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At least 289 records · Page 16

Methane dissociation on Pt(111): Searching for a specific reaction parameter density functional

The theoretical description of methane dissociating on metal surfaces is a current frontier in the field of gas-surface dynamics. Dynamical models that aim at achieving a highly accurate description of this reaction rely on potential energy surfaces based on density functional theory calculations at the generalized gradient approximation. We focus here on the effect that the exchange-correlation functional has on the reactivity of methane on a metal surface, using CHD{sub 3} + Pt(111) as a test case. We present new ab initio molecular dynamics calculations performed with various density functionals, looking also at functionals that account for the van der Waals (vdW) interaction. While searching for a semi-empirical specific reaction parameter density functional for this system, we find that the use of a weighted average of the PBE and the RPBE exchange functionals together with a vdW-corrected correlation functional leads to an improved agreement with quantum state-resolved experimental data for the sticking probability, compared to previous PBE calculations. With this semi-empirical density functional, we have also investigated the surface temperature dependence of the methane dissociation reaction and the influence of the rotational alignment on the reactivity, and compared our results with experiments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Theoretical Study of Structural, Magnetic, Elastic, Phonon, and Thermodynamic Properties of Heusler Alloys Fe{sub 2}CrX (X = Al, Ga)

First-principle calculations based on generalized gradient approximation and quasi-harmonic Debye model were executed to analyze the structural, magnetic, elastic, phonon, and thermodynamic properties of Fe{sub 2}CrX (X = Al, Ga) Heusler alloys. The computed lattice parameters concurred well with available experimental and theoretical data. The calculated elastic constants reveal that the Fe{sub 2}CrAl is brittle and Fe{sub 2}CrGa is ductile. The phonon dispersion relation of Fe{sub 2}CrX (X = Al, Ga) are calculated using finite displacement method with a cutoff radius of 5 Å. We likewise explored the thermodynamic properties by utilizing quasi-harmonic Debye model in which bulk modulus, heat capacity, Debye temperature, Grüneisen parameter, and thermal expansion coefficient are resolved at 0–30 Gpa pressure and 0–900 K temperature from the non-equilibrium Gibbs functions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Vertical gradients in the theory of radio aurora.

Study of vertical density gradients as a potential source of irregularities responsible for radio aurorae and as a possible cause that might modify the aspect sensitivity of radio-auroral reflections coming from two-stream instability irregularities. Both of these effects are examined in a single calculation which incorporates vertical gradients into the two-stream instability theory of Farley (1963).

Moorcroft, D. R.↗

Scale setting the Möbius domain wall fermion on gradient-flowed HISQ action using the omega baryon mass and the gradient-flow scales 𝑡 0 and 𝑤 0

We report on a subpercent scale determination using the omega baryon mass and gradient-flow methods. The calculations are performed on 22 ensembles of 𝑁 𝑓 =2 +1 +1 highly improved, rooted staggered sea-quark configurations generated by the MILC and CalLat Collaborations. The valence quark action used is Möbius domain wall fermions solved on these configurations after a gradient-flow smearing is applied with a flowtime of 𝑡 gf = 1 in lattice units. The ensembles span four lattice spacings in the range 0.06 ≲ 𝑎 ≲0.15 fm, six pion masses in the range 130 ≲ 𝑚 𝜋 ≲ 400 MeV and multiple lattice volumes. On each ensemble, the gradient-flow scales 𝑡 0 /𝑎 2 and 𝑤 0 /𝑎 and the omega baryon mass 𝑎⁢𝑚 Ω are computed. The dimensionless product of these quantities is then extrapolated to the continuum and infinite volume limits and interpolated to the physical light, strange and charm quark mass point in the isospin limit, resulting in the determination of $\sqrt{t}_0$ = 0.1422⁢(14) fm and 𝑤 0 = 0.1709⁢(11) fm with all sources of statistical and systematic uncertainty accounted for. The dominant uncertainty in both results is the stochastic uncertainty, though for $\sqrt{t}_0$ there are comparable continuum extrapolation uncertainties. For 𝑤 0 , there is a clear path for a few-per-mille uncertainty just through improved stochastic precision, as recently obtained by the Budapest-Marseille-Wuppertal Collaboration.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Parameterization of photon beam dosimetry for a linear accelerator

Purpose: In radiation therapy, accurate data acquisition of photon beam dosimetric quantities is important for (1) beam modeling data input into a treatment planning system (TPS), (2) comparing measured and TPS modeled data, (3) the quality assurance process of a linear accelerator’s (Linac) beam characteristics, (4) the establishment of a standard data set for comparison with other data, etcetera. Parameterization of the photon beam dosimetry creates a data set that is portable and easy to implement for different applications such as those previously mentioned. The aim of this study is to develop methods to parameterize photon beam dosimetric quantities, including percentage depth doses (PDDs), profiles, and total scatter output factors (S{sub cp}). Methods: S{sub cp}, PDDs, and profiles for different field sizes, depths, and energies were measured for a Linac using a cylindrical 3D water scanning system. All data were smoothed for the analysis and profile data were also centered, symmetrized, and geometrically scaled. The S{sub cp} data were analyzed using an exponential function. The inverse square factor was removed from the PDD data before modeling and the data were subsequently analyzed using exponential functions. For profile modeling, one halfside of the profile was divided into three regions described by exponential, sigmoid, and Gaussian equations. All of the analytical functions are field size, energy, depth, and, in the case of profiles, scan direction specific. The model’s parameters were determined using the minimal amount of measured data necessary. The model’s accuracy was evaluated via the calculation of absolute differences between the measured (processed) and calculated data in low gradient regions and distance-to-agreement analysis in high gradient regions. Finally, the results of dosimetric quantities obtained by the fitted models for a different machine were also assessed. Results: All of the differences in the PDDs’ buildup and the profiles’ penumbra regions were less than 2 and 0.5 mm, respectively. The differences in the low gradient regions were 0.20% ± 0.20% (<1% for all) and 0.50% ± 0.35% (<1% for all) for PDDs and profiles, respectively. For S{sub cp} data, all of the absolute differences were less than 0.5%. Conclusions: This novel analytical model with minimum measurement requirements was proved to accurately calculate PDDs, profiles, and S{sub cp} for different field sizes, depths, and energies.

61 RADIATION PROTECTION AND DOSIMETRY↗

Impact of Hydration and Sulfonation on the Morphology and Ionic Conductivity of Sulfonated Poly(phenylene) Proton Exchange Membranes

Multiple computational and experimental techniques are used here to understand the nanoscale morphology and water/proton transport properties in a series of sulfonated Diels–Alder poly(phenylene) (SDAPP) membranes over a wide range of temperature, hydration, and sulfonation conditions. New synthetic methods allow us to sulfonate the SDAPP membranes to much higher ion exchange capacity levels than has been previously possible. Nanoscale phase separation between the hydrophobic polymer backbone and the hydrophilic water/sulfonic acid groups was observed for all membranes studied. We find good agreement between structure factors calculated from atomistic molecular dynamics (MD) simulations and those measured by X-ray scattering. With increasing hydration, the scattering ionomer peak in SDAPP is found to decrease in intensity. This intensity decrease is shown to be due to a reduction of scattering contrast between the water and polymer and is not indicative of any loss of nanoscale phase separation. Both MD simulations and density functional theory (DFT) calculations show that as hydration levels are increased, the nanostructure morphology in SDAPP evolves from isolated ionic domains to fully percolated water networks containing progressively weaker hydrogen bond strengths. The conductivity of the membranes is measured by electrical impedance spectroscopy and the equivalent proton conductivity calculated from pulsed-field-gradient (PFG) NMR diffusometry measurements of the hydration waters. Comparison of the measured and calculated conductivity reveals that in SDAPP the proton conduction mechanism evolves from being dominated by vehicular transport at low hydration and sulfonation levels to including a significant contribution from the Grötthuss mechanism (also known as structural diffusion) at higher hydration and sulfonation levels. The observed increase in conductivity reflects the impact that changing hydration and sulfonation have on the morphology and hydrogen bond network and ultimately on the membrane performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Thermodynamic evaluation of transonic compressor rotors using the finite volume approach

Research at NASA Lewis Research Center gave the opportunity to incorporate new control volumes in the Denton 3-D finite-volume time marching code. For duct flows, the new control volumes require no transverse smoothing and this allows calculations with large transverse gradients in properties without significant numerical total pressure losses. Possibilities for improving the Denton code to obtain better distributions of properties through shocks were demonstrated. Much better total pressure distributions through shocks are obtained when the interpolated effective pressure, needed to stabilize the solution procedure, is used to calculate the total pressure. This simple change largely eliminates the undershoot in total pressure down-stream of a shock. Overshoots and undershoots in total pressure can then be further reduced by a factor of 10 by adopting the effective density method, rather than the effective pressure method. Use of a Mach number dependent interpolation scheme for pressure then removes the overshoot in static pressure downstream of a shock. The stability of interpolation schemes used for the calculation of effective density is analyzed and a Mach number dependent scheme is developed, combining the advantages of the correct perfect gas equation for subsonic flow with the stability of 2-point and 3-point interpolation schemes for supersonic flow.

Moore, J.↗

Flow through the tile gaps in the Space Shuttle Thermal Protection System

The problem of predicting aerodynamic loads on the insulating tiles of the Space Shuttle Thermal Protection System (TPS) is discussed and seen to require a method for predicting pressure and mass flux in the gaps between tiles. A mathematical model of the tile-gap flow is developed based upon a slow viscous (Stokes) flow analysis and is verified against available experimental data. This model derives the tile-gap pressure field from a solution of the two-dimensional Laplace equation; the mass flux vector is then calculated from the pressure gradient. The means for incorporating this model into a lumped-parameter network analogy for porous-media flow is also given. The flow model shows tile-gap mass flux to be very sensitive to the gap width indicating a need for coupling the TPS flow and tile displacement calculations. Finally recommendations are made concerning additional analytical and experimental work to improve TPS flow predictions.

Dwoyer, D. L.↗

Integrating deep neural networks with full-waveform inversion: Reparameterization, regularization, and uncertainty quantification

Full-waveform inversion (FWI) is an accurate imaging approach for modeling the velocity structure by minimizing the misfit between recorded and predicted seismic waveforms. However, the strong nonlinearity of FWI resulting from fitting oscillatory waveforms can trap the optimization in local minima. We have adopted a neural-network-based full-waveform inversion (NNFWI) method that integrates deep neural networks with FWI by representing the velocity model with a generative neural network. Neural networks can naturally introduce spatial correlations as regularization to the generated velocity model, which suppresses noise in the gradients and mitigates local minima. Furthermore, the velocity model generated by neural networks is input to the same partial differential equation (PDE) solvers used in conventional FWI. The gradients of the neural networks and PDEs are calculated using automatic differentiation, which back propagates gradients through the acoustic PDEs and neural network layers to update the weights of the generative neural network. Experiments on 1D velocity models, the Marmousi model, and the 2004 BP model determine that NNFWI can mitigate local minima, especially for imaging high-contrast features such as salt bodies, and it significantly improves the inversion in the presence of noise. Adding dropout layers to the neural network model also allows analyzing the uncertainty of the inversion results through Monte Carlo dropout. NNFWI opens a new pathway to combine deep learning and FWI for exploiting the characteristics of deep neural networks and the high accuracy of PDE solvers. Because NNFWI does not require extra training data and optimization loops, it provides an attractive and straightforward alternative to conventional FWI.

58 GEOSCIENCES↗

Effect of High-Gradient Magnetic Field on Electrical Property of Carbon Nanotube-Polypyrrole Composite; Nanotube Separation Mechanism

High- and low-gradient magnetic fields are produced by resistor-inductor-capacitor (RLC) discharge apparatuses. The maximum magnetic field is 12.5 Tesla with 1-ms pulse duration. Multiwall carbon nanotube–polypyrrole composite is prepared. The samples are exposed to high- and low-gradient magnetic fields. To understand the behavior of carbon nanotubes (CNTs) in high-gradient magnetic fields (HGMFs), we theoretically calculated the equivalent magnetic susceptibility of a CNT in the gradient magnetic field. We found that the gradient force which is exerted on a CNT could be repellent or absorbent depending on the parallel and perpendicular susceptibilities of the CNT, as well as on the initial orientation of the CNT with respect to magnetic field direction. Four-probe studies show that the electrical conductivity of CNT composites decreases after exposure to a high-gradient magnetic field. Microscopic observation of the electrical current profile of composites reveals rearrangement of CNTs under HGMF.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

A title-gap flow model for use in aerodynamic loads assessment of space shuttle thermal protection system: Parallel gap faces

The problem of predicting aerodynamic loads on the insulating tiles of the space shuttle thermal protection system (TPS) is discussed and seen to require a method for predicting pressure and mass flux in the gaps between tiles. A mathematical model of the tile-gap flow is developed, based upon a slow viscous (Stokes) flow analysis, and is verified against experimental data. The tile-gap pressure field is derived from a solution of the two-dimensional Laplace equation; the mass-flux vector is then calculated from the pressure gradient. The means for incorporating this model into a lumped-parameter network analogy for porous-media flow is given. The means for incorporating this model into a lumped-parameter network analogy for porous-media flow is given. The flow model shows tile-gap mass flux to be very sensitive to the gap width indicating a need for coupling the TPS flow and tile displacement calculation. Analytical and experimental work to improve TPS flow predictions and a possible shuttle TPS hardware modification are recommended.

Dwoyer, D. L.↗

Geothermal Play-Fairway Analysis of Washington State Prospects: Final Report

The Washington State Geothermal Play-Fairway Analysis overcomes the exploration challenges posed by dense vegetation, glacial deposits, and extreme precipitation. The geothermal play-fairways we target are locations where heat, permeability, and saturated porosity are present in sufficient volume to provide adequate heat exchange at depths accessible by modern drilling technology. The three study areas lie along the Cascade Range magmatic arc and are near Mount Baker, Mount St. Helens, and the Wind River Valley. The seven-year project is divided into three phases. In Phase 1 we build on a previous statewide assessment of geothermal resources and develop an initial modeling approach. The results are a series of favorability, uncertainty, and risk maps for three targeted study areas. Based on these initial results, we collect new geologic and geophysical data to further refine our modeling and reduce exploration uncertainty in Phase 2. We improve the modeling method to handle the new data and update the favorability, uncertainty, and risk maps. We also update the conceptual geothermal resource models. In Phase 3 we validate our modeling approach by drilling two temperature-gradient holes and collecting and analyzing core, image logs, and new geochemistry. Our modeling approach improves on an earlier statewide method through a more-rigorous and detailed assessment of heat and permeability. Permeability potential is assessed through geomechanical modeling of the deformation that can generate and maintain reservoir porosity and permeability. Metrics to inform heat potential include temperature-gradient wells, which are sparse in Washington; proximity of Quaternary volcanic vents and young intrusive rock; spring temperature; and reservoir temperature inferred from geothermometry. We weight the individual components using an expert-guided approach known as the Analytical Hierarchy Process. During Phase 2 we also develop a fluid-filled fracture model, and an infrastructure model that helps to delineate areas which are more favorable for geothermal development based on proximity to transmission lines, elevation, land ownership and use restrictions, and availability of process water. New geologic and geophysical data is collected during Phase 2 in each of our three main study areas. At Mount Baker and north of Mount St. Helens we conduct 1:24,000-scale geologic mapping and lidar analysis to better constrain the location and character of surface faults; detailed mapping in the Wind River Valley was completed just prior to the start of this project. Ages of intrusive rocks are determined with 40 Ar/ 39 Ar geochronology, though all of our samples are Miocene or older. We collect ground based gravity observations (a total of 1,580 new stations) in all of our study areas and ground-based magnetic lines (a total of 93 km) at Mount Baker. These data are combined with existing gravity and aeromagnetic data and used to constrain fault locations and geometry. Two to three cross sections are constructed at each study area using the mapped surface geology and forward-modeling of the gravity and magnetic data; these cross sections form the basis for our updated conceptual models. We collect magnetotelluric surveys at Mount Baker and Mount St. Helens and these data are inverted to form a resistivity model from the surface to about 10 km depth; each model shows conductive zones that can be interpreted as upwelling geothermal fluids. At Mount St. Helens we deploy a passive seismic array and use the newly detected events to refine the location of the Saint Helens seismic zone. We also employ ambient-noise tomography to develop a detailed seismic-velocity model for the study area and use this model to help constrain our cross sections and conceptual model. Based on the new data collected during Phase 2—and our updated models—we develop a campaign of temperature-gradient holes and core analysis to validate our modeling in Phase 3. Drill hole MB76-31 is located near Little Park Creek, 11 km west-southwest of the summit of Mount Baker, and is 1,471 ft deep. About 410 ft of core from the lower portion of the hole—and image logs from ~175 ft below ground surface to the bottom—are collected and analyzed. Water samples are collected and processed for geothermometry. Drill hole MSH17-24 is located along upper Schultz Creek, 16 km north-northeast of Mount St. Helens and has core from 470 ft to the bottom at 1,053 ft. We did not collect image logs due to borehole stability concerns, but water samples are collected and analyzed for geothermometry. Repeat temperature-gradient measurements are made at both sites and thermal conductivity is measured from core samples. At MB76-31, the equilibrated temperature gradient of 64°C/km and calculated heat flow of 141–159 mW/m 2 is more than twice the regional average. Detailed mapping and analysis of the core, coupled with correlation to the image logs, indicates a history of permeability generation consistent with our predictions of high permeability. Because the site has high favorability in the Phase 2 model, we consider the results a positive validation of the modeling. At site MSH17-24, the equilibrated temperature gradient of ~15°C/km and calculated heat flow of 41–43 mW/m 2 are similar to regional. Geochemical analysis of the water samples indicates a meteoric source without any geothermal component. Detailed outcrop-based mapping of fault exposures near the drill site and analysis of image logs from nearby boreholes indicates a history of permeability generation consistent with our predictions. Because the site has low favorability in the Phase 2 model, we consider the results a positive validation of the modeling. Together, the two sites provide a reasonably positive validation of the Phase 2 modeling and should encourage future use of this modeling approach.

15 GEOTHERMAL ENERGY↗

Airship stresses due to vertical velocity gradients and atmospheric turbulence

Munk's potential flow method is used to calculate the resultant moment experienced by an ellipsoidal airship. This method is first used to calculate the moment arising from basic maneuvers considered by early designers, and then expended to calculate the moment arising from vertical velocity gradients and atmospheric turbulence. This resultant moment must be neutralized by the transverse force of the fins. The results show that vertical velocity gradients at a height of 6000 feet in thunderstorms produce a resultant moment approximately three to four times greater than the moment produced in still air by realistic values of pitch angle or steady turning. Realistic values of atmospheric turbulence produce a moment which is significantly less than the moment produced by maneuvers in still air.

Sheldon, D.↗

Alpha channeling with high-field launch of lower hybrid waves

Although lower hybrid waves are effective at driving currents in present-day tokamaks, they are expected to interact strongly with high-energy particles in extrapolating to reactors. In the presence of a radial alpha particle birth gradient, this interaction can take the form of wave amplification rather than damping. While it is known that this amplification more easily occurs when launching from the tokamak high-field side, the extent of this amplification has not been made quantitative. Here, by tracing rays launched from the high-field-side of a tokamak, the required radial gradients to achieve amplification are calculated for a temperature and density regime consistent with a hot-ion-mode fusion reactor. These simulations, while valid only in the linear regime of wave amplification, nonetheless illustrate the possibilities for wave amplification using high-field launch of the lower hybrid wave.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Scaling of thermal stratification in outlet plena of SFRs with gallium as a surrogate fluid

Due to its high thermal diffusivity, liquid sodium can develop thermally stratified regions in the hot and cold pools of SFRs under certain off normal operating conditions. The temperature gradients in the fluid give rise to mixed convection flow in which flow velocities result both from pressure gradients and from volume forces induced by density gradients. High thermal diffusivity and low momentum diffusivity leads to reduced thermal mixing and enhanced stratification. Thermal stratification, if not looked carefully in the design, can lead to severe consequences in normal operation with forced coolant circulation and during off-normal natural circulation. The resulting hydraulic and thermal loads can cause the failure modes in structures and components critical for reactor safety. Thermal stratification in the SFR pools can lead to thermal fatigue, which can lead to structural and material failure, or pose serious concerns for the reactor safety. In addition to thermo-structural issues, the reactivity changes are significantly impacted due to density or temperature driven movement of liquid sodium. Temperature changes or gradients in the Upper Instrumentation Structures (UIS) of SFRs can lead to thermal contraction, a case that can lead to positive reactivity insertion after core shut-down. The motivation of this work is to design a scaled down experimental facility which can generate high fidelity data for thermal stratification physics to validate 3-dimensional (3D) Computational Fluid Dynamics (CFD) models. These validated CFD codes can be used to improve the 1-dimensional (1D) system level codes such as SAS4A/SASSYS-1 which are currently not capable of simulating thermal stratification accurately. These improvements in 1D system level SAS4A/SASSYS-1 codes can significantly improve the safety analyses and design of SFRs. The GaTE facility outlet plenum model is designed based on physics based similarities. Thermal stratification physics is governed primarily by the Richardson numbers (Ri). The expected low flow rates during off-normal conditions can lead to a high degree of thermal stratification in the outlet plenum with a corresponding Ri = 530. Therefore, the inlet flow velocities and inlet hydraulic diameter for the gallium coolant entering the test vessel are required to achieve same Ri. The design of test vessel in GaTE facility is finalized to a 1/20. scale outlet plenum height of the ABTR. This design of the test facility will allow the decoupling of the thermal stratification physics at low flow rates with the transient natural circulation. In other words, it will enable effective control to study thermal stratification at very low flow rates. Numerical studies are conducted with a 3D CFD code to examine the thermal behavior of the selected test design. Simulation results show that thermal gradients are present only in the vertical or axial direction which are similar to the behavior reported in previous studies on full scale SFR models. Future work will involve the experimental studies using the GaTE facility with the high fidelity instrumentation.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Radiative cooling of a hydrogen plasma in a shock tube

A method of computing radiative cooling of a hydrogen plasma assuming quasi-isothermal radiative transfer is described. A comparison with nonisothermal calculations for a plane parallel slab indicates good agreement for temperature gradients up to 300 K/cm. The calculations are compared with shock-tube data obtained in the JPL high-performance shock-tube facility. The calculations agreed with the data for one run but were 20 percent high for the other. Due to greater radiative cooling at the test slug boundaries a lateral temperature variation typically exists. This would cause the intensity measurement, which is integrated across the diameter of the test slug, to be below the prediction.

Stickford, G. H., Jr.↗

Gradient-Informed Design Optimization of Select Nuclear Systems

In this work, we present a gradient-informed design optimization of nuclear reactor core components based on neutronics objectives with both continuous and discrete materials. The main argument in favor of using gradient-informed design optimization is that it scales well with increasing dimensionality of the design space. First, a challenge problem with 121 free parameters is solved with a gradient-informed method and then with a genetic algorithm. Then, a challenge problem to optimize the flux profile of a simplified assembly with eight axial zones is solved. Both challenge problems are solved using directly calculated derivatives from Tools for Sensitivity and Uncertainty Analysis Methodology Implementation (TSUNAMI) in the SCALE package. Furthermore, we demonstrate how a discrete optimization problem—selection of materials for 121 voxels—can be lifted into a continuous problem with mixed materials. In the continuous space, adjoint-based gradients are well-defined, and gradient descent is applicable. Then, a forcing function is introduced that with the selection of an appropriately sized hyperparameter can be used to guide the optimized continuous solution back into a discrete solution. This paper presents an account of the challenges that were faced when applying a gradient-informed optimization algorithm using a Monte Carlo calculation to estimate the gradient information and compares a gradient descent optimization method to a genetic algorithm optimization of the same geometry. Overall, this work demonstrates the potential use of adjoint-based gradient calculations in design optimization of nuclear systems.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Radiative Characteristics of Clouds Embedded in Smoke Derived from Airborne Multiangular Measurements

Clouds in the presence of absorbing aerosols result in their apparent darkening, observed at the top of atmosphere (TOA), which is associated with the radiative effects of aerosol absorption. Owing to the large radiative effect and potential impacts on regional climate, above-cloud aerosols have recently been characterized in multiple satellite-based studies. While satellite data are particularly useful in showing the radiative impact of above-cloud aerosols at the TOA, recent literature indicates large uncertainties in satellite retrievals of above-cloud aerosol optical depth (AOD) and single scattering albedo (SSA), which are among the most important parameters in the assessment of associated radiative effects. In this study, we analyze radiative characteristics of clouds in the presence of wildfire smoke using airborne data primarily from NASA's Cloud Absorption Radiometer, collected during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites campaign in Canada during the 2008 summer season. We found a strong positive reflectance (R) gradient in the UV-visible (VIS)-near infrared (NIR) spectrum for clouds embedded in dense smoke, as opposed to an (expected) negative gradient for cloud-free smoke and a flat spectrum for smoke-free cloud cover. Several cases of clouds embedded in thick smoke were found, when the aircraft made circular/spiral measurements, which not only allowed the complete characterization of angular distribution of smoke scattering but also provided the vertical distribution of smoke and clouds (within 0.5-5 km). Specifically, the largest darkening by smoke was found in the UV/VIS, with R(sub 0.34 microns) reducing to 0.2 (or 20%), in contrast to 0.8 at NIR wavelengths (e.g., 1.27 microns). The observed darkening is associated with large AODs (0.5-3.0) and moderately low SSA (0.85-0.93 at 0.53 microns), resulting in a significantly large instantaneous aerosol forcing efficiency of 254 +/- 47 W/sq m/τ. Our observations of smoke-cloud radiative interactions were found to be physically consistent with theoretical plane-parallel 1-D and Monte Carlo 3-D radiative transfer calculations, capturing the observed gradient across UV-VIS-NIR. Results from this study offer insights into aerosol-cloud radiative interactions and may help in better constraining satellite retrieval algorithms.

absorbing aerosols↗