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DOE OSTI2024

Capturing carbon dioxide from air with charged-sorbents

Emissions reduction and greenhouse gas removal from the atmosphere are both necessary to achieve net-zero emissions and limit climate change. There is thus a need for improved sorbents for the capture of carbon dioxide from the atmosphere, a process known as direct air capture. In particular, low-cost materials that can be regenerated at low temperatures would overcome the limitations of current technologies. In this work, we introduce a new class of designer sorbent materials known as ‘charged-sorbents’. These materials are prepared through a battery-like charging process that accumulates ions in the pores of low-cost activated carbons, with the inserted ions then serving as sites for carbon dioxide adsorption. We use our charging process to accumulate reactive hydroxide ions in the pores of a carbon electrode, and find that the resulting sorbent material can rapidly capture carbon dioxide from ambient air by means of (bi)carbonate formation. Unlike traditional bulk carbonates, charged-sorbent regeneration can be achieved at low temperatures (90–100 °C) and the sorbent’s conductive nature permits direct Joule heating regeneration using renewable electricity. Given their highly tailorable pore environments and low cost, we anticipate that charged-sorbents will find numerous potential applications in chemical separations, catalysis and beyond.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

tert -Butyl peroxy radical: ground and first excited state energetics and fundamental frequencies

Alkylperoxy radicals (RO 2 ˙) are key intermediates in combustion and atmospheric oxidation processes. As such, reliable detection and monitoring of these radicals can provide a wealth of information about the underlying chemistry. The tert-butyl peroxy radical is the archetypal tertiary peroxy radical, yet its vibrational spectroscopy is largely unexplored. To aid in future experimental investigations, we have performed high-level theoretical studies of the fundamental vibrational frequencies of the ground- and first excited states. A conformer search on both electronic surfaces reveals single minimum-energy structures. We predict an à 2 A' ← X 2 A" adiabatic excitation energy of 7738 cm -1 via focal point analysis, approximating the CCSDT(Q)/CBS level of theory. This excitation energy agrees to within 17 cm -1 of the most accurate experimental measurement. We compute CCSD(T) fundamental vibrational frequencies via second-order vibrational perturbation theory (VPT2), using a hybrid force field in which the quadratic (cubic/quartic) force constants are evaluated with the ANO1 (ANO0) basis set. Anharmonic resonance polyads are treated with the VPT2 + K effective Hamiltonian approach. Among the predicted fundamental frequencies, the ground state O–O stretch, excited state O–O stretch, and excited state C–O–O bend fundamentals are predicted at 1138, 959, and 490 cm -1 , respectively. Basis set sensitivity is found to be particularly great for the O–O stretches, similar to what has already been noted in smaller, unbranched peroxy radicals. Exempting these O–O stretches, agreement with the available experimental fundamentals is generally good (±10 cm -1 ).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Electrical properties of GaAs metal–oxide–semiconductor structure comprising Al{sub 2}O{sub 3} gate oxide and AlN passivation layer fabricated in situ using a metal–organic vapor deposition/atomic layer deposition hybrid system

This paper presents a compressive study on the fabrication and optimization of GaAs metal–oxide–semiconductor (MOS) structures comprising a Al{sub 2}O{sub 3} gate oxide, deposited via atomic layer deposition (ALD), with an AlN interfacial passivation layer prepared in situ via metal–organic chemical vapor deposition (MOCVD). The established protocol afforded self-limiting growth of Al{sub 2}O{sub 3} in the atmospheric MOCVD reactor. Consequently, this enabled successive growth of MOCVD-formed AlN and ALD-formed Al{sub 2}O{sub 3} layers on the GaAs substrate. The effects of AlN thickness, post-deposition anneal (PDA) conditions, and crystal orientation of the GaAs substrate on the electrical properties of the resulting MOS capacitors were investigated. Thin AlN passivation layers afforded incorporation of optimum amounts of nitrogen, leading to good capacitance–voltage (C–V) characteristics with reduced frequency dispersion. In contrast, excessively thick AlN passivation layers degraded the interface, thereby increasing the interfacial density of states (D{sub it}) near the midgap and reducing the conduction band offset. To further improve the interface with the thin AlN passivation layers, the PDA conditions were optimized. Using wet nitrogen at 600 °C was effective to reduce D{sub it} to below 2 × 10{sup 12} cm{sup −2} eV{sup −1}. Using a (111)A substrate was also effective in reducing the frequency dispersion of accumulation capacitance, thus suggesting the suppression of traps in GaAs located near the dielectric/GaAs interface. The current findings suggest that using an atmosphere ALD process with in situ AlN passivation using the current MOCVD system could be an efficient solution to improving GaAs MOS interfaces.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Evaluating the WFIP2 updates to the HRRR model using scanning Doppler lidar measurements in the complex terrain of the Columbia River Basin

The wind-energy (WE) industry relies on numerical weather prediction (NWP) forecast models as foundational or base models for many purposes, including wind-resource assessment and wind-power forecasting. During the Second Wind Forecast Improvement Project (WFIP2) in the Columbia River Basin of Oregon and Washington, a significant effort was made to improve NWP forecasts through focused model development, to include experimental refinements to the High Resolution Rapid Refresh (HRRR) model physics and horizontal grid spacing. In this study, the performance of an experimental version of HRRR that includes these refinements is tested against a control version, which corresponds to that of the operational HRRR run by National Oceanic and Atmospheric Administration/National Centers for Environmental Protection at the outset of WFIP2. Furthermore, the effects of horizontal grid resolution were also tested by comparing wind forecasts from the HRRR (with 3-km grid spacing) with those from a finer-resolution HRRR nest with 750-m grid spacing. Model forecasts are validated against accurate wind-profile measurements by three scanning, pulsed Doppler lidars at sites separated by a total distance of 71 km. Model skill and improvements in model skill, attributable to physics refinements and improved horizontal grid resolution, varied by season, by site, and during periods of atmospheric phenomena relevant to WE. In general, model errors were the largest below 150 m above ground level (AGL). Experimental HRRR refinements tended to reduce the mean absolute error (MAE) and other error metrics for many conditions, but degradation in skill (increased MAE) was noted below 150 m AGL at the two lowest-elevation sites at night. Finer resolution was found to produce the most significant reductions in the error metrics.

17 WIND ENERGY↗
DOE OSTI2022

Observation of breakdown wave mechanism in avalanche ionization produced atmospheric plasma generated by a picosecond CO 2 laser

Understanding the formation and long-timescale evolution of atmospheric plasmas produced by ultrashort, long-wavelength infrared (LWIR) pulses is an important but partially understood problem. Of particular interest are plasmas produced in air with a peak laser intensity ~10 12 W/cm 2 , the so-called clamping intensity observed in LWIR atmospheric guiding experiments where tunneling and multi-photon ionization operative at near-IR or shorter wavelengths are inoperative. We find that avalanche breakdown on the surface of aerosol (dust) particles can act to seed the breakdown of air observed above the 200 GW/cm 2 threshold when a train of 3 ps 10.6 μm laser pulses separated by 18 ps is used. The breakdown first appears at the best focus but propagates backward toward the focusing optic as the plasma density approaches critical density and makes forward propagation impossible. The velocity of the backward propagating breakdown can be as high as 10 9 cm/s, an order of magnitude greater than measured with ns pulse-produced breakdown, and can be explained rather well by the so-called breakdown wave mechanism. Transverse plasma expansion with a similar velocity is assisted by UV photoionization and is observed as a secondary longitudinal breakdown mechanism in roughly 10% of the shots. When a cm-size, TW power beam is propagated, interception of aerosol particles is guaranteed and several (40 cm -3 ) breakdown sites appear, each initially producing a near-critical density plasma. On a 10 ns–1 μs timescale, shockwaves from each site expand radially and coalesce to produce a large hot gas channel. The radial velocity of the expansion agrees well with the prediction of the blast wave theory developed for ultrafast atmospheric detonations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Impact of metal diffusion, lattice distortions, native defects, and ambient on dielectric breakdown in Ni–Ga 2 O 3 Schottky diodes

Ga 2 O 3 unipolar devices are of high interest due to their ~8 MV/cm predicted breakdown fields, which have not yet been achieved due to premature device failure. Pre- and post-failure defect analysis of Ni–Ga 2 O 3 Schottky diodes in ultrahigh vacuum (UHV) and air were performed using depth-resolved cathodoluminescence, high angle annular dark field scanning transmission electron microscopy, and energy dispersive x-ray analysis to understand the physical mechanisms that precede premature breakdown. The breakdown voltage in UHV was dramatically reduced by nearly 40% compared with the breakdown in air. This reduction in the breakdown voltage correlated with post-breakdown differences in Ni distribution, indicating that the coordination and bonding of Ni contribute strongly to electrical behavior in Ni–Ga 2 O 3 Schottky diodes. Breakdown studies in UHV revealed that Ni diffuses away more from the metal–semiconductor interface than with air breakdown, where Ni localizes more near the interface, indicative of the preferential formation of a Ni oxide under O-poor conditions. These measurements also identified the formation of divacancy-interstitial complexes and their characteristic luminescence signature ~150 nm from the interface, the densities of which correlated with breakdown fields. These findings show that electric-field-induced degradation occurs via the rearrangement of native point defects, which act as an additional precursor to device failure. Macroscopically, they show the impact of both vacuum conditions and metal reactivity on Ga 2 O 3 device fabrication.

36 MATERIALS SCIENCE↗
DOE OSTI2015

X-ray perspective of the twisted magnetospheres of magnetars

Anomalous X-ray pulsars (AXPs) and soft gamma-ray repeaters (SGRs) are recognized as the most promising magnetar candidates, as indicated by their energetic bursts and rapid spin-downs. It is expected that the strong magnetic field leaves distinctive imprints on the emergent radiation both by affecting the radiative processes in atmospheres of magnetars and by scattering in the upper magnetospheres. We construct a self-consistent physical model that incorporates emission from the magnetar surface and its reprocessing in the three-dimensional (3D) twisted magnetosphere using a Monte Carlo technique. The synthetic spectra are characterized by four parameters: surface temperature kT, surface magnetic field strength B, magnetospheric twist angle Δϕ, and the normalized electron velocity β. We also create a tabular model (STEMS3D) and apply it to a large sample of XMM-Newton spectra of magnetars. The model successfully fits nearly all spectra, and the obtained magnetic field for 7 out of the 11 sources are consistent with the values inferred from the spin-down rates. We conclude that the continuum-fitting by our model is a robust method to measure the magnetic field strength and magnetospheric configuration of AXPs and SGRs. Investigating the multiple observations of variable sources, we also study the mechanism of their spectral evolution. Our results suggest that the magnetospheres in these sources are highly twisted (Δϕ>1), and the behavior of magnetospheric twisting and untwisting is revealed in the 2002 outburst of 1E 2259+586.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2013

THE BOLOCAM GALACTIC PLANE SURVEY. IX. DATA RELEASE 2 AND OUTER GALAXY EXTENSION

We present a re-reduction and expansion of the Bolocam Galactic Plane Survey (BGPS), first presented by Aguirre et al. and Rosolowsky et al. The BGPS is a 1.1 mm survey of dust emission in the Northern galactic plane, covering longitudes –10° < l < 90° and latitudes |b| < 0.°5 with a typical 1σ rms sensitivity of 30-100 mJy in a ∼33'' beam. Version 2 of the survey includes an additional ∼20 deg{sup 2} of coverage in the third and fourth quadrants and ∼2 deg{sup 2} in the first quadrant. The new data release has improved angular recovery, with complete recovery out to ∼80'' and partial recovery to ∼300'', and reduced negative bowls around bright sources resulting from the atmospheric subtraction process. We resolve the factor of 1.5 flux calibration offset between the v1.0 data release and other data sets and determine that there is no offset between v2.0 and other data sets. The v2.0 pointing accuracy is tested against other surveys and is demonstrated to be accurate and an improvement over v1.0. We present simulations and tests of the pipeline and its properties, including measurements of the pipeline's angular transfer function. The Bolocat cataloging tool was used to extract a new catalog, which includes 8594 sources, with 591 in the expanded regions. We have demonstrated that the Bolocat 40'' and 80'' apertures are accurate even in the presence of strong extended background emission. The number of sources is lower than in v1.0, but the amount of flux and area included in identified sources is larger.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2015

Printed Module Interconnects

Monolithic interconnects in photovoltaic modules connect adjacent cells in series, and are typically formed sequentially involving multiple deposition and scribing steps. Interconnect widths of 500 um every 10 mm result in 5% dead area, which does not contribute to power generation in an interconnected solar panel. This work expands on previous work that introduced an alternative interconnection method capable of producing interconnect widths less than 100 um. The interconnect is added to the module in a single step after deposition of the photovoltaic stack, eliminating the need for scribe alignment. This alternative method can be used for all types of thin film photovoltaic modules. Voltage addition with copper-indium-gallium-diselenide (CIGS) solar cells using a 2-scribe printed interconnect approach is demonstrated. Additionally, interconnect widths of 250 um are shown.

14 SOLAR ENERGY↗
DOE OSTI2015

Opportunities for Improving Photovoltaic Performance with Better Transparent Contacts

NREL and DOE recently held a workshop to assess the challenges, opportunities and potential impacts for improved transparent contacts (TCs) to positively impact current and emerging photovoltaic conversion technologies. Here, we report on the workshop outcomes based on the collective input and participation from industry, academia, national laboratories and DOE. A primary conclusion is that new emerging materials can have significant impacts on the overall performance, reliability and cost for commercial scale PV. One key observation is that TC's should no longer be thought of as a single-layer single-purpose material but as an integrated contact layer stack that includes a charge selective interface layer, a conducting layer and sometimes layers for reliability or light management. In addition, the long standing goal of developing of high performance atmospheric-pressure-processed TCs has finally been met by the rapidly improving Ag nanowire based composites with better than ITO performance from an all ink based process. Even the more conventional metal oxide materials are improving rapidly by introducing solution processed buffer layers, and even conductor layers. This rapid evolution has opened the way to high-throughput low-cost TC processing. Key desired metrics for TCs and approaches to achieving them are discussed.

14 SOLAR ENERGY↗
DOE OSTI2024

A comparison of smartphone and infrasound microphone data from a fuel air explosive and a high explosive

For prompt detection of large (>1 kt) above-ground explosions, infrasound microphone networks and arrays are deployed at surveyed locations across the world. Denser regional and local networks are deployed for smaller explosions, however, they are limited in number and are often deployed temporarily for experiments. With the expanded interest in smaller yield explosions targeted at vulnerable areas such as population centers and key infrastructures, the need for more dense microphone networks has increased. An “attritable” (affordable, reusable, and replaceable) and flexible alternative can be provided by smartphone networks. Explosion signals from a fuel air explosive (thermobaric bomb) and a high explosive with trinitrotoluene equivalent yields of 6.35 and 3.63 kg, respectively, were captured on both an infrasound microphone and a network of smartphones. The resulting waveforms were compared in time, frequency, and time-frequency domains. The acoustic waveforms collected on smartphones produced a filtered explosion pulse due to the smartphone's diminishing frequency response at infrasound frequencies (<20 Hz) and was found difficult to be used with explosion characterization methods utilizing waveform features (peak overpressure, impulse, etc.). However, the similarities in time frequency representations and additional sensor inputs are promising for other explosion signal identification and analysis. As an example, a method utilizing the relative acoustic amplitudes for source localization using the smartphone sensor network is presented.

47 OTHER INSTRUMENTATION↗
DOE OSTI2016

Ice-nucleating bacteria control the order and dynamics of interfacial water

Ice-nucleating organisms play important roles in the environment. With their ability to induce ice formation at temperatures just below the ice melting point, bacteria such as Pseudomonas syringae attack plants through frost damage using specialized ice-nucleating proteins. Besides the impact on agriculture and microbial ecology, airborne P. syringae can affect atmospheric glaciation processes, with consequences for cloud evolution, precipitation, and climate. Biogenic ice nucleation is also relevant for artificial snow production and for biomimetic materials for controlled interfacial freezing. We use interface-specific sum frequency generation (SFG) spectroscopy to show that hydrogen bonding at the water-bacteria contact imposes structural ordering on the adjacent water network. Experimental SFG data and molecular dynamics simulations demonstrate that ice active sites within P. syringae feature unique hydrophilic-hydrophobic patterns to enhance ice nucleation. Finally, the freezing transition is further facilitated by the highly effective removal of latent heat from the nucleation site, as apparent from time-resolved SFG spectroscopy.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2013

Collapse and backward motion of axisymmetric toroidal vortices in an accretion flow

The problem of the interaction of two coaxial, counter-rotating ring vortices in the presence of a convergent (accretion) flow with a sink at the center of symmetry has been solved. The vortices that would recede from each other in the absence of a flow (the problem inverse to the Helmholtz problem) are shown to be brought closer together by the flow and then ejected with acceleration along the axis of symmetry. The ejection velocity increases with sink strength. However, if the sink strength exceeds some critical value that depends on the initial conditions, then no ejection occurs and the vortices are captured by the flow and collapse. A similar capture and collapse are also possible during the motion of a single vortex in a flow. The difference from the planar case, where no collapse occurs, is significant. The detected phenomenon can be applied when studying nonlinear processes in atmospheric vortices as well as in active galactic nuclei and planetary atmospheres.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Surface Quantitative Precipitation Estimates (SQUIRE) of Snow Water Equivalent from the Surface Atmospheric Integrated Field Laboratory

The upper Colorado River basin is the primary source of water for 40 million people. With declining snowpack in the basin, forecasting hydrological budgets in the Southwest United States is more important than ever. However, due in part, to a lack of reliable observations of precipitation in complex terrain, hydrological models struggle to assess and forecast snowpack snow water equivalent (SWE) in the upper Colorado River basin (UCRB). Therefore, the need for more reliable SWE forecasts in the UCRB motivated the U.S. Department of Energy Atmospheric Radiation Measurement Facility’s Surface Atmospheric Integrated Field Laboratory (SAIL) that occurred from June 2021 to June 2023. During SAIL, the X-band precipitation radar from Colorado State University conducted volume scans sampling the precipitation properties over the UCRB. The ARM facility developed a gridded Surface Quantitative Precipitation Estimates (SQUIRE) product from the radar observations. To do this, various daily SWE estimates from radar using the radar reflectivity factor Z e and specific differential phase K dp were compared against ground-based precipitation gauges. SWE in precipitation calculated from Wolfe and Snider’s S–Z e estimator was in best agreement with the rain gauges for the days when SWE < 12 mm. For days with SWE > 12 mm, the WSR-88D Intermountain West relationship had the best agreement with the precipitation gauges. Airborne snow depth observations show that SQUIRE captures regions of orographic enhancement in the mountains to the west and northwest of the SAIL study area, indicating that the scientific community should focus on understanding and ultimately simulating orographic atmospheric precipitation processes to improve UCRB snowpack SWE assessment and forecasting.

Hydrology↗
DOE OSTI2013

Collaborative Research: Using ARM Observations to Evaluate GCM Cloud Statistics for Development of Stochastic Cloud-Radiation Parameterizations

The long-range goal of several past and current projects in our DOE-supported research has been the development of new and improved parameterizations of cloud-radiation effects and related processes, using ARM data, and the implementation and testing of these parameterizations in global models. The main objective of the present project being reported on here has been to develop and apply advanced statistical techniques, including Bayesian posterior estimates, to diagnose and evaluate features of both observed and simulated clouds. The research carried out under this project has been novel in two important ways. The first is that it is a key step in the development of practical stochastic cloud-radiation parameterizations, a new category of parameterizations that offers great promise for overcoming many shortcomings of conventional schemes. The second is that this work has brought powerful new tools to bear on the problem, because it has been an interdisciplinary collaboration between a meteorologist with long experience in ARM research (Somerville) and a mathematician who is an expert on a class of advanced statistical techniques that are well-suited for diagnosing model cloud simulations using ARM observations (Shen). The motivation and long-term goal underlying this work is the utilization of stochastic radiative transfer theory (Lane-Veron and Somerville, 2004; Lane et al., 2002) to develop a new class of parametric representations of cloud-radiation interactions and closely related processes for atmospheric models. The theoretical advantage of the stochastic approach is that it can accurately calculate the radiative heating rates through a broken cloud layer without requiring an exact description of the cloud geometry.

58 GEOSCIENCES↗
DOE OSTI2017

Multidisciplinary Approaches to Radiation Balanced Lasers (MARBLe): 1st Annual Progress Report

The initial main modifications of the existing μPD crystal-growth system at LANL have been completed. This now gives us the new capability to develop the growth of crystalline RBL materials by both the μPD and the Bridgman method. Quantitative mass spectrometry of the growth atmosphere was conducted to identify possible sources of gaseous trace species (primarily hydrogen) that could cause the undesired reduction of Yb 3+ to Yb 2+ during the crystal growth. Hydrogen was found to be at sufficiently low levels to not be a respective concern. Studies on the thermal decomposition of YbF 3 to form Yb 2+ are currently underway in collaboration with MARBLe team member Prof. Pauzauskie. First samples of Yb 3+ -doped YLiF 4 (YLF:Yb) and undoped LiLuF 4 (LLF) were grown, and MARBLe team member Prof. Sheik-Bahae has performed measurements of laser-induced heating (YLF:Yb) and background absorption coefficient (LLF). We discovered that one or several of the YF 3 , LiF, and YbF 3 precursors contains organic impurities that chemically reduce to black residue during the high-temperature growth in oxygen-free argon atmosphere. A process for removal of these residues prior to growth is being considered. Comparing the results from incongruently melting YLF with those of congruently melting LLF indicate that a congruently melting material is preferred for Bridgman growth. Crystal-growth experiments with LLF are currently underway. The results of these studies on Yb 3+ doped materials will be directly applicable to the future growth of Er 3+ and Tm 3+ doped as well as Yb 3+ , Nd 3+ co-doped RBL crystals. There was no activity on the parallel effort of developing rareearth- doped chalcogenide glasses. The primary reason was a lack of manpower due to a delayed hiring of a student. In September 2017, we have hired a Postdoctoral Researcher who will be able to contribute to the growth (at LANL) and optical characterization (at UNM) of RBL materials.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Commercialization of an Atmospheric Iron-based CDCL Process for Power Production: Phase II

This project is focused on supporting the use of coal for power production through the continued development of the Coal Direct Chemical Looping (CDCL) technology. The objective of the program is to evaluate the commercial viability of the CDCL technology. This report describes the results of Phase II of the project up to the date of the period of performance as listed above. The Phase II objectives are to reduce the technology gaps associated with the oxygen-carrier properties, coal conversion, and reducer design of the CDCL process. During this project, a 250 kWth CDCL pilot unit was designed, fabricated, installed and subsequently tested to demonstrate critical components. The pilot unit simulates actual design concepts envisioned for the commercial unit. The knowledge gained from laboratory and pilot-scale testing is used to refine the commercial plant design and cost analyses.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2023

Assessing the link between aerosol mixing state, structure and composition and their optical properties: Ascension Island as a testbed for the South‐East Atlantic aerosol regimes

Forest and savanna fires are a major source of pollution over the globe. Such fire events emit to the atmosphere a considerable amount of “fluffy” fractal black looking particles that are often referred to as black carbon (BC) or soot aerosols. In fact, BC particles (aerosols) emitted from savanna and agricultural fires over the African continent play an important role in the region’s and the global climate. These fires occur each year between July and October, which is referred to as the biomass burning (BB) season and are considered among the globe's largest man-made emission sources of BC particles. However, during these fire events, not only BC particles are emitted, but also other types of particles and gases that can interact with each other to create new particles, generating a slew of particles often generally referred to as BB aerosols. Although the majority of the fire emissions occur inland in the sub-Saharan part of Africa, their effect reaches far beyond the continent due to the prevailing easterly winds, which transport those aerosols over the South-East Atlantic (SEA) ocean, off the west-coast of Africa. The reason why these particles are so important to the regional and global climate is that they absorb sunlight radiation, which overall warms the climate. However, the magnitude of this warming effect is highly uncertain and depends upon a multitude of aspects. Our overarching goal for this project was to better understand the changes in the aerosol properties as they transport from fire sources downstream toward the ocean and how this can eventually affect the earth's radiative budget in terms of warming or cooling. Following the above, our work here was focused on the investigation of the African BB aerosol plumes mixing state (mixing of BB aerosols and other aerosol types), composition and size distribution as they transport from the African continent towards the SEA ocean, and their link with some of the commonly measurable bulk optical properties such as mass absorption coefficient (MAC) and single scattering albedo (SSA). We utilized three field missions that were conducted over the SEA ocean between 2016 and 2018. Specifically, we used (1) ground-based measurements from the DOE ARM Mobile Facility (AMF1), which was deployed at Ascension Island (ASI) for the LASIC (Layered Atlantic Smoke Interactions with Clouds) campaign between June 2016 and October 2017, (2) airborne measurements from the UK CLARIFY (Clouds and Aerosol Radiative impacts and Forcing) campaign during Aug-Sep-2017, and (3) airborne measurements from the ORACLES (Observations of Aerosols above Clouds and their interactions) campaign during Aug-2017, and Sep-Oct-2018. The three campaigns cover a relatively large region, from the western African coast on the east towards Ascension Island in the middle of the SEA to the west. We used the data gathered by these campaigns to find how BB properties and composition change from near emission sources (the ORACLES campaign flights) downstream (the CLARIFY flights and the ground based LASIC measurements). We used particle trajectory following methodologies to connect the measurements from the different campaigns, which allowed us to follow a certain aerosol plume (airmass) from near-source towards Ascension Island. We found out that atmospheric aging processes governed by the UV light from the sun (photochemistry) and cloud processes (aqueous chemistry) govern the changes seen in the particle composition during the transport were more dominant in dictating aerosol composition than specific emission composition or source types. We assessed how aerosol optical properties change during the BB season and what are the main drivers of this change. We found that the enhanced ratio of BC to CO is well correlated with single scattering albedo (SSA) and mass absorption coefficient (MACBC), providing a simple way to estimate the aerosol optical characteristics in the south-eastern Atlantic Ocean. From the analysis of the location of BB, the primary source fuel, the water content in the fuel, combined with the mean cloud cover and precipitation in the transport areas of the BB plume, we conclude that the increase in BC/CO from June to August is likely to be caused by burning becoming more flaming (hot fires), and the decrease in BC/CO in September and October may be caused by smoldering (colder) fires. We found that aerosol hygroscopicity increases with decreasing altitude below 2km, and that enhanced BB hygroscopicity at lower altitudes is mainly due to a lower organic aerosol (OA) fraction, increased sulfate fraction, and greater hygroscopicity parameter of OA at lower altitudes.

54 ENVIRONMENTAL SCIENCES↗