The authors examine atmospheric processes and their influence on cloud condensation nucleic activity. Topics discussed include the fundamentals of water uptake by particles.
The effect of an increase in atmospheric aerosol concentrations on the distribution and radiative properties of Earth’s clouds is the most uncertain component of the overall global radiative forcing ...from preindustrial time. General circulation models (GCMs) are the tool for predicting future climate, but the treatment of aerosols, clouds, and aerosol–cloud radiative effects carries large uncertainties that directly affect GCM predictions, such as climate sensitivity. Predictions are hampered by the large range of scales of interaction between various components that need to be captured. Observation systems (remote sensing, in situ) are increasingly being used to constrain predictions, but significant challenges exist, to some extent because of the large range of scales and the fact that the various measuring systems tend to address different scales. Fine-scale models represent clouds, aerosols, and aerosol–cloud interactions with high fidelity but do not include interactions with the larger scale and are therefore limited from a climatic point of view. We suggest strategies for improving estimates of aerosol–cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.
Biomass burning is a major source of atmospheric particulate matter (PM) with impacts on health, climate, and air quality. The particles and vapors within biomass burning plumes undergo chemical and ...physical aging as they are transported downwind. Field measurements of the evolution of PM with plume age range from net decreases to net increases, with most showing little to no change. In contrast, laboratory studies tend to show significant mass increases on average. On the other hand, similar effects of aging on the average PM composition (e.g., oxygen-to-carbon ratio) are reported for lab and field studies. Currently, there is no consensus on the mechanisms that lead to these observed similarities and differences. This review summarizes available observations of aging-related biomass burning aerosol mass concentrations and composition markers, and discusses four broad hypotheses to explain variability within and between field and laboratory campaigns: (1) variability in emissions and chemistry, (2) differences in dilution/entrainment, (3) losses in chambers and lines, and (4) differences in the timing of the initial measurement, the baseline from which changes are estimated. We conclude with a concise set of research needs for advancing our understanding of the aging of biomass burning aerosol.
The evolution of organic aerosol (OA) and brown carbon (BrC) in wildfire plumes, including the relative contributions of primary versus secondary sources, has been uncertain in part because of ...limited knowledge of the precursor emissions and the chemical environment of smoke plumes. We made airborne measurements of a suite of reactive trace gases, particle composition, and optical properties in fresh western US wildfire smoke in July through August 2018. We use these observations to quantify primary versus secondary sources of biomass-burning OA (BBPOA versus BBSOA) and BrC in wildfire plumes. When a daytime wildfire plume dilutes by a factor of 5 to 10, we estimate that up to one-third of the primary OA has evaporated and subsequently reacted to form BBSOA with near unit yield. The reactions of measured BBSOA precursors contribute only 13 ± 3% of the total BBSOA source, with evaporated BBPOA comprising the rest. We find that oxidation of phenolic compounds contributes the majority of BBSOA from emitted vapors. The corresponding particulate nitrophenolic compounds are estimated to explain 29 ± 15% of average BrC light absorption at 405 nm (BrC Abs405) measured in the first few hours of plume evolution, despite accounting for just 4 ± 2% of average OA mass. These measurements provide quantitative constraints on the role of dilution-driven evaporation of OA and subsequent radical-driven oxidation on the fate of biomass-burning OA and BrC in daytime wildfire plumes and point to the need to understand how processing of nighttime emissions differs.
Microorganisms are ubiquitous and highly diverse in the atmosphere. Despite the potential impacts of airborne bacteria found in the lower atmosphere over the Southern Ocean (SO) on the ecology of ...Antarctica and on marine cloud phase, no previous region-wide assessment of bioaerosols over the SO has been reported. We conducted bacterial profiling of boundary layer shipboard aerosol samples obtained during an Austral summer research voyage, spanning 42.8 to 66.5°S. Contrary to findings over global subtropical regions and the Northern Hemisphere, where transport of microorganisms from continents often controls airborne communities, the great majority of the bacteria detected in our samples were marine, based on taxonomy, back trajectories, and source tracking analysis. Further, the beta diversity of airborne bacterial communities varied with latitude and temperature, but not with other meteorological variables. Limited meridional airborne transport restricts southward community dispersal, isolating Antarctica and inhibiting microorganism and nutrient deposition from lower latitudes to these same regions. A consequence and implication for this region’s marine boundary layer and the clouds that overtop it is that it is truly pristine, free from continental and anthropogenic influences, with the ocean as the dominant source controlling low-level concentrations of cloud condensation nuclei and ice nucleating particles.
In order to study airborne bacterial community dynamics over Tokyo, including fine-scale correlations between airborne microorganisms and meteorological conditions, and the influence of local versus ...long-range transport of microbes, air samples were collected on filters for periods ranging from 48 to 72 h. The diversity of the microbial community was assessed by next generation sequencing. Predicted source regions of airborne particles, from back trajectory analyses, changed abruptly from the Pacific Ocean to the Eurasian Continent in the beginning of October. However, the microbial community composition and the alpha and beta diversities were not affected by this shift in meteorological regime, suggesting that long-range transport from oceanic or continental sources was not the principal determinant controlling the local airborne microbiome. By contrast, we found a significant correlation between the local meteorology, especially relative humidity and wind speed, and both alpha diversity and beta diversity. Among four potential local source categories (soil, bay seawater, river, and pond), bay seawater and soil were identified as constant and predominant sources. Statistical analyses point toward humidity as the most influential meteorological factor, most likely because it is correlated with soil moisture and hence negatively correlated with the dispersal of particles from the land surface. In this study, we have demonstrated the benefits of fine-scale temporal analyses for understanding the sources and relationships with the meteorology of Tokyo's "aerobiome."
Despite increasing incidence of wildfires in the United States, wildfire smoke is poorly characterized, with little known about particle composition and emission rates. Chemistry in transported ...plumes confounds interpretation of ground and aircraft data, but near-field observations can potentially disentangle the effects of oxidation and dilution on aerosol mass and chemical composition. We report the organic aerosol (OA) emission ratios from aircraft observations near the fire source for the 20 wildfires sampled during the Western Wildfire Experiment: Cloud Chemistry, Aerosol Absorption, and Nitrogen (WE-CAN) study of summer 2018. We observe no changes in submicron nonrefractory OA mass concentration, relative to CO which accounts for simple dilution, between 0.5 and up to 8 h of aging. However, static OA excess mixing ratios hide shifts in the aerosol chemical composition that suggest near-balanced, simultaneous oxidation-driven condensation and dilution-driven evaporation. Specifically, we observe significant increases in the extent of oxidation, evident by an increase in oxidation marker f44 and loss of the biomass burning marker f60, as the smoke ages through chemistry and dilution. We discuss the competing effects of oxidative chemistry and dilution-driven evaporation on the evolution of the chemical composition of aerosols in wildfire smoke over time.
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