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.