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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.

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.

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.

The Arctic is warming at a rapid rate, with implications for microbial communities as the ecosystems change. Some microbes and biogenic materials can affect the persistence of long-lived mixed-phase clouds by serving as ice nucleating particles (INPs). The presence of INPs modulates the cloud phase, and long-term measurements are important to elucidate their seasonal sources and to predict future change. The Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition in 2019–2020 provided the first year-long measurements of bioaerosols and INPs in the central Arctic, with 3 d filters for amplicon sequencing and cumulative INP concentrations from −5 to −30 °C. Here, we investigated the INP seasonal cycle and its relation to the seasonal cycle of bacteria and eukaryotes. INPs were greatly elevated and compositionally similar in summer, aligning with a greater prevalence of local bioaerosol sources, but, despite this, a diverse mixture of sources (marine and terrestrial) was present all times. A common broader Arctic INP population is hypothesized for much of the year by comparable coincident data collected in Svalbard and a sensitivity of both the INPs and bioaerosols to large-scale events.

Black carbon (BC) aerosol plays an important role in the Earth’s climate system because it absorbs solar radiation and therefore potentially warms the climate; however, BC can also act as a seed for cloud particles, which may offset much of its warming potential. If BC acts as an ice nucleating particle (INP), BC could affect the lifetime, albedo, and radiative properties of clouds containing both supercooled liquid water droplets and ice particles (mixed-phase clouds). Over 40% of global BC emissions are from biomass burning; however, the ability of biomass burning BC to act as an INP in mixed-phase cloud conditions is almost entirely unconstrained. To provide these observational constraints, we measured the contribution of BC to INP concentrations ([INP]) in real-world prescribed burns and wildfires. We found that BC contributes, at most, 10% to [INP] during these burns. From this, we developed a parameterization for biomass burning BC and combined it with a BC parameterization previously used for fossil fuel emissions. Applying these parameterizations to global model output, we find that the contribution of BC to potential [INP] relevant to mixed-phase clouds is ∼5% on a global average.

Agricultural activities can modify natural ecosystems and change the nature of the aerosols emitted from those landscapes. The harvesting of crops can loft plant fragments and soil dust into the atmosphere that can travel long distances and interact with clouds far from their sources. In this way harvesting may contribute substantially to ice-nucleating particle (INP) concentrations, especially in regions where agriculture makes up a large percentage of land use. However, a full characterization of particles emitted during harvesting has not been reported. This study characterizes immersion mode INPs emitted during harvesting of several crops in the High Plains region of the United States. The Colorado State University Continuous Flow Diffusion Chamber (CFDC) and the Ice Spectrometer (IS) were utilized to measure INP concentrations during active harvesting of four crops in Kansas and Wyoming. Large spikes of INPs were observed during harvesting, with concentrations over 200 L−1 at −30 °C measured during a wheat harvest. To differentiate between mineral and organic components, a novel heating tube method was employed in real time upstream of the CFDC to deactivate organic INPs in situ. The results indicate that harvesting produces a complex mixture of organic, soil dust, and mineral components that varies for different crops. Electron microscopy analysis showed that while mineral components made up a large proportion of INPs, organic components comprised over 40 % of measured INPs for certain crops at warm temperatures. Heating and enzyme post-treatment of aerosol samples collected for IS processing indicated that bacteria and heat-labile and heat-stable organics contributed to wheat harvest-produced INPs. These results indicate that plant material and organic particles are a significant component of harvest INPs and their impacts on ice formation in clouds and precipitation on a regional scale should be explored.

Rapid Arctic climate warming, amplified relative to lower-latitude regions, has led to permafrost thaw and associated thermokarst processes. Recent work has shown permafrost is a rich source of ice-nucleating particles (INPs) that can initiate ice formation in supercooled liquid clouds. Since the phase of Arctic clouds strongly affects the surface energy budget, especially over ice-laden surfaces, characterizing INP sources in this region is critical. For the first time, we provide a large-scale survey of potential INP sources in tundra terrain where thermokarst processes are active and relate to INPs in the air. Permafrost, seasonally thawed active layer, ice wedge, vegetation, water, and aerosol samples were collected near Utqiaġvik, Alaska, in late summer and analyzed for their INP contents. Permafrost was confirmed as a rich source of INPs that was enhanced near the coast. Sensitivity to heating revealed differences in INPs from similar sources, such as the permafrost and active layer. Water, vegetation, and ice wedge INPs had the highest heat-labile percentage. The aerosol likely contained a mixture of known and unsurveyed INP types that were inferred as biological. Arctic water bodies were shown to be potential important links of sources to the atmosphere in thermokarst regions. Therefore, a positive relationship found with total organic carbon considering all water bodies gives a mechanism for future parameterization as permafrost continues to thaw and drive regional landscape shifts.

Emission rates and properties of ice nucleating particles (INPs) are required for proper representation of aerosol–cloud interactions in atmospheric models. Few investigations have quantified marine INP emissions, a potentially important INP source for remote oceanic regions. Previous studies have suggested INPs in sea spray aerosol (SSA) are linked to oceanic biological activity. This proposed link was explored in this study by measuring INP emissions from nascent SSA during phytoplankton blooms during two mesocosm experiments. In a Marine Aerosol Reference Tank (MART) experiment, a phytoplankton bloom was produced with chlorophyll-a (Chl a) concentrations reaching 39 μg L−1, while Chl a concentrations more representative of natural ocean conditions were obtained during the Investigation into Marine Particle Chemistry and Transfer Science (IMPACTS; peak Chl a of 5 μg L−1) campaign, conducted in the University of California, San Diego, wave flume. Dynamic trends in INP emissions occurred for INPs active at temperatures > −30°C. Increases in INPs active between −25° and −15°C lagged the peak in Chl a in both studies, suggesting a consistent population of INPs associated with the collapse of phytoplankton blooms. Trends in INP emissions were also compared to aerosol composition, abundances of microbes, and enzyme activity. In general, increases in INP concentrations corresponded to increases in organic species in SSA and the emissions of heterotrophic bacteria, suggesting that both microbes and biomolecules contribute to marine INP populations. INP trends were not directly correlated with a single biological marker in either study. Direct measurements of INP chemistry are needed to accurately identify particles types contributing to marine INP populations.

Secondary organic aerosol (SOA) has been shown to form in biomass-burning emissions in laboratory and field studies. However, there is significant variability among studies in mass enhancement, which could be due to differences in fuels, fire conditions, dilution, and/or limitations of laboratory experiments and observations. This study focuses on understanding processes affecting biomass-burning SOA formation in laboratory smog-chamber experiments and in ambient plumes. Vapor wall losses have been demonstrated to be an important factor that can suppress SOA formation in laboratory studies of traditional SOA precursors; however, impacts of vapor wall losses on biomass-burning SOA have not yet been investigated. We use an aerosol-microphysical model that includes representations of volatility and oxidation chemistry to estimate the influence of vapor wall loss on SOA formation observed in the FLAME III smog-chamber studies. Our simulations with base-case assumptions for chemistry and wall loss predict a mean OA mass enhancement (the ratio of final to initial OA mass, corrected for particle-phase wall losses) of 1.8 across all experiments when vapor wall losses are modeled, roughly matching the mean observed enhancement during FLAME III. The mean OA enhancement increases to over 3 when vapor wall losses are turned off, implying that vapor wall losses reduce the apparent SOA formation. We find that this decrease in the apparent SOA formation due to vapor wall losses is robust across the ranges of uncertainties in the key model assumptions for wall-loss and mass-transfer coefficients and chemical mechanisms.We then apply similar assumptions regarding SOA formation chemistry and physics to smoke emitted into the atmosphere. In ambient plumes, the plume dilution rate impacts the organic partitioning between the gas and particle phases, which may impact the potential for SOA to form as well as the rate of SOA formation. We add Gaussian dispersion to our aerosol-microphysical model to estimate how SOA formation may vary under different ambient-plume conditions (e.g., fire size, emission mass flux, atmospheric stability). Smoke from small fires, such as typical prescribed burns, dilutes rapidly, which drives evaporation of organic vapor from the particle phase, leading to more effective SOA formation. Emissions from large fires, such as intense wildfires, dilute slowly, suppressing OA evaporation and subsequent SOA formation in the near field. We also demonstrate that different approaches to the calculation of OA enhancement in ambient plumes can lead to different conclusions regarding SOA formation. OA mass enhancement ratios of around 1 calculated using an inert tracer, such as black carbon or CO, have traditionally been interpreted as exhibiting little or no SOA formation; however, we show that SOA formation may have greatly contributed to the mass in these plumes.In comparison of laboratory and plume results, the possible inconsistency of OA enhancement between them could be in part attributed to the effect of chamber walls and plume dilution. Our results highlight that laboratory and field experiments that focus on the fuel and fire conditions also need to consider the effects of plume dilution or vapor losses to walls.

Understanding the drivers of airborne microbial community structure is essential for predicting microbial dispersal, ecosystem connectivity, and responses to environmental change. This study reveals that atmospheric fungal and bacterial communities are shaped by distinct ecological and environmental factors, with fungi exhibiting stronger site-specific responses and vertical stratification than bacteria. The contrasting patterns between subalpine forest and grassland ecosystems underscore how local conditions influence microbial diversity and transport potential. Importantly, the detection of shared taxa, especially at greater sampling heights, suggests that atmospheric transport may connect distant ecosystems and that certain taxa are ubiquitous. These findings highlight the complexity of the aerobiome and its sensitivity to spatial and temporal dynamics, providing new insights into microbial distribution and the role of the atmosphere in microbial exchange across landscapes.