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Results for “Chemical Dynamics Initiative”

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 289 records · Page 16
All sourcesNASA NTRSDOE OSTI
NASA NTRS2011

The Two Components of the Evolved Massive Binary LZ Cephei: Testing the Effects of Binarity on Stellar Evolution

We present an in-dep(h study of the two components of the binary system LZ Cep to constrain the effects of binarity on the evolution of massive stars. Methods. We analyzed a set of high-resolution, high signal-to-noise ratio optical spectra obtained over the orbital period of the system to perform a spectroscopic disentangling and derive an orbital solution. We subsequently determine the stellar properties of each component by means of an analysis with the CMFGEN atmosphere code. Finally, with the derived stellar parameters, we model the Hipparcos photometric light curve using the program NIGHTFALL to obtain the orbit inclination and the stellar masses. Results.LZ Cep is a O9III+ON9.7V binary. It is as a semi-detailed system in which either the primary or the secondary star almost fills up its Roche lobe. The dynamical masses are about 16.0 Stellar Mass (primary) and 6.5 Stellar Mass (secondary). The latter is lower than the typical mass of late-type O stars. The secondary component is chemically more evolved than the primary (which barely shows any sign of CNO processing), with strong helium and nitrogen enhancements as well as carbon and oxygen depletions. These properties (surface abundances and mass) are typical of Wolf-Rayet stars, although the spectral type is ON9.7V. The luminosity of the secondary is consistent with that of core He-burning objects. The preferred, tentative evolutionary scenario to explain abe observed properties involves mass transfer from the secondary - which was initially more massive- towards the primary. The secondary is now almost a core He-burning object, probably with only a thin envelope of H-rich and CNO processed material. A very inefficient mass transfer is necessary to explain the chemical appearance of the primary. Alternative scenarios are discussed but they are affected by greater uncertainties.

Mahy, L.↗
DOE OSTI2026

Shapeshifting Nanocatalyst for CO2 Conversion

The conversion of CO2 into high-value chemicals through a photoreduction reaction in water is a promising route to reduce the dependence on fossil fuels. Enhancing selectivity toward hydrocarbons or alcohols can be achieved by Ag-Cu alloys. However, the stabilized surface state created by Ag-Cu interactions is still poorly understood. In this work, multi-modal in situ X-ray experiments reveals underlying mechanisms and the evolution of Ag-Cu nanoparticles under CO2 reduction reaction (CO2RR) conditions. Both morphological and chemical changes of Ag and Cu species induced by diffusion mechanics are tracked during nanocatalyst operation. The initial spheroid Ag-Cu nanoparticles are composed of a Cu-rich shell and Ag-rich core. The reduction treatment promotes Ag migration toward the surface. During photocatalytic CO2 reduction reaction, Cu atoms migrate back to the surface, forming Ag-Cu-O species. The study observes the surface oxidation of Cu(0) to Cu+ and the presence of Ag at the sub-surface region. Furthermore, nanoparticles change their shape, decreasing their specific surface area, driven by Cu diffusion during the CO2 photoreduction reaction. The results provide invaluable insights into the dynamic restructuring of the catalyst under reaction conditions and into the active species responsible for CO2 conversion.

CO2 reduction reaction↗
NASA NTRS1999

Chemical Vapor Deposition at High Pressure in a Microgravity Environment

In this paper we present an evaluation of critical requirements of organometallic chemical vapor deposition (OMCVD) at elevated pressure for a channel flow reactor in a microgravity environment. The objective of using high pressure is to maintain single-phase surface composition for materials that have high thermal decomposition pressure at their optimum growth temperature. Access to microgravity is needed to maintain conditions of laminar flow, which is essential for process analysis. Based on ground based observations we present an optimized reactor design for OMCVD at high pressure and reduced gravity. Also, we discuss non-intrusive real-time optical monitoring of flow dynamics coupled to homogeneous gas phase reactions, transport and surface processes. While suborbital flights may suffice for studies of initial stages of heteroepitaxy experiments in space are essential for a complete evaluation of steady-state growth.

McCall, Sonya↗
NASA NTRS1998

Modelling the Diversity of Outer Planetary Systems: Formation and Evolution - 1

The process of planetary growth is extremely complicated, involving a myriad of physical and chemical processes, many of which are poorly understood. The ultimate configuration that a planetary system attains depends upon the properties of the disk out of which it grew, of the star at the center of the disk and, at least in some cases, of the interstellar environment. However, this dependence is poorly understood. Thus, in an effort to numerically survey the possible diversity of planetary systems, we have constructed synthetic systems of giant planets and integrated their orbits to determine the dynamical lifetimes and thus the viability of these systems. Our construction algorithm begins with 110 -- 180 planetesimals located between 4 and 40 AU from a one solar mass star; most initial planetesimals have masses several tenths that of Earth. We integrate the orbits of these bodies subject to mutual gravitational perturbations and gas drag for $10^6 - 10^7$ years, merging any pair of planetesimals which passed within one-tenth of a Hill Sphere of one another and adding "gas" to embryos larger than 10 Earth masses. Use of such large planetesimal radii provided sufficient damping to prevent the system from excessive dynamical heating. Subsequently, systems were evolved without gas drag, either with the inflated radii or with more realistic radii. Systems took from a few million years to greater than ten billion years to become stable ($10^9$ years without mergers of ejections). Some of the systems produced with the inflated radii closely resemble our Solar System. Encounters in simulations using realistic radii resulted in ejections, typically leaving only a few planets per system, most of which were in highly eccentric orbits. The structure and dynamics of the resulting "stable" systems is discussed in detail in the abstract by Levison et al.

Lissauer, J. J.↗
NASA NTRS1986

Systematic development of reduced reaction mechanisms for dynamic modeling

A method for systematically developing a reduced chemical reaction mechanism for dynamic modeling of chemically reactive flows is presented. The method is based on the postulate that if a reduced reaction mechanism faithfully describes the time evolution of both thermal and chain reaction processes characteristic of a more complete mechanism, then the reduced mechanism will describe the chemical processes in a chemically reacting flow with approximately the same degree of accuracy. Here this postulate is tested by producing a series of mechanisms of reduced accuracy, which are derived from a full detailed mechanism for methane-oxygen combustion. These mechanisms were then tested in a series of reactive flow calculations in which a large-amplitude sinusoidal perturbation is applied to a system that is initially quiescent and whose temperature is high enough to start ignition processes. Comparison of the results for systems with and without convective flow show that this approach produces reduced mechanisms that are useful for calculations of explosions and detonations. Extensions and applicability to flames are discussed.

Frenklach, M.↗
NASA NTRS1993

Low-power millimeter-wave radar observations of the atmosphere

Historically, cloud structures, dynamics, and precipitation processes have been observed and measured with sensors from two different spatial resolutions. Laser-based sensors have volume resolutions on the order of 10(exp -4) to 10(exp -2) cubic meters for a 1-s sample. Radar systems operating at wavelengths between 1 and 10 cm have resolutions on the order of 10(exp 4) to 10(exp 7) cubic meters. The resolutions of micro-wave systems depend primarily on the system RF bandwidth and antenna bandwidth. Both resolution regimes were useful in the study of cloud structures and processes - the former for determining resolution on the individual cloud particle scale and the latter for studying the coarse characteristics of cloud dynamics and structure. There are, however, cloud processes and structures that occur on scales that lie between these two regimes: the process of entrainment, where outside air is brought within the cloud boundaries; the mixing of in-cloud particles with different histories; cloud particle coalescence; and ice formation. The use of mm-wave (30- to 300-GHz) radars offers an opportunity to observe cloud processes at these scales and determine their influence on precipitation development, cloud albedos, cloud lifetimes, chemical cycling of tract substances, aircraft icing, and other meteorological phenomena. To determine the usefulness of a 35-GHz radar for observing these precipitation and cloud processes, a research program was initiated. The objectives of this program are to develop a 35-GHz radar, to measure scattering from precipitation and clouds, and to develop a model to compute scattering from clouds using the finite-difference time-domain (FDTD) technique.

Ronnau, James F.↗
DOE OSTI2026

Brittle-to-Ductile Transition Temperature Decreases at the Microscale in Muscovite Mica

Characterizing the structural and chemical transitions of muscovite mica across various scales and thermal profiles is essential for ensuring the reliability of high-voltage power insulation, aerospace thermal barriers, and nanoscale semiconductor substrates under extreme operational stress. Here, we investigate notch fracture toughness $K^{n}_{Ic}$ of muscovite mica as a function of feature size w and temperature T with microscale shear testing. $K^{n}_{Ic}$ decreased and then stayed constant as w increased, likely from fabrication-induced changes to the microstructure and roughness. Moreover, $K^{n}_{Ic}$ initially decreased and then increased as temperature T increased, with the reversal in trend indicative of a brittle-to-ductile transition. Complementary Raman spectroscopy and molecular dynamics showed that the observed trends were due to an increase in bond lengths and a decrease in critical stresses/strains. In comparing the microscale results to macroscale counterparts, it was surmised that the decrease in brittle-to-ductile transition temperature was due to an increase in the dehydroxylation rate.

DelRio, Frank W. [Sandia National Laboratories (SN↗
DOE OSTI2020

Mechanistic Insights into Photocatalyzed H 2 Dissociation on Au Clusters

Localized surface plasmon resonances (LSPRs) have attracted much recent attention for their potential in promoting chemical reactions with light. However, the mechanism of LSPR-induced chemical reactions is still not clear, even for H 2 dissociation on metal nanoparticles. Here, we investigate the mechanism for photoinduced H 2 dissociation using a simple H 2 @Au 6 model. Our time-dependent density functional theory calculations indicate that the initial excitation is largely restricted to the metal cluster, involving intraband excitation that produces hot electrons (HEs). However, diabatization via overlapping orbitals reveals two types of nested electronic states, one involving excitations of the metallic electrons, namely, the HE states, and the other concerned with charge transfer (CT) to the adsorbate antibonding σ* orbital. Dissociation of H 2 thus takes place by transitions from the former to the latter. Quantum dynamics simulations on the diabatic CT states suggest rapid dissociation of H 2 , while no such dissociation occurs on diabatic HE states. Our research provides a clear physical picture of photoinduced H 2 dissociation on Au clusters, which has important implications in plasmonic facilitated photocatalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Characterizing particle-like charge-migration dynamics with high-order harmonic sideband spectroscopy

Here, we introduce high-order harmonic sideband spectroscopy and show that it can be a robust probe of charge migration (CM) in a halogenated carbon-chain molecule. We simulate both the CM and high-order harmonic generation (HHG) dynamics using ab initio time-dependent density-functional theory. We find that CM dynamics initiated along the molecular backbone induces sidebands in the HHG spectrum driven by a delayed laser pulse that is polarized perpendicular to the molecular axis. Monitoring the spectrum as either the HHG laser frequency or the relative delay is scanned allows for the extraction of detailed information about the time-domain characteristics of the CM process.

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRS1993

Scientific goals of the Cooperative Multiscale Experiment (CME)

Mesoscale Convective Systems (MCS) form the focus of CME. Recent developments in global climate models, the urgent need to improve the representation of the physics of convection, radiation, the boundary layer, and orography, and the surge of interest in coupling hydrologic, chemistry, and atmospheric models of various scales, have emphasized the need for a broad interdisciplinary and multi-scale approach to understanding and predicting MCS's and their interactions with processes at other scales. The role of mesoscale systems in the large-scale atmospheric circulation, the representation of organized convection and other mesoscale flux sources in terms of bulk properties, and the mutually consistent treatment of water vapor, clouds, radiation, and precipitation, are all key scientific issues concerning which CME will seek to increase understanding. The manner in which convective, mesoscale, and larger scale processes interact to produce and organize MCS's, the moisture cycling properties of MCS's, and the use of coupled cloud/mesoscale models to better understand these processes, are also major objectives of CME. Particular emphasis will be placed on the multi-scale role of MCS's in the hydrological cycle and in the production and transport of chemical trace constituents. The scientific goals of the CME consist of the following: understand how the large and small scales of motion influence the location, structure, intensity, and life cycles of MCS's; understand processes and conditions that determine the relative roles of balanced (slow manifold) and unbalanced (fast manifold) circulations in the dynamics of MCS's throughout their life cycles; assess the predictability of MCS's and improve the quantitative forecasting of precipitation and severe weather events; quantify the upscale feedback of MCS's to the large-scale environment and determine interrelationships between MCS occurrence and variations in the large-scale flow and surface forcing; provide a data base for initialization and verification of coupled regional, mesoscale/hydrologic, mesoscale/chemistry, and prototype mesoscale/cloud-resolving models for prediction of severe weather, ceilings, and visibility; provide a data base for initialization and validation of cloud-resolving models, and for assisting in the fabrication, calibration, and testing of cloud and MCS parameterization schemes; and provide a data base for validation of four dimensional data assimilation schemes and algorithms for retrieving cloud and state parameters from remote sensing instrumentation.

Cotton, William↗
NASA NTRS2005

Chemistry, Dynamics, and Radiation of Ozone Loss: Airborne Measurements of OH, HO2, NO2, ClO, BrO, IO, ClONO2, BrONO2, ClOOCl, and H2O

This grant continued the research initially funded under NAG1-01095. This research addresses, through a combination of in situ and remote aircraft-borne instruments, the following scientific questions: Which mechanisms are responsible for the continuing erosion of ozone over midlatitudes of the Northern Hemisphere? Will the rapid loss of ozone over the Arctic in late winter continue to worsen over the next two decades? Are these large losses dynamically coupled to midlatitudes? Which mechanisms dictate the rate of exchange of material between the troposphere and stratosphere? How will these processes change in response to changes in climate? Will regional scale pollution episodes, that are emerging as predictable seasonal events, significantly affect the middle-to-upper troposphere chemical composition. If so, how will these changes alter the chemical composition of the middle world? What changes are predicted for the overworld? Why has the arctic stratosphere become colder in the late winter phase in recent years? Have increases in tropical upper troposphere temperatures increased the temperature gradient such as to change the trajectories of vertically propagating waves, thus reducing the effectiveness of the meridional circulation for transport of heat, momentum and ozone from the tropics to high latitudes?

Anderson, James G.↗
DOE OSTI2025

Elucidating the Role of Electric Fields in Fe Oxidation via an Environmental Atom Probe

Abstract We quantify the effects of intensely applied electric fields on the Fe oxidation mechanism. The specimen are pristine Fe single crystals exposing a variety of surface structures identified by field ion microscopy. These crystals are simultaneously exposed to low pressures of pure oxygen gas, on the order of 10 −7 mbar, while applying intense electric fields on their surface of several tens of volts per nanometer. The local composition of the different surface structures is probed directly and in real time using an Environmental Atom Probe and successfully compared with first principles‐based models. We found that rough Fe{244} and Fe{112} facets are more reactive toward oxygen than compact Fe{024} and Fe{011} facets. Results demonstrate that the influence of an electric field on the oxidation kinetics depends on the timescales that are involved as the system evolves toward equilibrium. The initial oxidation kinetics show that strong increases in electric fields facilitate the formation of an oxide. However, as one approaches equilibrium, high field values mitigate this formation. Ultimately, this study elucidates how high externally applied electric fields can be used to dynamically exploit reaction dynamics at the nanoscale towards desired products in a catalytic reaction at mild reaction conditions.

Lambeets, Sten V. [Physical and Computational Scie↗
DOE OSTI2024

Properties of molecular clumps and cores in colliding magnetized flows

ABSTRACT We simulate the formation of molecular clouds in colliding flows of warm neutral medium with the adaptive mesh refinement code flash in eight simulations with varying initial magnetic field strength, between 0.01–5 μG. We include a chemical network to treat heating and cooling and to follow the formation of molecular gas. The initial magnetic field strength influences the fragmentation of the forming cloud because it prohibits motions perpendicular to the field direction and hence impacts the formation of large-scale filamentary structures. Molecular clump and core formation occurs anyhow. We identify 3D clumps and 3D cores, which are defined as connected, CO-rich regions. Additionally, 3D cores are heavily shielded. While we do not claim those 3D objects to be directly comparable to observations, this enables us to analyse their full virial state. With increasing field strength, we find more fragments with a smaller average mass; yet the dynamics of the forming clumps and cores only weakly depends on the initial magnetic field strength. The molecular clumps are mostly unbound, probably transient objects, which are weakly confined by ram pressure or thermal pressure, indicating that they are swept up by the turbulent flow. They experience significant fluctuations in the mass flux through their surface, such that the Eulerian reference frame shows a dominant time-dependent term due to their indistinct nature. We define the cores to encompass highly shielded molecular gas. Most cores are in gravitational-kinetic equipartition and are well described by the common virial parameter $\alpha _\mathrm{vir}$, while some undergo minor dispersion by kinetic surface effects.

Weis, M. (ORCID:0000000256838860)↗
NASA NTRSDate not supplied

Thermal Analysis of an In-Space Heat Shield Exposed to a Rocket Plume During Stage Separation

Thermal analyses were conducted to evaluate the thermal response of various individual materials and multi-layer configurations for an in-space heat shield exposed to a rocket plume during stage separation. Frequently used, readily available thermal protection materials consisting of cork, carbon cloth phenolic (CCP), and silica cloth phenolic (SCP) were selected for an initial screening analysis. SCP was chosen as the primary material for further evaluation using an updated thermal environment calculated using computational fluid dynamics (CFD) results. A multi-layer configuration consisting of SCP providing erosion resistance and a Nomex honeycomb providing thermal protection was then evaluated as a solution for more mass-efficient performance. Pyrolysis depth, bondline temperature, back-side temperature, and a thermal factor of safety were used to define the necessary material thickness profile. Adhesives were included in the analyses with considerations for maximum temperature and application method. One dimensional thermal analyses at several stations along the heat shield surface were performed for the initial screening and follow-on analyses. The methodology used standard processes and computer programs applicable to solid rocket motor internal insulation and nozzle thermal analysis such as Chemical Equilibrium and Applications (CEA), Aerotherm Chemical Equilibrium (ACE), Momentum/Energy Integral Technique (MEIT), and Insulation Thermal Response and Ablation Code (ITRAC). The baseline SCP/Nomex honeycomb multi-layer configuration thermal performance predictions satisfied the objectives with an acceptable mass estimate for the design maturity. The EA9673 film adhesive and SCP resin were the best performing bonding agents considered for the SCP/Nomex honeycomb and Nomex honeycomb/structural substrate interfaces. The baseline mass estimate was lowest when the resin was the bonding agent due to the higher maximum service temperature. These thermal analyses evaluated typical internal and external nozzle materials using a calculated thermal environment and heat loads that were lower than a typical rocket motor internal environment but greater than standard external aeroheating.

Andrew T Hiatt↗
DOE OSTI2020

Design and performance of high-temperature furnace and cell holder for in situ spectroscopic, electrochemical, and radiolytic investigations of molten salts

To facilitate the development of molten salt reactor technologies, a fundamental understanding of the physical and chemical properties of molten salts under the combined conditions of high temperature and intense radiation fields is necessary. Optical spectroscopic (UV–Vis–near IR) and electrochemical techniques are powerful analytical tools to probe molecular structure, speciation, thermodynamics, and kinetics of solution dynamics. In this paper, we report the design and fabrication of three custom-made apparatus: (i) a multi-port spectroelectrochemical furnace equipped with optical spectroscopic and electrochemical instrumentation, (ii) a high-temperature cell holder for time-resolved optical detection of radiolytic transients in molten salts, and (iii) a miniaturized spectroscopy furnace for the investigation of steady-state electron beam effects on molten salt speciation and composition by optical spectroscopy. Initial results obtained with the spectroelectrochemical furnace (i) and high-temperature cell holder (ii) are reported.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

The stable carbon isotope fractionation of methanogenesis products at complete carbon consumption

The stable carbon isotope signature (δ 13 C) of methane (CH 4 ) is used to discriminate between biological, thermogenic, and abiotic sources. Methanogens, or methane producing archaea, inhabit a broad range of chemical conditions. Many of these environments are replete in dissolved inorganic carbon (DIC), causing isotopically depleted δ 13 C biogenic CH 4 . However, some extreme environments inhabited by methanogens, such as serpentinising systems, exhibit low carbon dioxide (CO 2 ) availability, replete H 2 , and isotopically enriched δ 13 C CH 4 that is outside the known biogenic range. We measured the δ 13 C of CO 2 , biomass, lipids, and CH 4 during hydrogenotrophic methanogenesis under hydrogen replete conditions with a limited carbon pool to investigate carbon isotope dynamics at complete DIC consumption. As theory predicts, we found that the final, accumulated methane δ 13 C values closely reflect the δ 13 C of the initial DIC supply, and that methane is more 13 C enriched than biomass and lipids. This provides the first experimental evidence that methanogens can achieve complete carbon consumption and thus can produce accumulated CH 4 products that isotopically reflect the initial CO 2 . These data show that the range of possible δ 13 C values from biogenic methane needs to be expanded for natural environments impacted by extreme carbon limitation.

biomass↗
NASA NTRS1991

Supernova remnants in dense clouds. I - Blast-wave dynamics and X-ray irradiation

Simplified models of cooling SNRs in uniform media together with an idealized emission spectrum are used to investigate the X-ray irradiation of the surrounding gas. The radiative transfer of the emitted X-rays through both the dense cooling shell and the unshocked cloud is calculated, with a simplified treatment to allow for an ionized zone surrounding the SNR. Numerical results are presented for SN energy of 10 exp 51 ergs and ambient densities ranging from 100 to 1,000,000 cu cm. It is found that an appreciable fraction of the X-ray energy is absorbed in regions where the X-ray energy deposited per H nucleon is between 1 and 30 eV; if the gas is initially molecular, the X-ray irradiation will result in warm molecular gas in which endothermic chemical reactions may proceed, and from which there may be strong emission in rotation-vibration transitions of H2 and other molecular species.

Draine, B. T.↗
NASA NTRSDate not supplied

Predicting Char Yield of High-Temperature Resins

A simulation technique has been developed for predicting the char yield of organic resins during high-temperature processing. In silico methods can aid in the screening of new advanced materials for a number of important properties, but no chemistry-sensitive protocol currently exists for predicting the important experimental value of char yield. The proposed method utilizes a reactive force field (ReaxFF) to model the chemical transformation of precursor monomers into carbonized structures during three processing stages: ramp-up to pyrolysis temperatures (~3000 K), pyrolysis, and quenching. Achieving good agreement with experimental char yields requires continuous removal of small by-product molecules to mimic outgassing, and the application of high pressure to encourage the formation of a dense, glassy network. Six different resin chemistries were investigated: an ethynyl, a phenylethynyl, a cyanate ester, a phthalonitrile, acrylonitrile, and adamantane. These candidates represent a diverse group of precursors with respect to initial cyclic content, presence of heteroatoms, and types of reactive groups. The protocol developed accurately predicts the relative char yield between the investigated chemistries and provides quantitative agreement with experimental values, especially for high char yield resins. Several simulated properties of the carbonized structures are compared with experimental results, including outgassing products, morphology of the final chemical configurations, cyclic content, and mechanical properties.

polymer simulations, molecular dynamics↗