameters. This issue can be addressed by analyzing the anhydride hydrolysis independently. The rate of attack of the pyridines on the anhydride follows expected nucleophilicity trends, although this is offset by increased protonation of more-nucleophilic pyridines at typical pH's. The optimized parameters can be used to model the full carbodiimide-driven process, although the presence of the common carbodiimide EDC has unanticipated effects on the anhydride hydrolysis rate. The results offer context for controlling carbodiimide-fueled reaction networks through the choice of suitable catalysts and pH.

Anhydrides↗

NASA NTRS2009

Physics of Reconnection and MMS Mission

Reconnection is the most important process driving the Earth's magnetosphere. Key to the success of the MMS science plan is the coupling of theory and observation. Determining the kinetic processes occurring in the diffusion region and physical parameters that control the rate of magnetic reconnection are among primary objectives of the MMS mission. Analysis of the role played by particle inertial effects in the diffusion region where the plasma is unmagnetized will be presented. The reconnection electric field in he diffusion region is supported primarily by particle non-gyrotropic effects. At the quasi-steady stage the reconnection electric field serves to accelerate and heat the incoming plasma population to maintain the current flow in the diffusion region the pressure balance. The primary mechanism controlling the dissipation in the vicinity of the reconnection site is incorporated into the fluid description in terms of non-gyrotropic corrections to the. induction and energy equations. The results of kinetic and fluid simulations illustrating the physics of magnetic reconnection will be presented. We will dem~:tistrate that kinetic nongyrotropic effects can significantly alter the global magnetosphere evolution and location of reconnection sites.

Kuznetsova, M. M.↗

DOE OSTI2021

Assessment the leaching characteristics and long-term leaching behavior of some radionuclides from synthesized zeolite cement matrix

Highlights: • Synthesis and characterization of zeolite cement synthesized from fly ash • Leaching tests were used to assess the release rate of {sup 85}Sr and {sup 60}Co radionuclides. • Simple mathematical models were used to detect leaching mechanisms. • Long-term leaching behavior of {sup 85}Sr and {sup 60}Co from cementitious matrix was assessed. The development of cementitious materials remains a vital goal to produce valuable products with good mechanical, physical and chemical properties suitable for the safe disposal of concentrated radionuclides resulted from the treatment of contaminated solutions. In this paper, zeolite cement with good properties was laboratory synthesized from industrial by-products fly ash and characterized using various characterization techniques. The leaching characteristics of strontium and cobalt radionuclides from the synthesized zeolite cement were scrutinized conforming with the standard leaching methodology of International Atomic Energy Authority (IAEA). A mechanical strength assessment was executed to characterize the extent of immobilization process of the solidified matrices. The cumulative leaching fraction (φ) of the two studied radionuclides was found to be less than 5% in all examined conditions, which implies the applicability of the IAEA-recommended methodology for estimating the diffusion coefficient. The experimental leaching data were regressed nonlinearly to various mathematical kinetic models to assess the controlling leaching mechanism and to determine the leaching parameters. The regression results indicated that strontium ({sup 85}Sr) and cobalt ({sup 60}Co) leaching resulted from two succeeding mechanisms: as first order kinetic reaction, and then diffusion. The calculated values of leachability indices signify that the performance of each of the studied matrices is within an acceptable range. A simplified mathematical model, rooted in the first order reaction and diffusion mechanisms, was simulated to predict the radionuclides leaching rates from zeolite cement matrices. By comparing the synthesized zeolite cement with other cementitious materials, it can be concluded that the synthesized material can be classified as an efficient material suitable to immobilize {sup 85}Sr and {sup 60}Co from radioactive wastes. The acquired findings demonstrated that the studied immobilized waste matrices have acceptable mechanical effectiveness.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Probabilistic and maximum entropy modeling of chemical reaction systems: Characteristics and comparisons to mass action kinetic models

We demonstrate and characterize a first-principles approach to modeling the mass action dynamics of metabolism. Starting from a basic definition of entropy expressed as a multinomial probability density using Boltzmann probabilities with standard chemical potentials, we derive and compare the free energy dissipation and the entropy production rates. We express the relation between entropy production and the chemical master equation for modeling metabolism, which unifies chemical kinetics and chemical thermodynamics. Because prediction uncertainty with respect to parameter variability is frequently a concern with mass action models utilizing rate constants, we compare and contrast the maximum entropy model, which has its own set of rate parameters, to a population of standard mass action models in which the rate constants are randomly chosen. We show that a maximum entropy model is characterized by a high probability of free energy dissipation rate and likewise entropy production rate, relative to other models. We then characterize the variability of the maximum entropy model predictions with respect to uncertainties in parameters (standard free energies of formation) and with respect to ionic strengths typically found in a cell.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Degradation of performance in ICF implosions due to Rayleigh–Taylor instabilities: A Hamiltonian perspective

The Rayleigh–Taylor instability (RTI) is an ubiquitous phenomenon that occurs in inertial-confinement-fusion (ICF) implosions and is recognized as an important limiting factor of ICF performance. To analytically understand the RTI dynamics and its impact on ICF capsule implosions, we develop a first-principle variational theory that describes an imploding spherical shell undergoing RTI. The model is based on a thin-shell approximation and includes the dynamical coupling between the imploding spherical shell and an adiabatically compressed fluid within its interior. Using a quasilinear analysis, we study the degradation trends of key ICF performance metrics (e.g., stagnation pressure, residual kinetic energy, and areal density) as functions of initial RTI parameters (e.g., the initial amplitude and Legendre mode), as well as the 1D implosion characteristics (e.g., the convergence ratio). We compare analytical results from the theory against nonlinear results obtained by numerically integrating the governing equations of this reduced model. Our findings emphasize the need to incorporate polar flows in the calculation of residual kinetic energy and demonstrate that higher convergence ratios in ICF implosions lead to significantly greater degradation of key performance metrics.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2024

DRDMannTurb: A Python package for scalable, data-driven synthetic turbulence

Synthetic turbulence models (STMs) are used in wind engineering to generate realistic flow fields and are employed as inputs to industrial wind simulations. Examples include prescribing inlet conditions in large eddy simulations that model loads on wind turbines and tall buildings. We are interested in STMs capable of generating fluctuations based on prescribed second-moment statistics since such models can simulate environmental conditions that closely resemble on-site observations. To this end, the widely used Mann model (see Mann, 1994, 1998) is the inspiration for DRDMannTurb. The Mann model is described by three physical parameters: a magnitude parameter influencing the global variance of the wind field and corresponding to the Kolmogorov constant multiplied by the rate of viscous dissipation of the turbulent kinetic energy to the two-thirds, αϵ 2/3 , a turbulence length scale parameter L, and a nondimensional parameter Γ related to the lifetime of the eddies. A number of studies, as well as international standards (e.g., those by the International Electrotechnical Commission (IEC)), include recommended values for these three parameters with the goal of standardizing wind simulations according to observed energy spectra. Yet, having only three parameters, the Mann model faces limitations in accurately representing the diversity of observable spectra. This Python package enables users to extend the Mann model and more accurately fit field measurements through flexible neural network models of the eddy lifetime function. Following Keith et al. (2021), we refer to this class of models as Deep Rapid Distortion (DRD) models. DRDMannTurb also includes a general module implementing an efficient method for synthetic turbulence generation based on a domain decomposition technique. This technique is also described in Keith et al. (2021).

17 WIND ENERGY↗

DOE OSTI2025

Transient kinetic insights into selective propene oxidation over industrial bismuth molybdate catalysts

Selective oxidation of propene to acrolein over industrial multicomponent bismuth molybdate (BMO) catalysts significantly depends on reaction conditions that include operating parameters and catalyst state. Here, this work investigates selective propene oxidation in the intrinsic kinetic paradigm of Temporal Analysis of Products (TAP) reactor by systematically varying catalyst redox state, temperature, and oxygen-to-propene feed ratio. A 93 % propene conversion with an acrolein yield of 80 % is achieved at elevated temperatures (450 °C) on oxidized catalysts under oxygen-rich conditions (O 2 :C 3 H 6 = 10). However, these conditions diminish acrolein-to-CO 2 selectivity due to enhanced total oxidation to CO 2 . In contrast, a reduced catalyst state, moderate temperature (350 °C), and lower oxygen feed (O 2 :C 3 H 6 = 1) nearly doubles the acrolein to-CO 2 selectivity, albeit at a lower acrolein yield (33 %). Transient kinetic studies together with a kinetic model that simplify the major product formation pathways in lumped non-elementary forms reveal that the availability of surface oxygen species plays a pivotal role in governing reaction pathways. Additionally, density functional theory (DFT) calculations on pure BMO catalysts inform the role of surface redox states on propene and oxygen activation barriers. Lattice oxygen at acrolein-selective sites drives both acrolein and CO 2 formation, while adsorbed oxygen at activation sites favors unselective CO 2 generation. This work establishes a critical relationship between transient product selectivity and surface oxygen availability, which is strongly influenced by catalyst redox state, feed ratio, and reaction temperature. These insights underscore the importance of dynamic reactor operation strategies and offer a foundation for designing next-generation propene oxidation processes with tunable acrolein selectivity.

42 - ENGINEERING↗