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All sources NASA NTRS DOE OSTI

DOE OSTI2022

THERMAL MODELING OF HANFORD LEAD CANISTER’S HEATER BENCH TESTS

A computational fluid dynamics (CFD) model was built to simulate planned testing of heater assemblies for the Hanford Lead Canister (HLC) project. The HLC is a canister storage system that will contain heaters to simulate the decay heat of nuclear material and provide the canister storage system with environmental conditions equivalent to the operating conditions on a dry storage pad. The HLC will be equipped with long-term data collection and monitoring systems to provide an early warning of corrosion, pitting, cracking, or other signs of canister degradation that might threaten the integrity of the containment boundary over the potentially long term of dry storage. An important part of the HLC development is to confirm the function and ability of the electric heater assemblies that were specially designed to provide heating similar to the decay heat of nuclear material contained within the canister storage system. Heater bench testing is planned for early 2022 in a test configuration that does not include the canister. The goal of the bench testing is to verify that the heaters can replicate the decay heat of a canister with nuclear material and to validate the thermal models, which are critical to understanding the HLC’s thermal environment, including the local air flow within the canister storage system. Testing of the heater assemblies inside the canister system are planned in the future to validate canister level thermal models, and rigorous pre-deployment testing of the complete HLC cask and canister system is intended to be completed before the HLC is deployed in the 2025-2026 timeframe. This study presents the pre-test temperature predictions of the bench testing. A description of the heater assemblies and planned bench testing is presented. The model was developed with the commercial CFD code STAR-CCM+. An uncertainty analysis was run with the CFD model to determine the uncertainty in the temperature predictions and provide a range over which the predicted temperatures are expected to vary. The uncertainty analysis was performed by coupling STAR-CCM+ with the software Dakota, which provides advanced parametric analyses, including quantification of margins and uncertainty with computational models. This work is expected to provide insight into SNF canister behavior.

Suffield, Sarah R.↗

DOE OSTI2026

Photoelectrode Durability in Two- versus Three-Electrode Configurations: Understanding the Impact of Circuit Configuration on Water-Splitting Stability

Device durability remains a significant challenge in photoelectrochemical (PEC) water splitting under ambient conditions. Yet, a lack of understanding of the test configuration and applied bias effects continue to hinder progress. In this study, we differentiate two-electrode (2E) and three-electrode (3E) configurations for evaluating PEC material durability, focusing particularly on their impacts on photoabsorber solid-state operating conditions. Our results underscore the fallacy of inferring 2E device stability from durability measurements performed solely in 3E configurations. Unmeasured and often misunderstood total circuit bias in 3E tests moderates material degradation, leading to the overestimation of photoelectrode stability compared to short-circuit operation. We demonstrate how the photoabsorber's operating voltage critically governs charge separation, surface stability, and degradation mechanisms during PEC operation. With these findings, we propose a standardized framework for conducting more reliable 3E durability experiments that simulate unassisted performance to help accelerate the development of robust, stable materials for solar-driven water splitting.

08 HYDROGEN↗

DOE OSTI2021

Volatile aldehyde emissions from “sub-ohm” vaping devices

"Sub-ohm" atomizers with reduced resistance can deliver more power than conventional electronic cigarettes. Typical battery outputs are 100 watts or more. These devices are particularly popular among young users, and can be a significant source of volatile carbonyls in the indoor environment. Emissions from next-generation sub-ohm vaping products were characterized by determining e-liquid consumption and volatile aldehydes emissions for several combinations of popular high-power configurations. Tests explored the effect of dilution air flow (air vent opening), puffing volume, and coil assembly configuration. The mass of liquid consumed per puff increased as the puff volume increased from 50 to 100 mL, then remained relatively constant for larger puff volumes up to 500 mL. This is likely due to mass transfer limitations at the wick and coil assembly, which reduced the vaporization rate at higher puff volumes. Carbonyl emission rates were systematically evaluated using a 0.15 Ω dual coil atomizer as a function of the puffing volume and dilution air flow, adjusted by setting the air vents to either 100% (fully open), 50%, 25%, or 0% (closed). The highest formaldehyde emissions were observed for the lowest puff volume (50 mL) when the vents 31 were closed (48 ng mg-1), opened at 25% (39 ng mg -1 ) and at 50% (32 ng mg -1 ).. By contrast, 50-mL puffs with 100% open vents, and puff volumes >100 mL for any vent aperture, generated formaldehyde yields of 20 ng mg -1 or lower, suggesting that a significant cooling effect resulted in limited carbonyl formation. Considering the effect of the coil resistance when operated at a voltage of 3.8 V, the amount of liquid evaporated per puff decreased as the resistance increased, in the order of 0.15 Ω > 0.25 Ω > 0.6 Ω consistent with decreasing aerosol temperatures measured at the mouthpiece. Three different configurations of 0.15 Ω coils (dual, quadruple and octuple) were evaluated, observing significant variability. No clear trend was found between carbonyl emission rates and coil resistance or configuration, with highest emissions corresponding to a 0.25 Ω dual coil atomizer. Carbonyl emission rates were compared with those determined using the same methodology for conventional e-cigarettes (lower power tank systems), observing overall lower yields for the sub-ohm devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Prediction of Aluminum to Steel RSW Joint Failure (CRADA 405)

General Motors, LLC has developed a resistance spot welding process to join aluminum sheet to steel for body-in-white manufacturing. Efforts to develop the process for any one joint configuration (combination of alloy and thicknesses) is intensive. To aid in process understanding and eventual reduction in process development efforts, an initiative was created to develop an finite element model of the various destructive test configurations (lap shear, cross-tension, and coach peel) to help predict the failure mode and load displacement curves under tensile testing. This report describes the finite element modeling approach, the means by which local material properties were determined, as well as model validation and refinement efforts.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Evolution of Permeability in Sandstone During Confined Brazilian Testing

Permeability measurements were made on sandstone during confined Brazilian strength tests. The test involves 50 mm diameter disk-shaped, jacketed samples that are subjected to confining stresses while they are diametrically loaded. Specially designed end caps allow for concurrent gas flow measurements. The test configuration allows for the samples to be subjected to a range of stresses, with the confining stress as the intermediate principal stress. Furthermore, the majority of the tests measured permeability during loading to failure in the confined extension region. The permeability of the sandstone sample increases significantly well before the peak load is reached due to newly formed microcracks that continue to coalesce and dilate with further loading. Permeability increases are inversely proportional to the intermediate principal stress as increased confining pressures suppress growth, coalescence, and dilation of microcracks. Additional testing includes unloading and reloading cycles prior to failure. With each unloading–reloading cycle, permeability at comparable stresses is increased compared to the previous cycle, consistent with increasing damage in the form of an expanding microcrack network.

58 GEOSCIENCES↗

DOE OSTI2023

The effect of current and lambda on white-etch-crack failures

White etching cracks (WECs) have been associated with premature failure of wind turbine roller bearings. Various drivers for the generation of WECs have been identified such as loading conditions, slip, steel quality, lubrication, hydrogen embrittlement, corrosion fatigue cracking, and stray electrical currents passing through the surface. Here, in this work, a benchtop test rig utilizing a three-ring-on-roller test configuration was used to investigate the effect of electrical current and operation in different lubricating regimes, defined by lambda (λ), on high-quality bearing steel samples tested in a commercially available power transmission EP gear lubricant. It was observed that there is an inverse correlation between the magnitude of electric current applied to the ring/ roller system and time-to-failure. Higher current magnitudes lead to shorter time-to-failure than lower current magnitudes, with macropitting as the main failure mode. Sub-surface investigation revealed the presence of WECs in all cases. For the same current magnitude, tests conducted in boundary and mixed lubrication regimes showed that time-to-failure increased as lambda increased, and the tests resulted in WEC related macropits, whereas tests conducted in near-hydrodynamic regime resulted in surface damage with no macropit. It was also noted that a shift toward near-hydrodynamic lubrication resulted in a distinct surface distress on the roller surface. Furthermore, there seems to be a transition in the mixed regime during which the surface distress occurred. The damage on the surface of the test samples resembled non-spatially, periodic, groove-like corrugations and, in some cases, crater-like depressions. Sub-surface imaging, performed by sequential sectioning, revealed the presence of WECs in all cases, and broad, branching cracks that were more prevalent under the more severe boundary conditions.

17 WIND ENERGY↗

DOE OSTI2022

Hydrodynamics and Load Shedding Behavior of a Variable-Geometry Oscillating Surge Wave Energy Converter (OSWEC)

In order to improve their long-term viability, wave energy converters (WECs) need to be able to shed loads when a threshold wave condition is exceeded. As shown by Tom et al. (2016) [1], provision of adjustable flaps within the body of an oscillating surge wave energy converter (OSWEC) allows wave energy to pass through the device. A control system may then be able to open and close the flaps when waves approaching the device exceed preset thresholds. The variable-geometry OSWEC (VG-OSWEC) concept studied in this paper is a bottom-hinged, rectangular wave paddle with five flaps of elliptical cross-section embedded into the face of the paddle. System ID tests were conducted on this VG-OSWEC device at a 1:14 scale in a wave basin. Free decay tests showed that the damping was distinctly nonlinear when the flaps were fully open, and the natural frequency increased by 40% when compared with the flaps in a fully closed configuration. Tests with regular wave conditions were used to develop the response amplitude operator for the rotational motion about the hinge. These response amplitude operator results when compared with numerical simulations run using WEC-Sim/WAMIT and ANSYS AQWA, show strong agreement with the flap open and closed conditions. The regular-wave condition measurements also show that the wave excitation moment about the hinge was reduced by up to 60% when the flaps were fully open. The experiments serve to demonstrate the potential of the variable geometry design to shed loads and survive harsh ocean environments.

load shedding↗

DOE OSTI2020

Crystalline Silicotitanate Batch Contact Testing with Ba, Ca, Pb, and Sr

Washington River Protection Solutions is working to support initial production of immobilized low-activity waste (LAW) by feeding Hanford tank supernate from tank farms to the Hanford Waste Treatment and Immobilization Plant (WTP) LAW Facility. This goal incorporates the design of a Tank Side Cesium Removal system, which filters tank waste supernate to remove suspended solids and then removes Cs by processing it through crystalline silicotitanate (CST) ion exchange media manufactured by Honeywell UOP, LLC. The 137 Cs-depleted product is intended to be sent to the WTP for vitrification. Processing of actual tank waste supernate showed effectively complete uptake of Sr and Ba by CST and significant uptake of Ca. Further, Campbell et al. (2019) analyzed CST post-column testing and found significant (>1E-2 mmoles/g) uptake of Ca and Pb along with some Ba, Cd, Fe, Sr, and U. This led to concern that selected metals, particularly the +2 cations, Ca, Sr, Ba, and Pb may be consuming Cs exchange sites and possibly reducing CST capacity for Cs. Exchange of +2 cations was assumed to be associated with the M(OH) + species for the metal (M) ion in the caustic solution. A series of batch contact testing was conducted to evaluate the exchange behavior of Ba, Ca, Pb, and Sr onto CST. The Cs exchange behavior was also tested as a benchmark for direct comparisons. The CST was provided in the sodium form by Honeywell UOP, as IONSIV TM R9140-B, Lot 2002009604, 18 x 50 mesh. A <30-mesh aliquot was collected to match the sieve fraction expected for use in upcoming small column test configurations. Kinetic exchange rate and isotherms were measured at metal concentrations benchmarked from the AP-107 tank waste feed composition and as limited by the metal solubility in the alkaline solution. Two simplified matrices were tested: 1) 1.0 M NaOH/4.6 M NaNO 3 and 2) 0.1 M NaOH/5.5 M NaNO 3 ; these matrices represented the expected 5.6 M Na concentration of process feed and served to address the hydroxide concentration effect on exchange behavior.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Field Testing of PID-p Susceptible Bifacial PERC Modules: Impact of Light, Voltage and Module History

This work investigates the potential induced degradation-polarization (PID-p) of bifacial passivated emitter and rear contact (PERC) modules installed in the field at the Florida Solar Energy Center. 22 modules were stressed over 1 year under various voltage (-1500V, -3500, +1500V) and mounting configurations (close to ground, 2 meters from ground, close to roof). The positively stressed modules were anticipated to have experiences PID-p on their front side. However, no degradation was observed, as the light-induced recovery effect effectively counteracted the degradation. The negatively stressed modules experienced Pmax drops during 2 weeks before stabilizing at 5-6% loss. I-V and EL characteristics suggest a PID-p degradation on the rear side. Lower degradation rates are observed with lower voltage and when the mounting configuration allows more albedo light on the rear side to compensate for the degradation. PID-p is observed to stabilize at similar level for the voltage and mounting configuration tested with slightly lower Pmax in winter. EL imaging reveals that cells are not degrading at the same rate across a module. Some cells get darker and then brighter which corresponds to the silicon/passivation interface going through depletion and then inversion when enough positive charges are accumulated. After full light-recovery, the modules were tested again along with 22 brand-new ones to assess the impact of the module history. Results confirmed the trends observed in the first year with PID-p occurring at voltage as low as -600V and recovered modules degrading faster than brand-new ones.

14 SOLAR ENERGY↗

DOE OSTI2025

Quantifying particle movement in a spout-fluidized bed with irregular feedstock morphology

Here, the spout-bed fluidization behavior of nonspherical, 140 μm SiC feedstock was quantified via particle image velocimetry for varying gas distributor geometries. A bench-scale, room-temperature fluidization setup was assembled to model a 50 mm fluidized bed chemical vapor deposition (FB-CVD) system, and fluidized bed motion was captured using a high-speed camera. Modular tips with varying inlet geometries were 3D printed and tested on the bench-scale rig using identical feedstock and gas flow rates in the range of 3.0–9.0 L/min. Fluidization behavior was quantified by extracting parameters of the bed velocity, frequency, dead time, and other measurements, which were ranked for each inlet geometry configuration tested. The results from this work demonstrate that changing the path of inlet gas flow can significantly change the hydrodynamics within a spout-fluidized bed under identical feedstock, loading, and flow rate conditions, potentially enabling experimental control of particle fluidization behavior for a given condition. Moreover, composite rankings of fluidization behavior for unique distributor geometries hold potential to guide the design of FB-CVD experiments for various engineering and scientific applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Carbonate clumped isotope analysis (Δ 47 ) of 21 carbonate standards determined via gas‐source isotope‐ratio mass spectrometry on four instrumental configurations using carbonate‐based standardization and multiyear data sets

Rationale Clumped isotope geochemistry examines the pairing or clumping of heavy isotopes in molecules and provides information about the thermodynamic and kinetic controls on their formation. The first clumped isotope measurements of carbonate minerals were first published 15 years ago, and since then, interlaboratory offsets have been observed, and laboratory and community practices for measurement, data analysis, and instrumentation have evolved. Here we briefly review historical and recent developments for measurements, share Tripati Lab practices for four different instrument configurations, test a recently published proposal for carbonate‐based standardization on multiple instruments using multi‐year data sets, and report values for 21 different carbonate standards that allow for recalculations of previously published data sets. Methods We examine data from 4628 standard measurements on Thermo MAT 253 and Nu Perspective IS mass spectrometers, using a common acid bath (90°C) and small‐sample (70°C) individual reaction vessels. Each configuration was investigated by treating some standards as anchors (working standards) and the remainder as unknowns (consistency standards). Results We show that different acid digestion systems and mass spectrometer models yield indistinguishable results when instrument drift is well characterized. For linearity correction, mixed gas‐and‐carbonate standardization or carbonate‐only standardization yields similar results. No difference is observed in the use of three or eight working standards for the construction of transfer functions. Conclusions We show that all configurations yield similar results if instrument drift is robustly characterized and validate a recent proposal for carbonate‐based standardization using large multiyear data sets. Δ 47 values are reported for 21 carbonate standards on both the absolute reference frame (ARF; also refered to as the Carbon Dioxide Equilibrated Scale or CDES) and the new InterCarb‐Carbon Dioxide Equilibrium Scale (I‐CDES) reference frame, facilitating intercomparison of data from a diversity of labs and instrument configurations and restandardization of a broad range of sample sets between 2006, when the first carbonate measurements were published, and the present.

58 GEOSCIENCES↗

DOE OSTI2025

How does ion temperature gradient turbulence depend on magnetic geometry? Insights from data and machine learning

Magnetic geometry has a significant effect on the level of turbulent transport in fusion plasmas. Here, we model and analyse this dependence using multiple machine learning methods and a dataset of >200 000 nonlinear gyrokinetic simulations of ion-temperature-gradient turbulence in diverse non-axisymmetric geometries. The dataset is generated using a large collection of both optimised and randomly generated stellarator equilibria. At fixed gradients and other input parameters, the turbulent heat flux varies between geometries by several orders of magnitude. Trends are apparent among the configurations with particularly high or particularly low heat flux. Regression and classification techniques from machine learning are then applied to extract patterns in the dataset. Due to a symmetry of the gyrokinetic equation, the heat flux and regressions thereof should be invariant to translations of the raw features in the parallel coordinate, similar to translation invariance in computer vision applications. Multiple regression models including convolutional neural networks (CNNs) and decision trees can achieve reasonable predictive power for the heat flux in held-out test configurations, with highest accuracy for the CNNs. Using Spearman correlation, sequential feature selection and Shapley values to measure feature importance, it is consistently found that the most important geometric lever on the heat flux is the flux surface compression in regions of bad curvature. The second most important geometric feature relates to the magnitude of geodesic curvature. These two features align remarkably with surrogates that have been proposed based on theory, while the methods here allow a natural extension to more features for increased accuracy. The dataset, released with this publication, may also be used to test other proposed surrogates, and we find that many previously published proxies do correlate well with both the heat flux and stability boundary.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

Analysis of the HAE activity in the TJ-II stellarator using a Landau closure model

The aim of this study is to analyze the stability of helical Alfvén eigenmodes (HAEs) in TJ-II discharges and the stabilizing effect of the energetic particles generated by the neutral beam injector (NBI) on pressure gradient-driven modes (PGDMs). HAE and PGDM stability is studied using the linear version of the gyro-fluid code FAR3d and the continuous structure by the STELLGAP code. First, Alfvén eigenmode (AE) and PGDM activity observed in the experiments is reproduced by the simulations, identifying unstable m/n = 4/7 − 2/3 and 7/12 − 5/8 HAEs triggered around ρ = 0.66 showing a frequency of 209 and 204 kHz, respectively, as well as 5/3 PGDM. Next, a parametric study is performed with respect to the thermal ion density and iota profile in the middle-outer plasma region to verify the robustness of the simulation results with respect to the uncertainty of experimental profiles. The analysis confirms that experimental uncertainty does not cause large deviations in the simulation results, showing the destabilization of the same HAEs for all the configurations tested. The simulations also indicate the decay of the 5/3 PGDM growth rate as the energetic particle (EP) population in the plasma increases, consistent with the experiment. Stability analysis of the n = 3, 7, 11, n = 5, 9, 13, n = 6, 10, 14, and n = 8, 12 helical families is performed with respect to the NBI operational regime for different EP energies, β as well as deposition profiles. The most unstable configuration is the radially localized on-axis NBI operation (stiff EP density profile gradients nearby the magnetic axis). Using the simulation model that reproduces the observed Alfvén activity, we extend the study to analyze NBI performance within a theoretical framework. It shows that increasing NBI voltage (which raises EP energy) leads to a degradation in NBI performance for a given power (related to EP β and their density). To achieve better NBI operation, higher voltage must be balanced with lower injection power, ensuring stable AEs while keeping the same EP β.

Plasma confinement↗

DOE OSTI2025

Design of Critical Experiments Involving Graphite elements at the IPEN/MB-01 Plate-Type Core

A series of critical experiments were designed involving the use of characterized graphite elements in the new plate-type core of the IPEN/MB-01 reactor. Eleven configurations with different graphite quantities are considered, each producing distinct effects on neutron fluxes and offering opportunities to analyze varying sensitivities to k eff in the system. The analysis shows that the experiments can be performed with acceptably low k eff uncertainties considering an adequate characterization of the graphite elements to be used. The sensitivity results obtained using SCALE TSUNAMI calculations show that the experiments have a notable k eff sensitivity coefficient to graphite. In the configurations tested, the k eff sensitivity to graphite TSL is low. This experiment will be useful for criticality safety validation of applications using uranium fuel enriched to around 19.75 wt % 235 U, light water and graphite. It will also be useful to gain more insight into graphite material properties and their effect on k eff as a result of using the well-characterized graphite elements. The execution of the experiments is planned for the summer of 2025. The 11 designed configurations serve as a basis for the final design, and fewer configurations will be executed. Once executed, these critical experiments will be evaluated and submitted for publication in the International Criticality Safety Benchmark Evaluation Project Handbook, supporting the DOE/NRC Collaboration for Criticality Safety Support for Commercial-Scale HALEU for Fuel Cycles and Transportation project goal.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2023

A conservative, interface-resolved, compressible framework for the modeling and simulation of liquid/gas phase change

This paper presents a method for simulating evaporation in a compressible, interface-resolved framework appropriate for modeling problems of engineering interest. In order to achieve robustness and broad applicability, the method has been designed to discretely enforce consistent mass and thermal energy transport at the phase interface, to globally conserve mass, momentum, and energy, and to be capable of modeling compressible and incompressible systems. Verification is performed via the Sod-shock test, one-dimensional heat conduction, evaporation from a planar interface, and evaporation of three-dimensional droplets. Convergence with increasing mesh resolution is demonstrated in all tested configurations, and conservation is maintained near machine precision for a translating droplet. Conservation and accurate phase change rates are preserved at the low numerical resolutions commonly encountered in engineering calculations. Following verification, the method is validated by comparison to an empirical correlation for evaporating droplets in high temperature crossflow, and the presentation concludes with the simulation of an iso-octane spray at conditions representative of gasoline direct injection. In conclusion, successful verification, validation, and demonstrated practical utility suggest the method to be an accurate, efficient, and robust approach for the study of phase change in engineering systems.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2022

Integrated simulation, machine learning, and experimental approach to characterizing fracture instability in indentation pillar-splitting of materials

Measuring fracture toughness of materials at small scales remains challenging due to limited experimental testing configurations. A recently developed indentation pillar-splitting method has shown promise of improved flexibility in fracture toughness measurements at the microscale, partly due to the occurrence of an unusual fracture instability, i.e., a transition from stable to unstable crack propagation. In spite of growing interest in this method, the underlying mechanism of this phenomenon is yet to be elucidated. Furthermore, we provide a comprehensive description of fracture instability in indentation pillar-splitting by combining in situ experiments with high-fidelity simulations based on cohesive zone and J-integral methods. In addition, a machine-learning-based solution for predicting the critical indentation load of fracture instability is established through Gaussian processes regression for broad use of this method by the community.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Extraction and selective promotion of zero-group velocity and cutoff frequency resonances in bi-dimensional waveguides using the electromechanical impedance method

This study showcases the electromechanical impedance (EMI) technique for extracting and promoting zero-group velocity (ZGV) and cutoff frequency resonances in a waveguide structure. Here, we identify the mechanisms of multiple resonances in the EMI spectra via a wave propagation perspective. Both simulation and experiments reveal the fact that sharp resonances in the conductance spectra are associated with either ZGV or cutoff frequency points. Consequently, we design four test configurations to enhance local resonances by aligning induced motions with considered mode shapes. Reasonable agreement between simulation and experiment results is observed. We evaluate the performance of considered configurations in terms of mode enhancement, and configurations that can selectively promote certain mode families are summarized. This study also shines the light on the EMI technique for quantitative non-destructive evaluation (NDE) by potentially supporting the inverse characterization of mechanical properties of host structures.

42 ENGINEERING↗

DOE OSTI2024

Quantifying the thermal effect and methyl radical production in nanosecond repetitively pulsed glow discharges applied to a methane-air flame

In this work, we investigated non-equilibrium plasma produced by nanosecond repetitively pulsed glow discharges applied across a lean premixed methane-air flame. The flame is stationary, axisymmetric, and laminar. The discharges are applied on the symmetry axis crossing the reactant gases, flame front, and product gases, allowing phase-locked averaged measurements and comparisons with axisymmetric numerical simulations. The thermal effect and methyl radical production are quantified in the discharge in the reactant gas region. One-dimensional, two-beam, hybrid, femtosecond-picosecond, coherent anti-Stokes Raman scattering is used to acquire spatial and temporal profiles of temperature and oxygen-to-nitrogen concentration ratio. Photo-fragmentation laser-induced fluorescence is used to acquire quantitative two-dimensional profiles of methyl radicals in the discharge providing the first quantitative imaging of methyl produced ahead of a flame by plasma-induced methane dissociation. The spatial profiles of temperature and oxygen-to-nitrogen concentration ratio are in steady state, indicating that individual discharges have an insignificant heating effect. Upper and lower bounds of the produced mole fraction of methyl radicals in the plasma are obtained due to uncertainties in the collisional quenching rates of excited state methylidyne radicals in the plasma. The discharges produce a maximum of 600–1100 ppm of methyl radicals upstream of the flame front within 25 ns. This amount is similar to the predicted methyl mole fraction for the flame without plasma and thus represents a significant chemical perturbation to the reactants upstream of the flame front. The produced methyl follows an exponential decay in the first microsecond after the discharge with a decay constant of 8 µs close to the flame, and 0.8 µs further from the flame. The decay then deviates from the exponential curve and the methyl persists for tens of microseconds. The results suggest that for the tested configuration, the thermal effect of individual discharges through fast gas heating is negligible, while active chemical species are produced in large quantities in the reactant gases, upstream of the flame front.

hybrid fs-ps CARS↗