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DOE OSTI2014

Development and Benchmarking of a Hybrid PIC Code For Dense Plasmas and Fast Ignition (Final Report)

Radiation processes play an important role in the study of both fast ignition and other inertial confinement schemes, such as plasma jet driven magneto-inertial fusion, both in their effect on energy balance, and in generating diagnostic signals. In the latter case, warm and hot dense matter may be produced by the convergence of a plasma shell formed by the merging of an assembly of high Mach number plasma jets. This innovative approach has the potential advantage of creating matter of high energy densities in voluminous amount compared with high power lasers or particle beams. An important application of this technology is as a plasma liner for the flux compression of magnetized plasma to create ultra-high magnetic fields and burning plasmas. HyperV Technologies Corp. has been developing plasma jet accelerator technology in both coaxial and linear railgun geometries to produce plasma jets of sufficient mass, density, and velocity to create such imploding plasma liners. An enabling tool for the development of this technology is the ability to model the plasma dynamics, not only in the accelerators themselves, but also in the resulting magnetized target plasma and within the merging/interacting plasma jets during transport to the target. Welch pioneered numerical modeling of such plasmas (including for fast ignition) using the LSP simulation code. Lsp is an electromagnetic, parallelized, plasma simulation code under development since 1995. It has a number of innovative features making it uniquely suitable for modeling high energy density plasmas including a hybrid fluid model for electrons that allows electrons in dense plasmas to be modeled with a kinetic or fluid treatment as appropriate. In addition to in-house use at Voss Scientific, several groups carrying out research in Fast Ignition (LLNL, SNL, UCSD, AWE (UK), and Imperial College (UK)) also use LSP. A collaborative team consisting of HyperV Technologies Corp., Voss Scientific LLC, FAR-TECH, Inc., Prism Computational Sciences, Inc. and Advanced Energy Systems Inc. joined efforts to develop new physics and numerical models for LSP in several key areas to enhance the ability of LSP to model high energy density plasmas (HEDP). This final report details those efforts. Areas addressed in this research effort include: adding radiation transport to LSP, first in 2D and then fully 3D, extending the EMHD model to 3D, implementing more advanced radiation and electrode plasma boundary conditions, and installing more efficient implicit numerical algorithms to speed complex 2-D and 3-D computations. The new capabilities allow modeling of the dominant processes in high energy density plasmas, and further assist the development and optimization of plasma jet accelerators, with particular attention to MHD instabilities and plasma/wall interaction (based on physical models for ion drag friction and ablation/erosion of the electrodes). In the first funding cycle we implemented a solver for the radiation diffusion equation. To solve this equation in 2-D, we used finite-differencing and applied the parallelized sparse-matrix solvers in the PETSc library (Argonne National Laboratory) to the resulting system of equations. A database of the necessary coefficients for materials of interest was assembled using the PROPACEOS and ATBASE codes from Prism. The model was benchmarked against Prism's 1-D radiation hydrodynamics code HELIOS, and against experimental data obtained from HyperV's separately funded plasma jet accelerator development program. Work in the second funding cycle focused on extending the radiation diffusion model to full 3-D, continued development of the EMHD model, optimizing the direct-implicit model to speed up calculations, add in multiply ionized atoms, and improved the way boundary conditions are handled in LSP. These new LSP capabilities were then used, along with analytic calculations and Mach2 runs, to investigate plasma jet merging, plasma detachment and transport, restrike and advanced jet accelerator design. In addition, a strong linkage to diagnostic measurements was made by modeling plasma jet experiments on PLX to support benchmarking of the code. A large number of upgrades and improvements advancing hybrid PIC algorithms were implemented in LSP during the second funding cycle. These include development of fully 3D radiation transport algorithms, new boundary conditions for plasma-electrode interactions, and a charge conserving equation of state that permits multiply ionized high-Z ions. The final funding cycle focused on 1) mitigating the effects of a slow-growing grid instability which is most pronounced in plasma jet frame expansion problems using the two-fluid Eulerian remap algorithm, 2) extension of the Eulerian Smoothing Algorithm to allow EOS/Radiation modeling, 3) simulations of collisionless shocks formed by jet merging, 4) simulations of merging jets using high-Z gases, 5) generation of PROPACEOS EOS/Opacity databases, 6) simulations of plasma jet transport experiments, 7) simulations of plasma jet penetration through transverse magnetic fields, and 8) GPU PIC code development. The tools developed during this project are applicable not only to the study of plasma jets, but also to a wide variety of HEDP plasmas of interest to DOE, including plasmas created in short-pulse laser experiments performed to study fast ignition concepts for inertial confinement fusion.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2012

UNBURNED MATERIAL IN THE EJECTA OF TYPE Ia SUPERNOVAE

The presence of unburned material in the ejecta of normal Type Ia supernovae (SNe Ia) is investigated using early-time spectroscopy obtained by the Carnegie Supernova Project. The tell-tale signature of pristine material from a C+O white dwarf progenitor star is the presence of carbon, as oxygen is also a product of carbon burning. The most prominent carbon lines in optical spectra of SNe Ia are expected to arise from C II. We find that at least 30% of the objects in the sample show an absorption at Almost-Equal-To 6300 A which is attributed to C II {lambda}6580. An alternative identification of this absorption as H{alpha} is considered to be unlikely. These findings imply a larger incidence of carbon in SNe Ia ejecta than previously noted. We show how observational biases and physical conditions may hide the presence of weak C II lines, and account for the scarcity of previous carbon detections in the literature. This relatively large frequency of carbon detections has crucial implications on our understanding of the explosive process. Furthermore, the identification of the 6300 A absorptions as carbon would imply that unburned material is present at very low expansion velocities, merely Almost-Equal-To 1000 km s{sup -1} above the bulk of Si II. Based on spectral modeling, it is found that the detections are consistent with a mass of carbon of 10{sup -3} to 10{sup -2} M{sub Sun }. The presence of this material so deep in the ejecta would imply substantial mixing, which may be related to asymmetries of the flame propagation. Another possible explanation for the carbon absorptions may be the existence of clumps of unburned material along the line of sight. However, the uniformity of the relation between C II and Si II velocities is not consistent with such small-scale asymmetries. The spectroscopic and photometric properties of SNe Ia with and without carbon signatures are compared. A trend toward bluer color and lower luminosity at maximum light is found for objects which show carbon.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2019

Strong ultralight foams based on nanocrystalline cellulose for high-performance insulation

Environmentally friendly, sustainable, and high-performance thermal insulators are in high demand. Petroleum based insulator foams usually have high thermal conductivity and pose health hazards. In this paper, we report ultralight composite foams that are highly strong, elastic, and super-insulating. The foams are composed of nanocrystalline cellulose (NCC) (74 wt%), polyvinyl alcohol (7.5 wt%), and a crosslinking agent (18.5 wt%). The fabrication process is simple and uses only water. The composite foams exhibit an elastic strain of ⁻13% at a modulus of 250 K Pa and a stress of 73 K Pa at 50% strain (100+ and 18 times, respectively, higher than those of pure NCC foam); both exceed the values of reported nanocellulose-based foams with no reinforcement. The foams exhibit a thermal conductivity of 0.027 Wm -1 K -1 , which is superior to those of traditional insulating materials. The structural integrity is also preserved after burning. Our results show that NCC-based materials can be engineered towards high-performance insulation applications.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Fire effects on the persistence of soil organic matter and long-term carbon storage

One paradigm in biogeochemistry is that frequent disturbance tends to deplete carbon (C) in soil organic matter (SOM) by reducing biomass inputs and promoting losses. However, disturbance by fire has challenged this paradigm because soil C responses to frequent and/or intense fires are highly variable, despite observed declines in biomass inputs. Here, we review recent advances to illustrate that fire-driven changes in decomposition, mediated by altered SOM stability, are an important compensatory process offsetting declines in aboveground biomass pools. Fire alters the stability of SOM by affecting both the physicochemical properties of the SOM and the environmental drivers of decomposition, potentially offsetting C lost via combustion, but the mechanisms affecting the SOM stability differ across ecosystems. Thus, shifting our focus from a top-down view of fire impacting C cycling via changes in plant biomass to a bottom-up view of changes in decomposition may help to elucidate counterintuitive trends in the response of SOM to burning. Finally, given that 70% of global topsoil C is in fire-prone regions, using fire to promote SOM stability may be an important nature-based climate solution to increase C storage.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

Design and Modeling of Vacuum Pumping for Steady-State Pellet Fueling Systems

We report that future long-pulse magnetic confinement fusion reactors will require density and isotopic mixture control using steady-state repeating pellet injectors. For high-energy density burning plasmas, pellet velocities of 1 km/s and above will be required for sufficient plasma penetration to achieve high fueling efficiency. Currently, steady-state repeating injection systems utilize cryogenic extruder systems to produce an extrusion of solid deuterium or deuterium-tritium. In repeating light gas gun injectors, the solid extrusion is cut and simultaneously loaded into a barrel. Once loaded, a fast operating gas valve delivers a high pressure burst of gas to accelerate the pellet down the barrel and into the machine. This process takes ~10 ms to achieve. Adequate gas pumping of the extruder exhaust and injection line propellant gas collection chambers is necessary for optimal operation of the pellet fueling system. Excess solid from the extruder sublimates in an exhaust chamber. The gas pressure in the extruder exhaust chamber must remain low to maintain low heating loads on the cooling mechanism (cryorefrigerators or liquid helium flow) and to reduce thermal conduction to the extrusion. Pumping the injection line chambers is necessary to limit propellant gas flow into the machine. A numerical simulation code was created to predict temporal pumping performance for these repeating pellet injection systems. Lastly, this paper outlines the methods and assumptions used to create this model and compares results to the pellet injection system currently employed on DIII-D, the steady-state pellet injection system planned for the Wendelstein 7-X, and a brief analysis of the ITER conceptual pellet fueling system.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Opportunistic experiments to constrain aerosol effective radiative forcing

Aerosol–cloud interactions (ACIs) are considered to be the most uncertain driver of present-day radiative forcing due to human activities. The nonlinearity of cloud-state changes to aerosol perturbations make it challenging to attribute causality in observed relationships of aerosol radiative forcing. Using correlations to infer causality can be challenging when meteorological variability also drives both aerosol and cloud changes independently. Natural and anthropogenic aerosol perturbations from well-defined sources provide “opportunistic experiments” (also known as natural experiments) to investigate ACI in cases where causality may be more confidently inferred. These perturbations cover a wide range of locations and spatiotemporal scales, including point sources such as volcanic eruptions or industrial sources, plumes from biomass burning or forest fires, and tracks from individual ships or shipping corridors. We review the different experimental conditions and conduct a synthesis of the available satellite datasets and field campaigns to place these opportunistic experiments on a common footing, facilitating new insights and a clearer understanding of key uncertainties in aerosol radiative forcing. Cloud albedo perturbations are strongly sensitive to background meteorological conditions. Strong liquid water path increases due to aerosol perturbations are largely ruled out by averaging across experiments. Opportunistic experiments have significantly improved process-level understanding of ACI, but it remains unclear how reliably the relationships found can be scaled to the global level, thus demonstrating a need for deeper investigation in order to improve assessments of aerosol radiative forcing and climate change.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1993

An Experimental and Theoretical Study of Radiative Extinction of Diffusion Flames

In a recent paper on 'Observations of candle flames under various atmospheres in microgravity' by Ross et al., it was found that for the same atmosphere, the burning rate per unit wick surface area and the flame temperature were considerably reduced in microgravity as compared with normal gravity. Also, the flame (spherical in microgravity) was much thicker and further removed from the wick. It thus appears that the flame becomes 'weaker' in microgravity due to the absence of buoyancy generated flow which serves to transport the oxidizer to the combustion zone and remove the hot combustion products from it. The buoyant flow, which may be characterized by the strain rate, assists the diffusion process to execute these essential functions for the survival of the flame. Thus, the diffusion flame is 'weak' at very low strain rates and as the strain rate increases the flame is initially 'strengthened' and eventually it may be 'blown out'. The computed flammability boundaries of T'ien show that such a reversal in material flammability occurs at strain rates around 5 sec. At very low or zero strain rates, flame radiation is expected to considerably affect this 'weak' diffusion flame because: (1) the concentration of combustion products which participate in gas radiation is high in the flame zone; and (2) low strain rates provide sufficient residence time for substantial amounts of soot to form which is usually responsible for a major portion of the radiative heat loss. We anticipate that flame radiation will eventually extinguish this flame. Thus, the objective of this project is to perform an experimental and theoretical investigation of radiation-induced extinction of diffusion flames under microgravity conditions. This is important for spacecraft fire safety.

Atreya, Arvind↗

NASA NTRS2022

Opportunistic Experiments to Constrain Aerosol Effective Radiative Forcing

Aerosol-cloud interactions (ACI) are considered to be the most uncertain driver of present-day radiative forcing due to human activities. The non-linearity of cloud-state changes to aerosol perturbations make it challenging to attribute causality in observed relationships of aerosol radiative forcing. Using correlations to infer causality can be challenging when meteorological variability also drives both aerosol and cloud changes independently. Natural and anthropogenic aerosol perturbations from well defined sources provide ‘opportunistic experiments’ (also known as natural experiments) to investigate ACI in cases where causality may be more confidently inferred. These perturbations cover a wide range of locations and spatio-temporal scales, including point sources such as volcanic eruptions or industrial sources, plumes from biomass burning or forest fires, and tracks from individual ships or shipping corridors.We review the different experimental conditions and conduct a synthesis of the available satellite data sets and field campaigns to place these opportunistic experiments on a common footing, facilitating new insights and a clearer understanding of key uncertainties in aerosol radiative forcing. Cloud albedo perturbations are strongly sensitive to background meteorological conditions. Strong liquid water path increases due to aerosol perturbations are largely ruled out by averaging across experiments. Opportunistic experiments have significantly improved process-level understanding of ACI, but it remains unclear how reliably the relationships found can be scaled to the global level, thus demonstrating a need for deeper investigation in order to improve assessments of aerosol radiative forcing and climate change.

Matthew W Christensen↗

DOE OSTI2017

Experimental Evaluation of an Oxidizing Hazard in the Presence of Sorbents

Oxidizing chemicals are commonly found in waste generated from actinide separations and other chemical processes. Because they can create and/or increase the combustion of combustible materials, they need to be experimentally evaluated, in order to provide a highly reliable assessment of their potential hazards. Two sets of experiments were performed using a modified approach to the Environmental Protection Agency (EPA) SW-846 Method 1040. In the first set of experiments (scoping studies), the purpose was to determine the relative strength of some selected oxidizers. In the second set of experiments, the potential of the strongest tested oxidizer to increase the burning rate or burning intensity of some selected sorbents was investigated. The overall goal of this work was to conservatively identify oxidizer/sorbent mixtures producing non-oxidizer results. A few results from this experimental study are presented herein. More exhaustive information on this work can be found in supporting documentation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Neutral beams for the burning plasma era: Simulations and modeling of deuterium ion beams for plasma heating (CRADA Final Report)

Together with Realta Fusion, we set up several simulation scenarios and ran simulations using the WarpX code which is developed by LBNL and especially by members of the LBNL team. We investigated beam transport and beam neutralization and ran optimization and benchmark simulations. To achieve this, several new features were added to the warpX code. These code additions will also be beneficial to other users of warpX including several fusion companies and researchers at National Laboratories. Furthermore, we supported Realta Fusion in setting up their own instances of WarpX. We presented our results at the American Physical Society Division of Plasma Physics meeting and are in the process of writing a publication that will be submitted to a peer-reviewed journal to share our results with the broader community.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Experimental observations of shock-wave-induced bubble collapse and hot-spot formation in nitromethane liquid explosive

We studied the collapse of individual helium gas bubbles in the homogeneous explosive nitromethane (NM) to investigate effects of hot-spot formation on the detonation process. A bubble was injected into a NM sample, and a shock wave from an explosive detonator compressed the bubble, creating a localized hot spot. We measured shock and detonation wave speeds with optical velocimetry, and we used a high-speed camera to image the shock propagation and the pre- and post-bubble collapse processes. An infrared camera image showed the residual radiance temperature distribution after the bubble collapse, and an optical fiber pyrometer measured the time-resolved thermal radiance. We measured the optical spectra of light emitted from detonating NM without a bubble and from a collapsing bubble in shocked, undetonated NM. We estimated temperatures of the detonation fronts and of the hot spots formed by bubble collapse. To study the incipient detonation process, we performed all bubble collapse experiments at pressures below the threshold for creating a sustained detonation. Where the bubble collapsed, we observed an opaque, thermally emissive region believed to be chemical reaction products. Chemical reactions in NM can be produced with lower shock pressures (~1 GPa) when a helium bubble is present than without a bubble (~10 GPa). We used hydrodynamic modeling to predict shock wave propagation, extent of chemical reaction, and subsequent temperature rise from the collapsing bubble. Simulations using a temperature-dependent Arrhenius burn model gave much better results than reactive burn models that depend only on pressure and density.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS1991

On the dynamics and composition of the high-latitude thermosphere

An overview is presented of some of the more recent progress made in the study of the dynamics and composition of the high-latitude thermosphere at the University of Michigan, with emphasis on the interpretation of experimental measurements made from the DE-2 spacecraft and from ground-based observatories in Greenland. Attention is focused on perturbations to the solar-driven upper thermospheric winds, temperatures, and compositional structures due to forcing associated with high-latitude ionosphere-thermosphere coupling processes. The nature of the experimental measurements made on DE-2 is discussed. The vector spherical harmonic model, some sample results, and experiment-model comparisons are described using both satellite and ground-based measurements of high-latitude thermosphere dynamics. Considerations pertaining to compositional perturbations at high latitudes are presented.

Killeen, T. L.↗

DOE OSTI2016

Assessment of wildland fire impacts on watershed annual water yield: Analytical framework and case studies in the United States

More than 50% of water supplies in the conterminous United States originate on forestland or rangeland and are potentially under increasing stress as a result of larger and more severe wildfires. Little is known, however, about the long-term impacts of fire on annual water yield and the role of climate variability within this context. We here propose a framework for evaluating wildland fire impacts on streamflow that combines double-mass analysis with new methods (change point analysis, climate elasticity modeling, and process-based modeling) to distinguish between multiyear fire and climate impacts. The framework captures a wide range of fire types, watersheds characteristics, and climate conditions using streamflow data, as opposed to other approaches requiring paired watersheds. The process is illustrated with three case studies. A watershed in Arizona experienced a +266% increase in annual water yield in the 5 years after a wildfire, where +219% was attributed to wildfire and +24% to precipitation trends. In contrast, a California watershed had a lower (–64%) post-fire net water yield, comprised of enhanced flow (+38%) attributed to wildfire offset (–102%) by lower precipitation in the post-fire period. Changes in streamflow within a watershed in South Carolina had no apparent link to periods of prescribed burning but matched a very wet winter and reports of storm damage. As a result, the presented framework is unique in its ability to detect and quantify fire or other disturbances, even if the date or nature of the disturbance event is uncertain, and regardless of precipitation trends.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2013

A SUPER-EDDINGTON WIND SCENARIO FOR THE PROGENITORS OF TYPE Ia SUPERNOVAE

The accretion of hydrogen-rich material on to carbon-oxygen white dwarfs (CO WDs) is crucial for understanding Type Ia supernova (SN Ia) from the single-degenerate model, but this process has not been well understood due to the numerical difficulties in treating H and He flashes during the accretion. For CO WD masses from 0.5 to 1.378 M {sub ☉} and accretion rates in the range from 10{sup –8} to 10{sup –5} M {sub ☉} yr{sup –1}, we simulated the accretion of solar-composition material on to CO WDs using the state-of-the-art stellar evolution code of MESA. For comparison with steady-state models, we first ignored the contribution from nuclear burning to the luminosity when determining the Eddington accretion rate, and found that the properties of H burning in our accreting CO WD models are similar to those from the steady-state models, except that the critical accretion rates at which the WDs turn into red giants or H-shell flashes occur on their surfaces are slightly higher than those from the steady-state models. However, the super-Eddington wind is triggered at much lower accretion rates than previously thought, when the contribution of nuclear burning to the total luminosity is included. This super-Eddington wind naturally prevents the CO WDs with high accretion rates from becoming red giants, thus presenting an alternative to the optically thick wind proposed by Hachisu et al. Furthermore, the super-Eddington wind works in low-metallicity environments, which may explain SNe Ia observed at high redshifts.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2012

Position Paper on Practicable Performance Criteria for the Removal Efficiency of Volatile Radionuclides

As a result of fuel reprocessing, volatile radionuclides may be released from the facility stack if no processes are put in place to remove them. The radionuclides that are of concern in this document are 3 H, 14 C, 85 Kr, and 129 I. The question we attempted to answer is how efficient must this removal process be for each of these radionuclides? To answer this question, we examined the three regulations that may impact the degree to which these radionuclides must be reduced before process gases can be released from the facility. These regulations are 40 CFR 61 (EPA 2010a), 40 CFR 190(EPA 2010b), and 10 CFR 20 (NRC 2012). These regulations apply to the total radionuclide release and to a particular organ - the thyroid. Because these doses can be divided amongst all the radionuclides in different ways and even within the four radionuclides in question, we provided several cases. We first looked at the inventories for these radionuclides for three fuel types (PWR UOX, PWR MOX, and AHTGR), several burn-up values, and time out of reactor extending to 200 y. We calculated doses to the maximum exposed individual (MEI) with the EPA code CAP-88 (Rosnick 1992). Finally, we looked at two dose cases. Allocating all of the allowable dose to be used by the volatile radionuclides is one case, but, perhaps, unrealistic. In lieu of this, we arbitrarily selected a value of 10% of the allowable dose to be assigned to the volatile radionuclides. We calculated the required decontamination factors (DFs) for both of these cases, including the case for the thyroid dose for which 14 C and 129 I were the main contributors. With respect to 129 I doses, we found that the highest dose was calculated with iodine as a fine particulate. The dose scaled as the fraction of the total 129 I that was particulate. Therefore, we assumed for all of our calculations that 100% of the 129 I was particulate and allow the user of the results given here to scale our calculated doses to their needs.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Vertical profiles of trace gas and aerosol properties over the eastern North Atlantic: variations with season and synoptic condition

Abstract. Because of their extensive coverage, marine low clouds greatly impact the global climate. Presently, the response of marine low clouds to the changes in atmospheric aerosols remains a major source of uncertainty in climate simulations. One key contribution to this large uncertainty derives from the poor understanding of the properties and processes of marine aerosols under natural conditions and the perturbation by anthropogenic emissions. The eastern North Atlantic (ENA) is a region of persistent but diverse subtropical marine boundary layer (MBL) clouds, where cloud albedo and precipitation are highly susceptible to perturbations in aerosol properties. Here we examine the key processes that drive the cloud condensation nuclei (CCN) population in the MBL using comprehensive characterizations of aerosol and trace gas vertical profiles during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. During ACE-ENA, a total of 39 research flights were conducted in the Azores: 20 during summer 2017 and 19 during winter 2018. During summer, long-range-transported aerosol layers were periodically observed in the lower free troposphere (FT), leading to elevated FT CCN concentrations (NCCN). Both biomass burning and pollution from North America contribute to submicron aerosol mass in these layers, with pollution likely the dominant contributor. In contrast, long-range transported continental emissions have a much weaker influence on the aerosol properties in the ENA during the winter season. While the entrainment of FT air is a major source of particle number in the MBL for both seasons, on average it does not serve as a direct source of CCN in the MBL because the average FT NCCN is the same or even lower than that in the MBL. The particle number flux due to FT entrainment is dominated by pre-CCN (particles that are too small to form cloud droplets under typical conditions, i.e., particles with sizes below the Hoppel minimum) due to the elevated Npre-CCN in the lower FT. Once these pre-CCN are entrained into the MBL, they can grow and reach CCN size range through condensational growth, representing an indirect and major source of MBL CCN in the ENA. The impact of synoptic conditions on the aerosol properties is examined. Under pre-front and post-front conditions, shallow convective activity often leads to a deep and decoupled boundary layer. Coalescence scavenging and evaporation of drizzle below clouds lead to reduced NCCN and larger accumulation-mode particle sizes in the upper cloud-containing decoupled layer, indicating that surface measurements overestimate the NCCN relevant to the formation of MBL clouds under decoupled conditions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Aircraft measurements of aerosol and trace gas chemistry in the eastern North Atlantic

The Aerosol and Cloud Experiment in the Eastern North Atlantic (ACE-ENA) investigated properties of aerosols and subtropical marine boundary layer (MBL) clouds. Low subtropical marine clouds can have a large effect on Earth's radiative budget, but they are poorly represented in global climate models. In order to understand their radiative effects, it is imperative to understand the composition and sources of the MBL cloud condensation nuclei (CCN). The campaign consisted of two intensive operation periods (IOPs) (June–July 2017 and January–February 2018) during which an instrumented G-1 aircraft was deployed from Lajes Field on Terceira Island in the Azores, Portugal. The G-1 conducted research flights in the vicinity of the Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) atmospheric observatory on Graciosa Island. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and Ionicon proton-transfer-reaction mass spectrometer (PTR-MS) were deployed aboard the aircraft, characterizing chemistry of non-refractory aerosol and trace gases, respectively. The eastern North Atlantic region was found to be very clean, with an average non-refractory submicrometer aerosol mass loading of 0.6 µg m −3 in the summer and 0.1 µg m −3 in the winter, measured by the AMS. Average concentrations of the trace reactive gases methanol and acetone were 1–2 ppb; benzene, toluene and isoprene were even lower, <1 ppb. Mass fractions of sulfate, organics, ammonium and nitrate in the boundary layer were 69 %, 23 %, 7 % and 1 % and remained largely similar between seasons. The aerosol chemical composition was dominated by sulfate and highly processed organics. Particulate methanesulfonic acid (MSA), a well-known secondary biogenic marine species, was detected, with an average boundary layer concentration of 0.021 µg m −3 , along with its gas-phase precursor, dimethyl sulfide (DMS). MSA accounted for no more than 3 % of the submicron, non-refractory aerosol in the boundary layer. Examination of vertical profiles of aerosol and gas chemistry during ACE-ENA reveals an interplay of local marine emissions and long-range-transported aged aerosol. A case of transport of biomass burning emissions from North American fires has been identified using back-trajectory analysis. In the summer, the non-refractory portion of the background CCN budget was heavily influenced by aerosol associated with ocean productivity, in particular sulfate formed from DMS oxidation. Episodic transport from the continents, particularly of biomass burning aerosol, periodically increased CCN concentrations in the free troposphere. In the winter, with ocean productivity lower, CCN concentrations were overall much lower and dominated by remote transport. These results show that anthropogenic emissions perturb CCN concentrations in remote regions that are sensitive to changes in CCN number and illustrate that accurate predictions of both transport and regional aerosol formation from the oceans are critical to accurately modeling clouds in these regions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Large spatiotemporal variability in aerosol properties over central Argentina during the CACTI field campaign

Abstract. Few field campaigns with extensive aerosol measurements have been conducted over continental areas in the Southern Hemisphere. To address this data gap and better understand the interactions of convective clouds and the surrounding environment, extensive in situ and remote sensing measurements were collected during the Cloud, Aerosol, and Complex Terrain Interactions (CACTI) field campaign conducted between October 2018 and April 2019 over the Sierras de Córdoba range of central Argentina. This study describes measurements of aerosol number, size, composition, mixing state, and cloud condensation nuclei (CCN) collected on the ground and from a research aircraft during 7 weeks of the campaign. Large spatial and multiday variations in aerosol number, size, composition, and CCN were observed due to transport from upwind sources controlled by mesoscale to synoptic-scale meteorological conditions. Large vertical wind shears, back trajectories, single-particle measurements, and chemical transport model predictions indicate that different types of emissions and source regions, including biogenic emissions and biomass burning from the Amazon and anthropogenic emissions from Chile and eastern Argentina, contribute to aerosols observed during CACTI. Repeated aircraft measurements near the boundary layer top reveal strong spatial and temporal variations in CCN and demonstrate that understanding the complex co-variability of aerosol properties and clouds is critical to quantify the impact of aerosol–cloud interactions. In addition to quantifying aerosol properties in this data-sparse region, these measurements will be valuable to evaluate predictions over the midlatitudes of South America and improve parameterized aerosol processes in local, regional, and global models.

54 ENVIRONMENTAL SCIENCES↗