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DOE OSTI2021

Ultrafast X-ray scattering offers a structural view of excited-state charge transfer

Intramolecular charge transfer and the associated changes in molecular structure in N,N'-dimethylpiperazine are tracked using femtosecond gas-phase X-ray scattering. The molecules are optically excited to the 3p state at 200 nm. Following rapid relaxation to the 3s state, distinct charge-localized and charge-delocalized species related by charge transfer are observed. The experiment determines the molecular structure of the two species, with the redistribution of electron density accounted for by a scattering correction factor. The initially dominant charge-localized state has a weakened carbon–carbon bond and reorients one methyl group compared with the ground state. Subsequent charge transfer to the charge-delocalized state elongates the carbon–carbon bond further, creating an extended 1.634 Å bond, and also reorients the second methyl group. At the same time, the bond lengths between the nitrogen and the ring-carbon atoms contract from an average of 1.505 to 1.465 Å. The experiment determines the overall charge transfer time constant for approaching the equilibrium between charge-localized and charge-delocalized species to 3.0 ps.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Observation of laser ablation of silicon as a function of pulse length at constant fluence via time-resolved x-ray spectroscopy

We investigate the ablation of silicon as a function of laser pulse length at a constant fluence using time-resolved x-ray spectroscopy data obtained from OMEGA EP experiments at the University of Rochester's Laboratory for Laser Energetics. Our targets consisted of three-layer planar structures composed of Si (50 μm), Cu (25 μm), and SiO 2 (500 μm) layers. The Si layer was irradiated by a 351-nm laser with varying pulse widths of 250 ps, 500 ps, 1 ns, and 10 ns while maintaining a constant fluence of ~27.9 kJ/cm 2 . Electron temperatures and densities of the ablated plasma were determined by analyzing the time-resolved x-ray spectroscopy data through a comparison of experimental measurements with synthetic results obtained from Si atomic calculations in a steady state and non-local thermodynamic equilibrium. These calculations were computed using PrismSPECT. Additionally, radiation-hydrodynamics simulations with FLASH are used to generate simulated plasma-density and plasma-temperature profiles, which are then compared with the experimental measurements. Our analyses reveal that increasing the laser pulse length at a constant fluence results in a decrease in electron temperatures and densities. Furthermore, the longer pulses with lower intensities lead to deeper ablation regions before reaching the peak ablation but lower ionization balances in the silicon layer. Furthermore, these findings emphasize the critical role of laser pulse length in plasma ablation and shock generation for laser-impulse studies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Spatially-resolved measurements of spin valley polarization in MOCVD-grown monolayer WSe 2

Time-resolved Kerr rotation microscopy is used to generate and measure spin valley polarization in MOCVD-grown monolayer tungsten diselenide (WSe 2 ). The Kerr signal reveals bi-exponential decay with time constants of 100 ps and 3 ns. Measurements are performed on several triangular flakes from the same growth cycle and reveal larger spin valley polarization near the edges of the flakes. This spatial dependence is observed across multiple WSe 2 flakes in the Kerr rotation measurements but not in the spatially resolved reflectivity or microphotoluminescence data. Time-resolved pump-probe overlap measurements further reveal that the Kerr signal’s spatial dependence is not due to spin diffusion on the nanosecond timescale.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Quantum Dynamics of Attractive and Repulsive Polarons in a Doped MoSe 2 Monolayer

When mobile impurities are introduced and coupled to a Fermi sea, new quasiparticles known as Fermi polarons are formed. There are two interesting, yet drastically different regimes of the Fermi polaron problem: (i) the attractive polaron (AP) branch connected to pairing phenomena spanning the crossover from BCS superfluidity to the Bose-Einstein condensation of molecules and (ii) the repulsive branch (RP), which underlies the physics responsible for Stoner’s itinerant ferromagnetism. Here, we study Fermi polarons in two-dimensional systems, where many questions and debates regarding their nature persist. The model system we investigate is a doped MoSe2 monolayer. We find the observed AP-RP energy splitting and the quantum dynamics of attractive polarons agree with the predictions of polaron theory. As the doping density increases, the quantum dephasing of the attractive polarons remains constant, indicative of stable quasiparticles, while the repulsive polaron dephasing rate increases nearly quadratically. The dynamics of Fermi polarons are of critical importance for understanding the pairing and magnetic instabilities that lead to the formation of rich quantum phases found in a wide range of physical systems including nuclei, cold atomic gases, and solids.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Structural and electronic properties of rare-earth chromites: A computational and experimental study

Here, in this work, the structural, optical, and electronic properties of rare-earth perovskites of the general formula R⁢ CrO 3 , where R⁢ represents the rare-earth Gd, Tb, Dy, Ho, Er, and Tm, have been studied in detail. These compounds were synthesized through a facile citrate route. X-ray diffraction, Raman spectroscopy, and UV-Visible spectroscopy were utilized to reveal the structural evolutions in R⁢ ⁢CrO 3 . The lattice parameters, Cr 3+ –O 2 –Cr 3+ bond angle, and CrO 6 octahedral distortions were found to strongly depend on the ionic radii of R⁢ . First-principles calculations based on density-functional theory within the generalized gradient approximation (GGA) of Perdew-Burke-Ernzerhof (PBE) and strongly constrained and appropriately normed (SCAN) meta-GGA were also employed to calculate the structural and electronic properties of R⁢ ⁢CrO 3 . The ground-state energy, lattice constants, electronic structures, and density of states of R⁢ ⁢CrO 3 were calculated. These provide some insights into the electronic characteristics of the R⁢ ⁢CrO 3 compounds. The calculated values of lattice parameters and band gaps with Hubbard U correction (SCAN+ U ) agree well with values measured experimentally and show more accuracy in predicting the ground-state crystal structure and band structure compared to PBE+ U approximation. The band gap of R⁢ ⁢CrO 3 is found to be independent of the ionic radii of R⁢ from both experiments and calculations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

Multiplexing Focusing Analyzer for Efficient Stress-Strain Measurements

Statement of the problem or situation that is being addressed. Although thermal and cold neutron scattering is widely used and is critical for success in many areas of materials science and engineering, relatively low neutron fluxes severely limit applications of not only laboratory neutrons generators, but also large national neutron facilities. State-of-the-art thermal and cold neutron sources are large expensive national facilities, which serve diverse community of scientific and industrial users. The constant need to improve the instruments performance, stems from the fact that neutron methods are gaining in popularity, and becoming more and more powerful, while new neutron sources are not being constructed to keep pace with the developments and needs of the scientific community. Small research reactors at universities and National Labs, and laboratory-based neutron generators, are necessary not only for education and training, but also when samples cannot be transported to other facilities. However, the standard neutron techniques, which were developed for high-flux facilities, require much higher efficiencies to be used effectively with the low fluxes of small sources. Thus, the efficient use of neutron sources, such as with our proposed analyzer, is important for the progress and broader use of these neutron techniques. General statement of how this problem is being addressed. We propose to design and demonstrate novel diffractive optical device, which will enable very efficient residual stress neutron diffractometers. The proposed device will be a multi-foil analyzer, where each foil is constructed of focusing bent single crystals of Si. Such device will enable polychromatic residual stress neutron diffraction. At large national facilities, such as at Oak Ridge National Laboratory, these analyzers would enable very fast measurements for determining residual stress tensors, raster large samples or screen multiple samples. Commercial Applications and Other Benefits The outcome of this project would be the demonstration of commercial devices, novel neutron optical components, which could be utilized to improve the performance of existing instruments or build novel neutron scattering instruments at DOE neutron facilities and commercial laboratory neutron sources. These new devices will widen the scope of research conducted using neutrons and enable measurements not feasible at present. Summary for Members of Congress Thermal and cold neutron beams are a powerful materials science probe, which provide unique information about the structure of matter. The proposed innovations expand the reach of neutron-based investigations to new materials and industries by enabling new instrumentation capabilities, thereby greatly enhancing and expanding the role of small, laboratory-based neutron instrumentation, and improving education and training of neutron users.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2024

Preliminary results of the 2023 International Fermilab Booster Studies

Here, an overview is given of the methods and preliminary results from dedicated beam studies on three topics conducted over five days in July 2023. In the first study, the Fermilab Booster magnets were held constant at magnetic fields corresponding to the injection energy. The beam loss and emittance growth were observed under varying intensity, tunes, and sextupole resonances. The corresponding beam conditions were also simulated with the MADX-SC code [1]. In the second study, measurements of the vertical half-integer resonance and correction methods are conducted for high-intensity beams ramping in the Booster. Finally, syncho-betatron instabilities are observed during transition-crossing in the Booster under strong space-charge conditions.

43 PARTICLE ACCELERATORS↗

DOE OSTI2020

Orbital Motion, Variability, and Masses in the T Tauri Triple System

We present results from adaptive optics imaging of the T Tauri triple system obtained at the Keck and Gemini Observatories in 2015−2019. We fit the orbital motion of T Tau Sb relative to Sa and model the astrometric motion of their center of mass relative to T Tau N. Using the distance measured by Gaia, we derived dynamical masses of M{sub Sa}=2.05±0.14 M {sub ⊙} and M {sub Sb} = 0.43 ± 0.06 M{sub ⊙}. The precision in the masses is expected to improve with continued observations that map the motion through a complete orbital period; this is particularly important as the system approaches periastron passage in 2023. Based on published properties and recent evolutionary tracks, we estimate a mass of ∼2 M {sub ⊙} for T Tau N, suggesting that T Tau N is similar in mass to T Tau Sa. Narrowband infrared photometry shows that T Tau N remained relatively constant between late 2017 and early 2019 with an average value of K = 5.54 ± 0.07 mag. Using T Tau N to calibrate relative flux measurements since 2015, we found that T Tau Sa varied dramatically between 7.0 and 8.8 mag in the K band over timescales of a few months, while T Tau Sb faded steadily from 8.5 to 11.1 mag in the K band. Over the 27 yr orbital period of the T Tau S binary, both components have shown 3–4 mag of variability in the K band, relative to T Tau N.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Coupling, lifetimes, and “strong coupling” maps for single molecules at plasmonic interfaces

The interaction between excited states of a molecule and excited states of a metal nanostructure (e.g., plasmons) leads to hybrid states with modified optical properties. When plasmon resonance is swept through molecular transition frequency, an avoided crossing may be observed, which is often regarded as a signature of strong coupling between plasmons and molecules. Such strong coupling is expected to be realized when 2|$\langle$U$\rangle$|/ℏΓ > 1, where $\langle$U$\rangle$ and Γ are the molecule–plasmon coupling and the spectral width of the optical transition, respectively. Because both $\langle$U$\rangle$ and Γ strongly increase with decreasing distance between a molecule and a plasmonic structure, it is not obvious that this condition can be satisfied for any molecule–metal surface distance. Here, in this work, we investigate the behavior of $\langle$U$\rangle$ and Γ for several geometries. Surprisingly, we find that if the only contributions to Γ are lifetime broadenings associated with the radiative and nonradiative relaxation of a single molecular vibronic transition, including effects on molecular radiative and nonradiative lifetimes induced by the metal, the criterion 2|$\langle$U$\rangle$|/ℏΓ > 1 is easily satisfied by many configurations irrespective of the metal–molecule distance. This implies that the Rabi splitting can be observed in such structures if other sources of broadening are suppressed. Additionally, when the molecule–metal surface distance is varied keeping all other molecular and metal parameters constant, this behavior is mitigated due to the spectral shift associated with the same molecule–plasmon interaction, making the observation of Rabi splitting more challenging.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Robust In-Situ Strain Measurements to Monitor CO 2 Storage

The goal of this project was to develop and demonstrate robust instrumentation to monitor the in-situ strain tensor in order to improve the reliability and security of CO 2 storage in geologic formations. We met the original goals of the project and the major overarching accomplishment is the advancement of strain tensor monitoring from an intriguing concept to a commercially available technology with a solid foundation of novel instruments supported by theoretical analyses and validation experiments. The main accomplishments of the project are summarized below. We designed, built and evaluated nine new optical fiber strainmeters and tiltmeters using Michelson interferometers to measure deformation with ultra-high resolution at both shallow and deep point locations in the subsurface. These are the robust strainmeters that motivated the title of the project. We designed, built and evaluated a novel method of measuring distributed strain in optical fibers with nanostrain resolution, and cm-scale location, and sampling into the seismic band. The new method is called Coherence-length-gated Microwave Photonics Interfereometry (CMPI). CMPI technology has advantages over existing commercial DAS and DSS methods. We developed and demonstrated capabilities to deploy instruments in the field and used them to measure strain caused by ambient signals like barometric pressure and tides, as well as induced signals like surface loading and pore pressure changes from pumping tests. We deployed a working strainmeter at 1,700 ft depth, slightly above an active reservoir. This is to our knowledge the greatest depth a strainmeter has been deployed and the techniques we used can readily be extended to greater depths. Optical fiber borehole tensor strainmeter techology was advanced from a TRL 4 at the start, to a TRL of 7 at the conclusion of the project. The project included advances in simulations and theoretical analyses. We developed and demonstrated a computational workflow that uses machine learning to reduce the computational requirements and make it practical to use Bayesian inversion to solve large numerical poroelastic analyses needed to interpret strain tensor field data. We evaluated the strain tensor fields and time series that would be caused by leaks of CO 2 or other fluids from reservoirs. These simulations demonstrated that signals from leaks could be measured with instruments developed for the project, opening a potentially new method for ensuring storage security. We showed that strains in caprock can be used to estimate pressure in a reservoir. This avoids the need to drill monitoring wells into the reservoir, and it expands the capabilities of monitoring in the caprock. The project includes a derivation and application of a novel analytical solution to the strains in the vicinity of a pressurized poroelastic inclusion. This solution explains field data measured during injeciton tests at the North Avant Field, and it will simplify future interpretation of strain tensor data. The project included a broad range of experiments, and of the most significant is the characterization of the strain tensor at an array three strainmeters during six injection tests at the North Avant Field, Oklahoma. This demonstrated repeatability of the strain signal measured by the new instruments developed for the project, and it showed similarities between the strain signal at shallow depths and pressure in the underlying reservoir. We also demonstrated that useful strain data can be measured at reservoir depths. This confirms that strain tensor data can be measured throughout the caprock over a reservoir. The project demonstrated the feasibility of using the strain tensor and distributed strain measured in caprock during a variety of different well tests where the pumping rate was constant, sinusoidal and positive, or a periodic square wave with zero net rate. This further strengthens the validity of using strain data to characterize reservoirs and aquifers. We also demonstrated that strain caused be fluctuations of air pressure and water pressure in the vadose zone can be measured and interpreted, suggesting that high resolution distributed strain measurements hold promise for monitoring the vadose zone. The project partially supported nine graduate students in the Environmental Engineering, Hydrogeology, Electrical Engineering programs at Clemson University. The research was described in nine journal papers, 23 talks and conference abstracts. Additional journal papers are in preparation. A new company called Tensora was started to provide strainmeter technology for commercial applications.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2022

Water-Accelerated Photooxidation of CH 3 NH 3 PbI 3 Perovskite

Optical absorbance is used to study the kinetics of methylammonium lead iodide (MAPbI 3 ) thin film degradation in response to combinations of moisture, oxygen, and illumination over a range of temperatures. 105 degradations were conducted over 41 unique environmental conditions. We discover that water acts synergistically with oxygen in a water-accelerated photo-oxidation (WPO) pathway. This pathway is the dominant pathway at 25 °C and is 10, 100, 1000, and >1000 times faster than dry photooxidation (DPO), degradation via hydrate formation, thermal degradation, and blue light degradation, respectively. We find that the rate determining step for DPO is proton abstraction from methylammonium while for WPO it is proton abstraction from water, which occurs at a faster rate and results in water acting as an accelerant for photooxidation of MAPbI 3 . A full kinetic rate equation is derived and fitted to the data to determine activation energies and rate constants.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Ligand Desorption and Fragmentation in Oleate-Capped CdSe Nanocrystals under High-Intensity Photoexcitation

Semiconductor nanocrystals (NCs) offer prospective use as active optical elements in photovoltaics, light-emitting diodes, lasers, and photocatalysts due to their tunable optical absorption and emission properties, high stability, and scalable solution processing, as well as compatibility with additive manufacturing routes. Over the course of experiments, during device fabrication, or while in use commercially, these materials are often subjected to intense or prolonged electronic excitation and high carrier densities. The influence of such conditions on ligand integrity and binding remains underexplored. Here, in this study, we expose CdSe NCs to laser excitation and monitor changes in oleate that is covalently attached to the NC surface using nuclear magnetic resonance as a function of time and laser intensity. Higher photon doses cause increased rates of ligand loss from the particles, with upward of 50% total ligand desorption measured for the longest, most intense excitation. Surprisingly, for a range of excitation intensities, fragmentation of the oleate is detected and occurs concomitantly with formation of aldehydes, terminal alkenes, H 2 , and water. After illumination, NC size, shape, and bandgap remain constant although low-energy absorption features (Urbach tails) develop in some samples, indicating formation of substantial trap states. The observed reaction chemistry, which here occurs with low photon to chemical conversion efficiency, suggests that ligand reactivity may require examination for improved NC dispersion stability but can also be manipulated to yield desired photocatalytically accessed chemical species.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Verification of diesel spray ignition phenomenon in dual-fuel diesel-piloted premixed natural gas engine

Dual-fuel (DF) engines, in which premixed natural gas and air in an open-type combustion chamber is ignited by diesel-fuel pilot sprays, have been more popular for marine use than pre-chamber spark ignition (PCSI) engines because of their superior durability. However, control of ignition and combustion in DF engines is more difficult than in PCSI engines. In this context, here we focus on the ignition stability of n-heptane pilot-fuel jets injected into a compressed premixed charge of natural gas and air at low-load conditions. To aid understanding of the experimental data, chemical-kinetics simulations were carried out in a simplified engine-environment that provided insight into the chemical effects of methane (CH4) on pilot-fuel ignition. The simulations reveal that CH4 has an effect on both stages of n-heptane autoignition: the small, first-stage, cool-flame-type, low-temperature ignition (LTI) and the larger, second-stage, high-temperature ignition (HTI). As the ratio of pilot-fuel to CH4 entrained into the spray decreases, the initial oxidization of CH4 consumes the OH radicals produced by pilot-fuel decomposition during LTI, thereby inhibiting its progression to HTI. Using imaging diagnostics, the spatial and temporal progression of LTI and HTI in DF combustion are measured in a heavy-duty optical engine, and the imaging data are analyzed to understand the cause of severe fluctuations in ignition timing and combustion completeness at low-load conditions. Images of cool-flame and hydroxyl radical (OH*) chemiluminescence serve as indicators of LTI and HTI, respectively. The cycle-to-cycle and spatial variation in ignition extracted from the imaging data are used as key metrics of comparison. The imaging data indicate that the local concentration of the pilot-fuel and the richness of the surrounding natural-gas air mixture are important for LTI and HTI, but in different ways. In particular, higher injection pressures and shorter injection durations increase the mixing rate, leading to lower concentrations of pilot-fuel more quickly, which can inhibit HTI even as LTI remains relatively robust. Decreasing the injection pressure from 80 MPa to 40 MPa and increasing the injection duration from 500 µs to 760 µs maintained constant pilot-fuel mass, while promoting robust transition from LTI to HTI by effectively slowing the mixing rate. This allows enough residence time for the OH radicals, produced by the two-stage ignition chemistry of the pilot-fuel, to accelerate the transition from LTI to HTI before being consumed by CH4 oxidation. Thus from a practical perspective, for a premixed natural gas fuel–air equivalence-ratio, it is possible to improve the “stability” of the combustion process by solely manipulating the pilot-fuel injection parameters while maintaining constant mass of injected pilot-fuel. This allows for tailoring mixing trajectories to offset changes in fuel ignition chemistry, so as to promote a robust transition from LTI to HTI by changing the balance between the local concentration of the pilot-fuel and richness of the premixed natural gas and air. This could prove to be a valuable tool for combustion design to improve fuel efficiency or reduce noise or perhaps even reduce heat-transfer losses by locating early combustion away from in-cylinder walls.

42 ENGINEERING↗

DOE OSTI2023

Adiabatically controlled motional states of a CaO + and Ca + trapped-ion chain cooled to the ground state

Control of the external degree of freedom of trapped molecular ions is essential for their promising applications to spectroscopy, precision measurements of fundamental constants, and quantum information technology. Here, in this study, we demonstrate near ground-state cooling of the axial motional modes of a calcium mono-oxide ion via sympathetic sideband cooling with a cotrapped calcium ion. We also show that the phonon state of the axial out-of-phase mode of the ion chain is maintained while the mode frequency is adiabatically ramped up and/or down. The adiabatic ramping of the motional mode frequency is a prerequisite for searching for the proposed molecular dipole-phonon interaction.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

Measurement of flow properties coupled to experimental and numerical analyses of dense, granular flows for solar thermal energy storage

Granular flows of sintered bauxite proppants were researched along an inclined plane for solar thermal energy storage applications. Granular flow properties needed to drive numeric granular models were measured for improved numerical model predictions for Carbobead CP 50/140, 40/100, and 30/60 particles. Particle shape and size distributions were determined by coupling optical microscopy to an in-house image processing algorithm. The impulse excitation technique was used to measure elastic and shear moduli, and compute Poisson’s ratio. The coefficient of static sliding friction was measured using the slip-stick method, and the static rolling friction was determined from measured shear on particles positioned between two hot-pressed plates. The coefficient of restitution was measured by dropping particles on a surface and determining the kinetic energy before and after impact with the surface using high resolution particle tracking velocimetry. Particle size did not significantly impact the coefficients of restitution and static rolling friction, however, particle shape distribution resulted in a large variation in measurements. An inclined flow experiment was performed to characterize granular flows of Carbobead CP 30/60 particles using particle image velocimetry. Numerical models of the experiment using discrete element method were generated with the measured mechanical properties as inputs for comparison with experimental results. A constant directional torque rolling friction model best predicted bulk granular flow behavior. Furthermore, good agreement between the model and experiment was achieved at ambient, steady state conditions, with average velocity differences <10%.

14 SOLAR ENERGY↗

DOE OSTI2020

Rapid evolution of aerosol particles and their optical properties downwind of wildfires in the western US

Abstract. During the first phase of the Biomass Burn Operational Project (BBOP) field campaign, conducted in the Pacific Northwest, the DOE G-1 aircraft was used to follow the time evolution of wildfire smoke from near the point of emission to locations 2–3.5 h downwind. In nine flights we made repeated transects of wildfire plumes at varying downwind distances and could thereby follow the plume's time evolution. On average there was little change in dilution-normalized aerosol mass concentration as a function of downwind distance. This consistency hides a dynamic system in which primary aerosol particles are evaporating and secondary ones condensing. Organic aerosol is oxidized as a result. On all transects more than 90 % of aerosol is organic. In freshly emitted smoke aerosol, NH4+ is approximately equivalent to NO3. After 2 h of daytime aging, NH4+ increased and is approximately equivalent to the sum of Cl, SO42, and NO3. Particle size increased with downwind distance, causing particles to be more efficient scatters. Averaged over nine flights, mass scattering efficiency (MSE) increased in ∼ 2 h by 56 % and doubled in one flight. Mechanisms for redistributing mass from small to large particles are discussed. Coagulation is effective at moving aerosol from the Aitken to accumulation modes but yields only a minor increase in MSE. As absorption remained nearly constant with age, the time evolution of single scatter albedo was controlled by age-dependent scattering. Near-fire aerosol had a single scatter albedo (SSA) of 0.8–0.9. After 1 to 2 h of aging SSAs were typically 0.9 and greater. Assuming global-average surface and atmospheric conditions, the observed age dependence in SSA would change the direct radiative effect of a wildfire plume from near zero near the fire to a cooling effect downwind.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Quantitative 2D thermometry in turbulent sooting non-premixed flames using filtered Rayleigh scattering

This paper demonstrates the application of a thermometry method in turbulent sooting non-premixed flames using filtered Rayleigh scattering (FRS). Fuel tailoring is used to establish a specific C 2 H 2 -based fuel mixture such that temperature can be determined accurately by a single FRS measurement over the entirety of mixture fraction space, or equivalently, for all relevant thermo-chemical states. Evaluation is performed in a hierarchy of flows to establish measurement precision and accuracy. Initial assessments in a series of heated fuel mixtures; non-sooting, near-adiabatic flat flames; and laminar non-premixed sooting flames show accuracy of the approach over a full range of expected temperatures and high single-shot measurement precision (e.g., 65 < <#comment/> S N R < <#comment/> 80 ) for temperatures between 1900 and 2200 K. Subsequently, 2D temperature measurements are evaluated in a turbulent non-premixed sooting flame. For the current fuel mixture, the local mixture-averaged Rayleigh scattering cross section is nearly constant over all composition space, and thus traditional laser Rayleigh scattering (LRS) is used as a measurement standard in the absence of soot. The results show excellent agreement between the proposed FRS thermometry approach and LRS in non-sooting regions. In the presence of soot, the proposed FRS-based approach shows no signs of interference. In addition, 2D temperature imaging shows high SNR (60–74) over all temperature conditions. Thus, we believe the proposed methodology successfully provides a high-resolution 2D temperature method under turbulent sooting flame conditions.

Pu, Jinpeng↗

DOE OSTI2020

Measurements of a 2.1 MeV H− beam with an Allison scanner

Transverse 2D phase space distributions of a 2.1 MeV, 5 mA H− beam are measured at the Proton Improvement Plan II Injector Test accelerator at Fermilab with an Allison scanner. This paper describes the design, calibration, and performance of the scanner along with the main results from beam measurements. Analyses of the recorded phase portraits are performed primarily in action-phase coordinates. The stability of the action under linear optics makes it easier to compare measurements taken under different beamline conditions. The amplitude of a single measured point (“pixel”) is proportional to the phase density in the corresponding portion of the beam. When the Twiss parameters are calculated using only the high-phase density part of the beam, the pixel amplitude in the beam core is found to be decreasing approximately exponentially with action and to be phase-independent. Outside of the core, the amplitudes decrease with action at a slower rate than in the core. This “tail” comprises 10%–30% of the beam, with 0.1% of the total measured intensity extending beyond action 10–20 times larger than the rms emittance. The transition from the core to the tail is accompanied by the appearance of two “branches” that are separated in phase and extend beyond the core. A set of selected measurements shows that there is no measurable emittance dilution along the beamline; the beam parameters are practically constant over a 0.5 ms pulse; and scraping in various parts of the beamline is an effective way to decrease the transverse tails by removing the branches.

Richard, C. (ORCID:000000029891135X)↗