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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.

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At least 271 records · Page 15
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Combined Experimental and Computational Efforts to Establish Ion Mobility, Solubility and Stability of Functional Liquids for Electrochemical Energy Storage

This work provides a computation-driven investigation of the stability of organic electrolytes for lithium-air batteries. Electrolyte instability is currently a key challenge that limits practical use of aprotic Li-air batteries, and the chemical processes that cause this instability are often kinetically-driven. Computational screening for kinetic stability involves the determination of reaction barriers for the numerous potential reaction mechanisms, barriers that are challenging to calculate due to the difficulty of locating transition state structures. Here we screen a broad set of substituted electrolytes for susceptibility to nucleophilic attack by superoxide. We find that carbonates are not typically expected to be stable and that sulfones are generally stable, validating literature trends. We study the effects of chemical functionalization with electron-donating and withdrawing groups and their interplay with steric factors, identifying functional groups and other chemical modifications that increase stability in these groups. User-input driven transition state identification is used for these initial calculations, and an automated computational pipeline is subsequently presented and validated as a means to perform further high-throughput searches across mechanisms and chemistries. The pipeline integrates cheminformatics-based reaction encoding, relaxed potential energy scans, and nudged elastic band calculations for an end-to-end approach to barrier calculations. We review this automated search approach and its current limitations, and discuss challenges and further work.

25 ENERGY STORAGE↗
DOE OSTI2022

High accuracy barrier heights, enthalpies, and rate coefficients for chemical reactions

Abstract Quantitative chemical reaction data, including activation energies and reaction rates, are crucial for developing detailed kinetic mechanisms and accurately predicting reaction outcomes. However, such data are often difficult to find, and high-quality datasets are especially rare. Here, we use CCSD(T)-F12a/cc-pVDZ-F12// ω B97X-D3/def2-TZVP to obtain high-quality single point calculations for nearly 22,000 unique stable species and transition states. We report the results from these quantum chemistry calculations and extract the barrier heights and reaction enthalpies to create a kinetics dataset of nearly 12,000 gas-phase reactions. These reactions involve H, C, N, and O, contain up to seven heavy atoms, and have cleaned atom-mapped SMILES. Our higher-accuracy coupled-cluster barrier heights differ significantly (RMSE of ∼5 kcal mol −1 ) relative to those calculated at ω B97X-D3/def2-TZVP. We also report accurate transition state theory rate coefficients $${k}_{\infty }(T)$$ k ∞ ( T ) between 300 K and 2000 K and the corresponding Arrhenius parameters for a subset of rigid reactions. We believe this data will accelerate development of automated and reliable methods for quantitative reaction prediction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2008

Understanding Black Hole X-ray Binaries: The Case of Cygnus X-1

Black Hole X-ray Binaries are known to display distinct emission states that differ in their X-ray spectra, their X-ray timing properties (on times scales less than 1 s) and their radio emission. In recent years monitoring observations, specially with NASA's Rossi X-ray Timing Explorer (RXTE), have provided us with detailed empirical modeling of the phenomenology of the different states as well as a unification scheme of the long term evolution of black holes, transient and persistent, in terms of these states. Observations of the persistent High Mass X-ray Binary (HMXB) Cygnus X-l have been at the forefront of learning about black hole states since its optical identification through a state transition in 1973. In this talk I will present in depth studies of several different aspects of the accretion process in this system. The main data base for these studies is an ongoing RXTE and Ryle radio telescope bi-weekly monitoring campaign that started in 1997. I will discuss high-resolution timing results, especially power spectra, which first gave rise to the Lorentzian description now widely used for black hole and neutron star binaries, and time lags, which we found to be especially well suited to identify state transitions. The evolution of spectral, timing, and radio parameters over years will be shown, including the rms-flux relation and the observation of a clearly correlated radio/x-ray flare. We also observed Cygnus X-1 with INTEGRAL, which allowed us to extend timing and spectral studies to higher energies, with XMM, which provided strong constraints on the parameters of the 6.4 keV iron fluorescence line, and with Chandra, which provided the most in depth study to date of the stellar wind in this system. Models based on the physical conditions in the accretion region are still mainly concentrated on the one or other of the observational areas but they are expanding: as an example I will review results from a jet model for the quantitative description of the radio through X-ray spectra. I will conclude with an outlook on a truly multi-instrument observing campaign of Cygnus X-1 that was performed in 2008 April in order to better constrain the jet models mentioned above (and provide a unique data set for cross-calibration).

Pottschmidt, Katja↗
DOE OSTI2025

Resolving the Coverage Dependence of Surface Reaction Kinetics with Machine Learning and Automated Quantum Chemistry Workflows

Microkinetic models for catalytic systems require estimation of many thermodynamic and kinetic parameters that can be calculated for isolated species and transition states using ab initio methods. However, the presence of nearby coadsorbates on the surface can dramatically alter these thermodynamic and kinetic parameters causing them to be dependent on species coverage fractions. As there are combinatorially many coadsorbed configurations on the surface, computing the coverage dependence of these parameters is far less straightforward. We present a framework for generating and applying machine learning models to predict coverage-dependent parameters for microkinetic models. Our toolkit enables automatic calculation and evaluation of coadsorbed configurations allowing us to sample 2,000 coadsorbed adsorbates and transition states (TSs) for a diverse set of 9 reactions on Cu(111), a challenging surface, with four possible coadsorbates. This dataset was then used to train subgraph isomorphic decision trees (SIDTs) to predict the stability and association energy of configurations. We were able to achieve mean absolute errors (MAEs) of 0.106 eV on adsorbates, 0.172 eV on TSs, and due to natural error cancellation in SIDTs for relative properties, 0.130 eV on reaction energies and 0.180 eV on activation barriers. In conclusion, we describe how to use these models to predict coverage-dependent corrections for adsorbates and TSs and demonstrate on H*, HO*, and O* comparing the generated SIDT model with an iteratively refined version.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2013

Optimal Propellant Maneuver Flight Demonstrations on ISS

In this paper, first ever flight demonstrations of Optimal Propellant Maneuver (OPM), a method of propulsive rotational state transition for spacecraft controlled using thrusters, is presented for the International Space Station (ISS). On August 1, 2012, two ISS reorientations of about 180deg each were performed using OPMs. These maneuvers were in preparation for the same-day launch and rendezvous of a Progress vehicle, also a first for ISS visiting vehicles. The first maneuver used 9.7 kg of propellant, whereas the second used 10.2 kg. Identical maneuvers performed without using OPMs would have used approximately 151.1kg and 150.9kg respectively. The OPM method is to use a pre-planned attitude command trajectory to accomplish a rotational state transition. The trajectory is designed to take advantage of the complete nonlinear system dynamics. The trajectory choice directly influences the cost of the maneuver, in this case, propellant. For example, while an eigenaxis maneuver is kinematically the shortest path between two orientations, following that path requires overcoming the nonlinear system dynamics, thereby increasing the cost of the maneuver. The eigenaxis path is used for ISS maneuvers using thrusters. By considering a longer angular path, the path dependence of the system dynamics can be exploited to reduce the cost. The benefits of OPM for the ISS include not only reduced lifetime propellant use, but also reduced loads, erosion, and contamination from thrusters due to fewer firings. Another advantage of the OPM is that it does not require ISS flight software modifications since it is a set of commands tailored to the specific attitude control architecture. The OPM takes advantage of the existing ISS control system architecture for propulsive rotation called USTO control mode1. USTO was originally developed to provide ISS Orbiter stack attitude control capability for a contingency tile-repair scenario, where the Orbiter is maneuvered using its robotic manipulator relative to the ISS. Since 2005 USTO has been used for nominal ISS operations.

Bhatt, Sagar↗
NASA NTRS2004

Part 1 of a Computational Study of a Drop-Laden Mixing Layer

This first of three reports on a computational study of a drop-laden temporal mixing layer presents the results of direct numerical simulations (DNS) of well-resolved flow fields and the derivation of the large-eddy simulation (LES) equations that would govern the larger scales of a turbulent flow field. The mixing layer consisted of two counterflowing gas streams, one of which was initially laden with evaporating liquid drops. The gas phase was composed of two perfect gas species, the carrier gas and the vapor emanating from the drops, and was computed in an Eulerian reference frame, whereas each drop was tracked individually in a Lagrangian manner. The flow perturbations that were initially imposed on the layer caused mixing and eventual transition to turbulence. The DNS database obtained included transitional states for layers with various liquid mass loadings. For the DNS, the gas-phase equations were the compressible Navier-Stokes equations for conservation of momentum and additional conservation equations for total energy and species mass. These equations included source terms representing the effect of the drops on the mass, momentum, and energy of the gas phase. From the DNS equations, the expression for the irreversible entropy production (dissipation) was derived and used to determine the dissipation due to the source terms. The LES equations were derived by spatially filtering the DNS set and the magnitudes of the terms were computed at transitional states, leading to a hierarchy of terms to guide simplification of the LES equations. It was concluded that effort should be devoted to the accurate modeling of both the subgridscale fluxes and the filtered source terms, which were the dominant unclosed terms appearing in the LES equations.

Okong'o, Nora A.↗
NASA NTRS2002

Gas-Phase Reaction Pathways and Rate Coefficients for the Dichlorosilane-Hydrogen and Trichlorosilane-Hydrogen Systems

As part of NASA Ames Research Center's Integrated Process Team on Device/Process Modeling and Nanotechnology our goal is to create/contribute to a gas-phase chemical database for use in modeling microelectronics devices. In particular, we use ab initio methods to determine chemical reaction pathways and to evaluate reaction rate coefficients. Our initial studies concern reactions involved in the dichlorosilane-hydrogen (SiCl2H2--H2) and trichlorosilane-hydrogen (SiCl2H-H2) systems. Reactant, saddle point (transition state), and product geometries and their vibrational harmonic frequencies are determined using the complete-active-space self-consistent-field (CASSCF) electronic structure method with the correlation consistent polarized valence double-zeta basis set (cc-pVDZ). Reaction pathways are constructed by following the imaginary frequency mode of the saddle point to both the reactant and product. Accurate energetics are determined using the singles and doubles coupled-cluster method that includes a perturbational estimate of the effects of connected triple excitations (CCSD(T)) extrapolated to the complete basis set limit. Using the data from the electronic structure calculations, reaction rate coefficients are obtained using conventional and variational transition state and RRKM theories.

Dateo, Christopher E.↗
NASA NTRS1994

The high-state/low-state transition in V794 Aquilae

We present a V-magnitude light curve of the cataclysmic binary V794 Quilae covering an 800 day time span. The system shows variations of ups to 3 mag. In particular, there are two dips of approximately 1 mag which last for about 50 days, and are followed by a rapid recovery to the original brightness, and a third dip of approximately 3 mag lasting about 100 days. These fluctuations are thought to be caused by the response of the accretion disk in the system to the cessation of mass transfer from the mass-losing secondary star. We present computations using a time-dependent accretion disk code to delineate a range of allowed behavior for th accretion disk. To model the observed light curve, we require that the model parameters alpha(sub cold) and alpha(sub hot), which characterize the degree of coupling of the viscous dissipation to the orbital shear in the low and high states of the accretion disk, be smaller than they have been inferred to be in the dwarf novae, and that the ratio alpha(sub hot)/alpha(sub cold) also be smaller. The fact that alpha seems to vary with the rate of mass transfer may provide support for the model of Vishniac and Diamond, in which the impact of the mass transfer stream onto the outer edge of the accretion disk excites internal waves which transport angular momentum outward and provide the viscous dissipation.

Honeycutt, R. Kent↗
DOE OSTI2026

Controlled Placement of Trivalent Heteroatoms in MFI Zeolite Frameworks Using Structure-Directing Agents

MFI zeolites contain distinct confining pore environments, either smaller (∼0.55 nm) channels or larger (∼0.70 nm) intersections. The substitution of trivalent heteroatoms generates Brønsted acid sites of varying acid strength, which, together with their location within different pore environments, dictates the stability of transition states via electrostatic (ion-pair) and van der Waals interactions. Here, we report that structure-directing agents (SDAs) that control Al 3+ substitutional patterns during MFI crystallization analogously position other trivalent heteroatoms (Ga 3+ , Fe 3+ , B 3+ ), altering the distribution of acid sites between channels and intersections, as probed by low-temperature (403 K) toluene methylation kinetics. Heteroatom-substituted MFI crystallized with tetrapropylammonium result in low selectivity toward p-xylene (<30%), while those crystallized using (co-)SDAs containing peripheral hydrogen-bonding groups (e.g., ethylenediamine) show high p-xylene selectivity (∼80%). These selectivities are consistent with DFT-calculated Gibbs free energy barriers for intersection-dominant and channel-dominant active site distributions, respectively. Transition states to form each xylene isomer are similar in size and charge; thus, their rate constants decrease with acid strength similarly, causing isomer selectivity to depend strongly on confinement but not on acid strength. These generalizable synthetic strategies enable independently controlling acid site strength and location in MFI zeolites and, in turn, catalytic rates and selectivities.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Role of the ionic environment in enhancing the activity of reacting molecules in zeolite pores

Tailoring the molecular environment around catalytically active site allows the enhancement of catalytic reactivity via a hitherto unexplored pathway. In zeolites, the presence of water creates an ionic environment via the formation of hydrated hydronium ions and the negatively charged framework Al tetrahedra. The high density of cation-anion pairs determined by the aluminum concentration of a zeolite induces a high local ionic strength that increases the excess chemical potential of sorbed and uncharged organic reactants. Charged transition states (as for example, the carbenium ions in the discussed alcohol dehydration) are stabilized, reducing the energy barrier and leading to a higher reaction rate. Using the intramolecular dehydration of cyclohexanol on H-MFI in water, we show quantitatively the enhancement of the reaction rate by the presence of high ionic strength as well as potential limitations of this strategy. The approach opens a new pathway to systematically enhance catalytic reactivity rates and has wide-ranging implications for understanding catalysis in condensed phase.

Pfriem, Niklas↗
DOE OSTI2020

A statistical model for the product energy distribution in reactions leading to prompt dissociation

Direct dynamics calculations have been performed for three reactions: C 3 H 8 + H → i-C 3 H 7 + H 2 , C 3 H 8 + H → n-C 3 H 7 + H 2 , and C 2 H 3 + O 2 → HCO + CH 2 O. The fraction of the population for the radical products that promptly dissociates is computed. Here the results for C 3 H 8 + H are qualitatively similar to previous results for C 3 H 8 + OH, but the new results exhibit a slightly higher branching fraction for prompt dissociation products, owing to the fact that a greater fraction of the internal energy in the transition state ends up in the radical. For C 2 H 3 + O 2 → HCO + CH 2 O, the fraction of HCO that promptly dissociates is in excess of 99%. Consequently, the main product for C 2 H 3 + O 2 at lower temperatures should be written as H + CO + CH 2 O and not HCO + CH 2 O. These results are then compared with four previous systems: CH 2 O + H → HCO + H 2 , CH 2 O + OH → HCO + H 2 O, C 3 H 8 + OH → i-C 3 H 7 + H 2 O, and C 3 H 8 + OH → n-C 3 H 7 + H 2 O. Based upon these seven system, several statistical models are presented. The goal of these statistical models is to predict the fraction of the transition state energy that ends up in the rovibrationally excited radical. On average, these statistical models provide an excellent prediction of product energy distribution. Consequently, these models can be used instead of costly trajectory simulations for predicting prompt radical dissociation for larger species.

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

The highly exothermic hydrogen abstraction reaction H 2 Te + OH → H 2 O + TeH: comparison with analogous reactions for H 2 Se and H 2 S

The “gold standard” CCSD(T) method is adopted along with the correlation consistent basis sets up to aug-cc-pV5Z-PP to study the mechanism of the hydrogen abstraction reaction H 2 Te + OH. Here, the predicted geometries and vibrational frequencies for reactants and products are in good agreement with the available experimental results. With the ZPVE corrections, the transition state in the favorable pathway of this reaction energetically lies 1.2 kcal mol -1 below the reactants, which is lower than the analogous relative energies for the H 2 Se + OH reaction (-0.7 kcal mol -1 ), the H 2 S + OH reaction (+0.8 kcal mol -1 ) and the H 2 O + OH reaction (+9.0 kcal mol -1 ). Accordingly, the exothermic reaction energies for these related reactions are predicted to be 47.8 (H 2 Te), 37.7 (H 2 Se), 27.1 (H 2 S), and 0.0 (H 2 O) kcal mol -1 , respectively. Geometrically, the low-lying reactant complexes for H 2 Te + OH and H 2 Se + OH are two-center three-electron hemibonded structures, whereas those for H 2 S + OH and H 2 O + OH are hydrogen-bonded. With ZPVE and spin–orbit coupling corrections, the relative energies for the reactant complex, transition state, product complex, and the products for the H 2 Te + OH reaction are estimated to be -13.1, -1.0, -52.0, and -52.6 kcal mol -1 , respectively. Finally, twenty-eight DFT functionals have been tested systematically to assess their ability in describing the potential energy surface of the H 2 Te + OH reaction. The best of these functionals for the corresponding energetics are -9.9, -1.4, -46.4, and -45.4 kcal mol -1 (MPWB1K), or -13.1, -2.4, -57.1, and -54.6 kcal mol -1 (M06-2X), respectively.

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

Operation Optimization Using Reinforcement Learning with Integrated Artificial Reasoning Framework

In large and complex systems, operational decision-making requires a systematic analysis with a vast amount of data from both process parameters and component status monitoring. In this paper, we present an integrated artificial reasoning approach for system state transition models that can help operational decision-making with explainable and traceable reasoning. The integrated artificial reasoning framework is a physics-based approach of defining the system structure in a Bayesian network, so we leveraged it in a Markov decision process (MDP) for finding optimal operational solutions. In our proposed framework, the MDP is implemented on a dynamic Bayesian network (DBN), which represents causalities in a system. The multilevel flow modeling was utilized in order to extract these causalities in a more efficient and objective manner. Since multilevel flow modeling is based on the fundamental energy and mass conservation laws, the target system is decomposed into several mass, energy, and information structures, which serve as the basis for a DBN. The MDP consists of the processes of finding a solution for the Bellman equation, which can be derived from the conditional probability equations of the constructed DBN. System operators can capture stochastic system dynamics as multiple subsystem state transitions based on their physical relations and uncertainties coming from the component degradation process or random failures. We analyzed a simplified example system to illustrate finding an optimal operational policy with this approach.

Kim, Junyung↗
NASA NTRS2012

A Posteriori Study of a DNS Database Describing Super critical Binary-Species Mixing

Currently, the modeling of supercritical-pressure flows through Large Eddy Simulation (LES) uses models derived for atmospheric-pressure flows. Those atmospheric-pressure flows do not exhibit the particularities of high densitygradient magnitude features observed both in experiments and simulations of supercritical-pressure flows in the case of two species mixing. To assess whether the current LES modeling is appropriate and if found not appropriate to propose higher-fidelity models, a LES a posteriori study has been conducted for a mixing layer that initially contains different species in the lower and upper streams, and where the initial pressure is larger than the critical pressure of either species. An initially-imposed vorticity perturbation promotes roll-up and a double pairing of four initial span-wise vortices into an ultimate vortex that reaches a transitional state. The LES equations consist of the differential conservation equations coupled with a real-gas equation of state, and the equation set uses transport properties depending on the thermodynamic variables. Unlike all LES models to date, the differential equations contain, additional to the subgrid scale (SGS) fluxes, a new SGS term that is a pressure correction in the momentum equation. This additional term results from filtering of Direct Numerical Simulation (DNS) equations, and represents the gradient of the difference between the filtered pressure and the pressure computed from the filtered flow field. A previous a priori analysis, using a DNS database for the same configuration, found this term to be of leading order in the momentum equation, a fact traced to the existence of high-densitygradient magnitude regions that populated the entire flow; in the study, models were proposed for the SGS fluxes as well as this new term. In the present study, the previously proposed constantcoefficient SGS-flux models of the a priori investigation are tested a posteriori in LES, devoid of or including, the SGS pressure correction term. The present pressure-correction model is different from, and more accurate as well as less computationally intensive than that of the a priori study. The constant-coefficient SGS-flux models encompass the Smagorinsky (SMC), in conjunction with the Yoshizawa (YO) model for the trace, the Gradient (GRC) and the Scale Similarity (SSC) models, all exercised with the a priori study constant coefficients calibrated at the transitional state. The LES comparison is performed with the filtered- and-coarsened (FC) DNS, which represents an ideal LES solution. Expectably, an LES model devoid of SGS terms is shown to be considerably inferior to models containing SGS effects. Among models containing SGS effects, those including the pressure-correction term are substantially superior to those devoid of it. The sensitivity of the predictions to the initial conditions and grid size are also investigated. Thus, it has been discovered that, additional to the atmospheric-pressure models currently used, a new model is necessary to simulate supercritical-pressure flows. This model depends on the thermodynamic characteristics of the chemical species involved.

Bellan, Josette↗
DOE OSTI2025

Doping Effects on Multivalence States, Electronic Structure, and Optical Band Gap in LaCrO 3 under Varied Atmospheres: An Integrated Experimental and Density Functional Theory Study

Doping effects on the valence state, electronic structure, and optical band and the effects on electrical conductivity were studied on the doped lanthanum chromite (LaCrO 3 ) system. The specific compositions studied were La 1–x Ca x CrO 3 (LCCx), La 1–x Sr x CrO 3 (LSCx), and La 0.8 Sr 0.2 Cr 1–x Mn x O 3 (LSCMx) (0.1 ≤ x ≤ 0.4). The powders were synthesized using a modified Pechini sol–gel method, and the ceramic samples were densified using a reactive sintering method resulting in densities >96% theoretical. X-ray photoelectron spectroscopy (XPS) was completed to characterize the defect states and cationic valence compensation as a result of divalent (Ca 2+ or Sr 2+ ) and trivalent (Mn 3+ ) substitutions. XPS was completed for samples tested in oxidizing and reducing atmospheres (up to 1500 °C), which provided insights into the oxidation state transitions induced by the Ca 2+ and Sr 2+ dopants. The work notably demonstrated, for the first time, the oxidation/reduction transitions of Cr 4+ to Cr 3+ in Sr 2+ /Mn 3+ co-doped samples under reducing atmospheres. Reflectance UV–vis spectrophotometry optical band gap measurements were also completed for the same materials; a decrease in the optical band gap (2.81–3.12 eV) was shown with increased substitution, suggesting electronic structure modifications in the LaCrO 3 perovskite. Density functional theory calculations validated experimental trends, predicting a diminishing band gap with a rising dopant concentration. The transition in Cr oxidation states was attributed to the presence of divalent/trivalent cations. These findings contribute some insights into methods to tune the LaCrO 3 electrical properties for various low- and high-temperature applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Oxidation and pyrolysis of methyl propyl ether

The ignition, oxidation, and pyrolysis chemistry of methyl propyl ether (MPE) was probed experimentally at several different conditions, and a comprehensive chemical kinetic model was constructed to help understand the observations, with many of the key parameters computed using quantum chemistry and transition state theory. Experiments were carried out in a shock tube measuring time variation of CO concentrations, in a flow tube measuring product concentrations, and in a rapid compression machine (RCM) measuring ignition delay times. The detailed reaction mechanism was constructed using the Reaction Mechanism Generator software. Sensitivity and flux analyses were used to identify key rate and thermochemical parameters, which were then computed using quantum chemistry to improve the mechanism. Validation of the final model against the 1-20 bar 600-1500 K experimental data is presented with a discussion of the kinetics. The model is in excellent agreement with most of the shock tube and RCM data. Strong non-monotonic variation in conversion and product distribution is observed in the flow-tube experiments as the temperature is increased, and unusually strong pressure dependence and significant heat release during the compression stroke is observed in the RCM experiments. These observations are largely explained by a close competition between radical decomposition and addition to O2 at different sites in MPE; this causes small shifts in conditions to lead to big shifts in the dominant reaction pathways. The validated mechanism was used to study the chemistry occurring during ignition in a diesel engine, simulated using Ignition Quality Test (IQT) conditions. At the IQT conditions, where the MPE concentration is higher, bimolecular reactions of peroxy radicals are much more important than in the RCM.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2020

A Rapid change in x-ray variability and a jet ejection in the black hole transient MAXI J1820+070

We present Neutron Star Interior Composition Explorer X-ray and Arcminute Microkelvin Imager Large Array radio observations of a rapid hard-to-soft state transition in the black hole X-ray transient MAXI J1820+070. During the transition from the hard state to the soft state a switch between two particular types of quasiperiodic oscillations (QPOs) was seen in the X-ray power density spectra, from type-C to type-B, along with a drop in the strength of the broadband X-ray variability and a brief flare in the 7–12 keV band. Soon after this switch (∼2–2.5 hr) a strong radio flare was observed that corresponded to the launch of superluminal ejecta. Although hints of a connection between QPO transitions and radio flares have been seen in other black hole X-ray transients, our observations constitute the strongest observational evidence to date for a link between the appearance of type-B QPOs and the launch of discrete jet ejections.

Jeroen Homan↗
DOE OSTI2025

A neural master equation framework for multiscale modeling of molecular processes: application to atomic-scale plasma processes

Plasma-surface interactions (PSI) play a crucial role in microelectronics fabrication; however, their multiscale nature and array of complex, often unknown interactions make computational modeling of PSIs extremely difficult. To this end, we propose a general neural master equation (NME) framework that uses master equations to describe the dynamics of a molecular process, wherein neural networks learned from atomistic simulations represent unknown transitions between different system states. By leveraging the physics-based structure of master equations and data-driven state transitions, the NME framework promotes generalizability and physics interpretability, and can bridge disparate length and time scales. The framework is demonstrated for multiscale modeling of Si atomic layer etching and reactive ion etching, where the learned NME-based surface kinetic models exhibit good predictive and extrapolative capabilities for predicting experimentally relevant observables as a function of process parameters. The NME-based surface kinetic models obey physical constraints, which are violated in models based on neural ordinary differential equations. The proposed NME framework for multiscale modeling of molecular processes can pave the way for the discovery of new chemistries and materials in atomic-scale plasma processes.

Chemical engineering↗