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DOE OSTI2016

Understanding the ignition mechanism of high-pressure spray flames

A conceptual model for turbulent ignition in high-pressure spray flames is presented. The model is motivated by first-principles simulations and optical diagnostics applied to the Sandia n-dodecane experiment. The Lagrangian flamelet equations are combined with full LLNL kinetics (2755 species; 11,173 reactions) to resolve all time and length scales and chemical pathways of the ignition process at engine-relevant pressures and turbulence intensities unattainable using classic DNS. The first-principles value of the flamelet equations is established by a novel chemical explosive mode-diffusion time scale analysis of the fully-coupled chemical and turbulent time scales. Contrary to conventional wisdom, this analysis reveals that the high Damköhler number limit, a key requirement for the validity of the flamelet derivation from the reactive Navier–Stokes equations, applies during the entire ignition process. Corroborating Rayleigh-scattering and formaldehyde PLIF with simultaneous schlieren imaging of mixing and combustion are presented. Our combined analysis establishes a characteristic temporal evolution of the ignition process. First, a localized first-stage ignition event consistently occurs in highest temperature mixture regions. This initiates, owed to the intense scalar dissipation, a turbulent cool flame wave propagating from this ignition spot through the entire flow field. This wave significantly decreases the ignition delay of lower temperature mixture regions in comparison to their homogeneous reference. This explains the experimentally observed formaldehyde formation across the entire spray head prior to high-temperature ignition which consistently occurs first in a broad range of rich mixture regions. There, the combination of first-stage ignition delay, shortened by the cool flame wave, and the subsequent delay until second-stage ignition becomes minimal. A turbulent flame subsequently propagates rapidly through the entire mixture over time scales consistent with experimental observations. As a result, we demonstrate that the neglect of turbulence-chemistry-interactions fundamentally fails to capture the key features of this ignition process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2018

Optimization of Secondary Air Injection in a Wood-Burning Cookstove: An Experimental Study

Nearly 40% of the world's population regularly cooks on inefficient biomass stoves that emit harmful airborne pollutants, such as particulate matter (PM). Secondary air injection can significantly reduce PM mass emissions to mitigate the health and climate impacts associated with biomass cookstoves. However, secondary air injection can also increase the number of ultrafine particles emitted, which may be more harmful to health. This research investigates the effect of secondary air injection on the mass and size distribution of PM emitted during solid biomass combustion. An experimental wood-burning cookstove platform and parametric testing approach are presented to identify and optimize secondary air injection parameters that reduce PM and other harmful pollutants. Size-resolved measurements of PM emissions were collected and analyzed as a function of parametric stove design settings. The results show that PM emissions are highly sensitive to secondary air injection flow rate and velocity. Although increasing turbulent mixing (through increased velocity) can promote more complete combustion, increasing the total flow rate of secondary air may cause localized flame quenching that increases particle emissions. As a result, biomass cookstoves that implement secondary air injection should be carefully optimized and validated to ensure that PM emission reductions are achieved throughout the particle size range.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2015

APPARENT CROSS-FIELD SUPERSLOW PROPAGATION OF MAGNETOHYDRODYNAMIC WAVES IN SOLAR PLASMAS

In this paper we show that the phase-mixing of continuum Alfvén waves and/or continuum slow waves in the magnetic structures of the solar atmosphere as, e.g., coronal arcades, can create the illusion of wave propagation across the magnetic field. This phenomenon could be erroneously interpreted as fast magnetosonic waves. The cross-field propagation due to the phase-mixing of continuum waves is apparent because there is no real propagation of energy across the magnetic surfaces. We investigate the continuous Alfvén and slow spectra in two-dimensional (2D) Cartesian equilibrium models with a purely poloidal magnetic field. We show that apparent superslow propagation across the magnetic surfaces in solar coronal structures is a consequence of the existence of continuum Alfvén waves and continuum slow waves that naturally live on those structures and phase-mix as time evolves. The apparent cross-field phase velocity is related to the spatial variation of the local Alfvén/slow frequency across the magnetic surfaces and is slower than the Alfvén/sound velocities for typical coronal conditions. Understanding the nature of the apparent cross-field propagation is important for the correct analysis of numerical simulations and the correct interpretation of observations.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Nonunique fraction of Fock exchange for defects in two-dimensional materials

By investigating the vacancy and substitutional defects in monolayer WS 2 with hybrid functionals, we find that there is no unique amount of Fock exchange that concurrently satisfies the generalized Koopmans' condition and reproduces the band-gap and band-edge positions. Fixing the mixing parameter of Fock exchange based on the band gap can lead to qualitatively incorrect defect physics in two-dimensional materials. Instead, excellent agreement is achieved with both experiment and many-body perturbation theory within the GW approximation once the mixing parameters are tuned individually for the defect species and the band edges. Here, we show the departure from a unique optimized mixing parameter is inherent to two-dimensional systems as the band edges experience a reduced screening while the localized defects are subject to bulklike screening.

2-dimensional systems↗

DOE OSTI2024

Quantifying Quantum Chaos through Microcanonical Distributions of Entanglement

A characteristic feature of “quantum chaotic” systems is that their eigenspectra and eigenstates display universal statistical properties described by random matrix theory (RMT). However, eigenstates of local systems also encode structure beyond RMT. To capture this feature, we introduce a framework that allows us to compare the properties of eigenstates in local systems with those of pure random states. In particular, our framework defines a notion of distance between quantum state ensembles that utilizes the Kullback-Leibler divergence to compare the microcanonical distribution of entanglement entropy (EE) of eigenstates with a reference RMT distribution generated by pure random states (with appropriate constraints). This notion gives rise to a quantitative metric for quantum chaos that not only accounts for averages of the distributions but also higher moments. The differences in moments are compared on a highly resolved scale set by the standard deviation of the RMT distribution, which is exponentially small in system size. As a result, the metric can distinguish between chaotic and integrable behaviors and, in addition, quantify and compare the of chaos (in terms of proximity to RMT behavior) between two systems that are assumed to be chaotic. We implement our framework in local, minimally structured, Floquet random circuits, as well as a canonical family of many-body Hamiltonians, the mixed-field Ising model (MFIM). Importantly, for Hamiltonian systems, we find that the reference random distribution must be appropriately constrained to incorporate the effect of energy conservation in order to describe the ensemble properties of midspectrum eigenstates. The metric captures deviations from RMT across all models and parameters, including those that have been previously identified as strongly chaotic, and for which other diagnostics of chaos such as level spacing statistics look strongly thermal. In Floquet circuits, the dominant source of deviations is the second moment of the distribution, and this persists for all system sizes. For the MFIM, we find significant variation of the KL divergence in parameter space. Notably, we find a small region where deviations from RMT are minimized, suggesting that “maximally chaotic” Hamiltonians may exist in fine-tuned pockets of parameter space. Published by the American Physical Society 2024

Physics↗

DOE OSTI2014

aosco (01)

As of 5 August, 2015, Los Gatos Research (LGR) CO/H2O/N2O analyzer instruments (COANALYZERs) were deployed in the Atmospheric Radiation Measurement (ARM) Aerial Facility (AAF), the third ARM Mobile Facility (AMF3) Aerosol Observing System (AOS), Eastern North Atlantic (ENA) AOS, and Mobile AOS (MAOS-C). The N2O/CO analyzer uses LGR’s patented Off-axis ICOS technology, which employs a high-finesse optical cavity as the measurement cell. LGR’s technology has many proven advantages over conventional first-generation cavity ringdown spectroscopy (CRDS) techniques. In brief, since the laser beam does not have to be resonantly coupled to the measurement cell, precise beam alignment is not critical. Mentors can disassemble the cell for cleaning (CAREFULLY) the front surface mirrors. Analyzers are relatively inexpensive and inherently robust thermally and mechanically. In addition, since LGR’s technology can record reliable absorption spectra over a far wider range of optical depths (absorbance values) than CRDS, LGR analyzers provide measurements over a much wider range of mixing ratios (gas concentrations). The N2O/CO analyzer includes an internal computer that sends real-time data to the local instrument computer through its digital (RS-232) output.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1975

Mean flow field and surface heating produced by unequal shock interactions at hypersonic speeds

Mean velocity profiles were measured in a free shear layer produced by the interaction of two unequal strength shock waves at hypersonic free-stream Mach numbers. Measurements were made over a unit Reynolds number range of 3,770,000 per meter to 17,400,000 per meter based on the flow on the high velocity side of the shear layer. The variation in measured spreading parameters with Mach number for the fully developed flows is consistent with the trend of the available zero velocity ratio data when the Mach numbers for the data given in this study are taken to be characteristic Mach numbers based on the velocity difference across the mixing layer. Surface measurements in the shear-layer attachment region of the blunt-body model indicate peak local heating and static pressure consistent with other published data. Transition Reynolds numbers were found to be significantly lower than those found in previous data.

Birch, S. F.↗

NASA NTRS1975

Crop identification technology assessment for remote sensing (CITARS). Volume 10: Interpretation of results

The CITARS was an experiment designed to quantitatively evaluate crop identification performance for corn and soybeans in various environments using a well-defined set of automatic data processing (ADP) techniques. Each technique was applied to data acquired to recognize and estimate proportions of corn and soybeans. The CITARS documentation summarizes, interprets, and discusses the crop identification performances obtained using (1) different ADP procedures; (2) a linear versus a quadratic classifier; (3) prior probability information derived from historic data; (4) local versus nonlocal recognition training statistics and the associated use of preprocessing; (5) multitemporal data; (6) classification bias and mixed pixels in proportion estimation; and (7) data with differnt site characteristics, including crop, soil, atmospheric effects, and stages of crop maturity.

Bizzell, R. M.↗

NASA NTRS1982

Exchange of sulfur between the free troposphere, marine boundary layer, and the sea surface

A steady state analysis has been made of the sources and sinks of sulfur in the remote marine atmosphere and of the steady state exhanges of SO2 and sulfate between the sea, boundary layer, and free troposphere. Two situations were examined: an area of high biological productivity (Gulf of Guinea) and an area of low productivity (tropical Atlantic). The results of the analysis suggest that about one-third of the background concentrations of SO2 and excess sulfate observed in the remote marine atmosphere mixes in from the free troposphere, with the balance, about 100 micrograms S/sq m per day, attributed to the local oxidation of reduced sulfur-bearing precursors in the boundary layer.

Kritz, M. A.↗

NASA NTRS1983

Petrology of the Apollo 11 highland component

New data for 38 highland fragments hand-picked from Apollo 11 coarse fines are reported. Petrographic, mineralogic, and bulk chemical data show that: (1) the Apollo 11 highland component is non-KREEPy and like that of Apollo 16; (2) poikilitic rocks, granulitic breccias, and the anorthosite-norite-troctolite suite are the most abundant rock types, followed by polymict breccias and glasses; (3) both the ferroan anorthosite and Mg-rich plutonic suites are represented in the Apollo 11 highland component; (4) except for one sample, the intermediate-K Fra Mauro and high-K Fra Mauro groups are not represented. The data and observations are consistent with local derivation of the highland material from beneath relatively thin basalt flows and addition to the regolith via vertical mixing.

Simon, S. B.↗

NASA NTRS1985

On the existence and stability conditions for mixed-hybrid finite element solutions based on Reissner's variational principle

The extensions of Reissner's two-field (stress and displacement) principle to the cases wherein the displacement field is discontinuous and/or the stress field results in unreciprocated tractions, at a finite number of surfaces ('interelement boundaries') in a domain (as, for instance, when the domain is discretized into finite elements), is considered. The conditions for the existence, uniqueness, and stability of mixed-hybrid finite element solutions based on such discontinuous fields, are summarized. The reduction of these global conditions to local ('element') level, and the attendant conditions on the ranks of element matrices, are discussed. Two examples of stable, invariant, least-order elements - a four-node square planar element and an eight-node cubic element - are discussed in detail.

Karlovitz, L. A.↗

NASA NTRS1987

Vortex-scalar element calculations of a diffusion flame stabilized on a plane mixing layer

The vortex-scalar element method, a scheme which utilizes vortex elements to discretize the region of high vorticity and scalar elements to represent species or temperature fields, is utilized in the numerical simulations of a two-dimensional reacting mixing layer. Computations are performed for a diffusion flame at high Reynolds and Peclet numbers without resorting to turbulence models. In the nonreacting flow, the mean and fluctuation profiles of a conserved scalar show good agreement with experimental measurements. Results for the reacting flow indicate that for temperature independent kinetics, the chemical reaction begins immediately downstream of the splitter plate where mixing starts. Results for the reacting flow with Arrhenius kinetics show an ignition delay, which depends on reactant temperature, before significant chemical reaction occurs. Harmonic forcing changes the structure of the layer, and concomitantly the rates of mixing and reaction, in accordance with experimental results. Strong stretch within the braids in the nonequilibrium kinetics case causes local flame quenching due to the temperature drop associated with the large convective fluxes.

Ghoniem, Ahmed F.↗

NASA NTRS2005

The Mega Mesospheric Parachute

The current understanding and modeling of the upper reaches of the atmosphere is incomplete. Upper atmospheric interactions with the lower atmosphere, effects of ionizing radiation, high altitude cloud phenomena, and the dynamical interaction with the magnetosphere require greater definition. The scientific objective of obtaining a greater understanding of the upper atmosphere can be achieved by designing, implementing, testing, and utilizing a facility that provides long period in-situ measurements of the mesosphere. Current direct sub-sonic measurements of the upper atmosphere are hampered by the approximately one minute sub-sonic observation window of a ballistic sounding rocket regardless of the launch angle. In-situ measurements at greater than transonic speeds impart energy into the molecular atmospheric system and distort the true atmospheric chemistry. A long duration, sub-sonic capability will significantly enhance our ability to observe and measure: (1) mesospheric lightning phenomena (sprites and blue jets) (2) composition, structure and stratification of noctilucent clouds (3) physics of seasonal radar echoes, gravity wave phenomena (4) chemistry of mesospheric gaseous ratio mixing (5) mesospheric interaction of ionizing radiation (6) dynamic electric and magnetic fields This new facility will also provide local field measurements which complement those that can be obtained through external measurements from satellite and ground-based platforms. The 400 foot (approximately 130 meter) diameter lightweight mega-mesospheric parachute system, deployed with a sounding rocket, is proposed herein as a method to increase sub-sonic mesospheric measurement time periods by more than an order of magnitude. The report outlines a multi-year evolving science instrumentation suite in parallel with the development of the mega meso-chute facility. The developmental issues surrounding the meso-chute are chiefly materials selection (thermal and structural) and deployment mechanism physics. Three mission cases were conceived and developed to include cost and schedules estimates. Each scenario has increasing scientific utility with paralleling launch weight, parachute hang-time, deployment altitude, and parachute size: (1) Case #1: $8.4M@24 months, 6kg payload, 20 min., 50km alt., 80 m. dia. (2) Case #2: $10.4M@24 months, 6kg payload, 20 min., 60km alt, 130m. dia. (3) Case #3: $13.6M@36 months, 30kg payload, 30 min., 90km alt., 200m. dia. The initial breakout cost for the parachute system is approximately $2M@24 months. This report identifies that although the challenges of the mega-meso-chute may be difficult, they can be surmounted and valuable results can be achieved.

Kloesel, Kurt J.↗

NASA NTRS2016

Formaldehyde Column Density Measurements as a Suitable Pathway to Estimate Near-Surface Ozone Tendencies from Space

In support of future satellite missions that aim to address the current shortcomings in measuring air quality from space, NASA's Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) field campaign was designed to enable exploration of relationships between column measurements of trace species relevant to air quality at high spatial and temporal resolution. In the DISCOVER-AQ data set, a modest correlation (r2 = 0.45) between ozone (O3) and formaldehyde (CH2O) column densities was observed. Further analysis revealed regional variability in the O3-CH2O relationship, with Maryland having a strong relationship when data were viewed temporally and Houston having a strong relationship when data were viewed spatially. These differences in regional behavior are attributed to differences in volatile organic compound (VOC) emissions. In Maryland, biogenic VOCs were responsible for approx.28% of CH2O formation within the boundary layer column, causing CH2O to, in general, increase monotonically throughout the day. In Houston, persistent anthropogenic emissions dominated the local hydrocarbon environment, and no discernable diurnal trend in CH2O was observed. Box model simulations suggested that ambient CH2O mixing ratios have a weak diurnal trend (+/-20% throughout the day) due to photochemical effects, and that larger diurnal trends are associated with changes in hydrocarbon precursors. Finally, mathematical relationships were developed from first principles and were able to replicate the different behaviors seen in Maryland and Houston. While studies would be necessary to validate these results and determine the regional applicability of the O3-CH2O relationship, the results presented here provide compelling insight into the ability of future satellite missions to aid in monitoring near-surface air quality.

Surface Conditions from Column and Vertically Reso↗

NASA NTRS2016

New Approach to Characterize CO2 and CH4 Emissions over Sacramento, California Using an Airborne Aircraft Measurement

Emission fluxes of carbon dioxide (CO2) and methane (CH4) over Sacramento, California, USA, are estimated using an aircraft equipped with a cavity ring-down greenhouse gas sensor through the Alpha Jet Atmospheric eXperiment (AJAX). To better quantify the emission fluxes over the entire city and two small point sources within the area, we designed flights in a cylindrical pattern and computed the emission fluxes from 9 flights over all seasons using the Kriging method based on Gausss divergence theorem. The concentrations at the downwind side of Sacramento show somewhat persistent patterns among the 9 flights, but the magnitudes and locations of the fluxes vary depending on the individual weather conditions and seasonality on a given flight day. The net emission fluxes tend to be smaller in summer (July) than winter (November). Both trace gas mixing ratios as well as the wind speed and direction show high spatial variability both horizontally and vertically. The local maximum emission fluxes over a landfill and a rice field measured on July 29, 2015, were 2-3 times lower than the maximum measured over the entire city. These low emission fluxes suggest that not only the local source but also the transport of greenhouse gases due to diurnal and seasonal variation in winds have a strong effect on the CO2 and CH4 flux estimation of the both local emissions and city-size emissions. Our results highlight that the aircraft-based approach is effective and useful for capturing city-size emission fluxes and estimating the greenhouse gas emissions and its sources.

airborne↗

DOE OSTI2015

Effects of partitioned enthalpy of mixing on glass-forming ability

We explore the inherent reason at atomic level for the glass-forming ability of alloys by molecular simulation, in which the effect of partitioned enthalpy of mixing is studied. Based on Morse potential, we divide the enthalpy of mixing into three parts: the chemical part (Δ E{sub nn}), strain part (Δ E{sub strain}), and non-bond part (Δ E{sub nnn}). We find that a large negative Δ E{sub nn} value represents strong AB chemical bonding in AB alloy and is the driving force to form a local ordered structure, meanwhile the transformed local ordered structure needs to satisfy the condition (Δ E{sub nn}/2 + Δ E{sub strain}) < 0 to be stabilized. Understanding the chemical and strain parts of enthalpy of mixing is helpful to design a new metallic glass with a good glass forming ability. Moreover, two types of metallic glasses (i.e., “strain dominant” and “chemical dominant”) are classified according to the relative importance between chemical effect and strain effect, which enriches our knowledge of the forming mechanism of metallic glass. Finally, a soft sphere model is established, different from the common hard sphere model.

36 MATERIALS SCIENCE↗

NASA NTRS2002

Retrieval of Kinetic Temperature and Carbon Dioxide Abundance from Non-Local Thermodynamic Equilibrium Limb Emission Measurements made by the SABER Experiment on the TIMED Satellite

The Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) experiment was launched onboard the TIMED satellite in December, 2001. SABER is designed to provide measurements of the key radiative and chemical sources and sinks of energy in the mesosphere and lower thermosphere (MLT). SABER measures Earth limb emission in 10 broadband radiometer channels ranging from 1.27 micrometers to 17 micrometers. Measurements are made both day and night over the latitude range from 54 deg. S to 87 deg. N with alternating hemisphere coverage every 60 days. In this paper we concentrate on retrieved profiles of kinetic temperature (T(sub k)) and CO2 volume mixing ratio (vmr), inferred from SABER-observed 15 micrometer and 4.3 micrometer limb emissions, respectively. SABER-measured limb radiances are in non-local thermodynamic equilibrium (non-LTE) in the MLT region. The complexity of non-LTE radiation transfer combined with the large volume of data measured by SABER requires new retrieval approaches and radiative transfer techniques to accurately and efficiently retrieve the data products. In this paper we present the salient features of the coupled non-LTE T(sub k)/CO2 retrieval algorithm, along with preliminary results.

Mertens, Christopher J.↗

DOE OSTI2022

Understanding Lithium Local Environments in LiMn 0.5 Ni 0.5 O 2 Cathodes: A DFT-Supported 6 Li Solid-State NMR Study

LiMn 0.5 Ni 0.5 O 2 has been plagued by the structural failure driven by the irreversible phase change upon subsequent cycling and the structural degradation caused by the seemingly unavoidable Li/Ni exchange. This begs for a better understanding of the correlation between lithium local structures, synthesis conditions, and overall electrochemical properties of materials. In this study, we use density functional theory (DFT) to assist experimental 6 Li solid-state magic angle spinning (MAS) nuclear magnetic resonance (NMR) spectroscopy to understand the nature and change in lithium local structures with extended annealing times (168 vs 15 h) synthesized at 900 °C. To correlate the NMR peak changes after different synthesis conditions, we calculated the NMR spectra of representative low-energy model configurations of LiMn 0.5 Ni 0.5 O 2 composition–zigzag, row, and flower structures–as well as the influence of Ni/Mn ordering and Li/Ni exchange on each spectrum using a supercell that is large enough to allow us to consider the effect of different relative configurations of adjacent transition metal (TM) layers. The analysis based on a combination of the calculated NMR and the experimental spectra suggests that most configurations contributing to the experimental spectra are in fact composed of a blend of configurations higher in energy than the classical well-ordered ground-state structures. Further, the extended annealing of LiMn 0.5 Ni 0.5 O 2 slightly enhances Ni/Mn and Li/Mn orderings while reducing the Li/Ni mixing ratio. This study shows how DFT calculations are crucial in providing a better understanding of the experimental characterization data and therefore local environments and domain structures in oxide materials, such as Li-ion battery cathodes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗