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Australian mega-wildfires in the summer of 2019-2020 injected smoke into the stratosphere, causing strong ozone depletion in the lower stratosphere. Here, we model the smoke plume and reproduce its unexpected trajectory toward the middle stratosphere at ~35-kilometer altitude. We show that a smoke-charged vortex (SCV) induced and maintained by absorbing aerosols played a key role in lofting pollutants from the lower stratosphere and nearly doubled the southern hemispheric aerosol burden in the middle stratosphere. The SCV caused a redistribution of stratospheric aerosols, which boosted heterogeneous chemistry in the middle stratosphere and enhanced ozone production, compensating for up to 70% of the ozone depletion in the lower stratosphere. As global warming continues, we expect a growing frequency and importance of SCVs in promoting the impacts of wildfires on stratospheric aerosols and chemistry.

Abstract. The Amazon Basin is frequently influenced by transatlantic transport of African dust plumes during its wet season (January–April), which not only interrupts the near-pristine atmospheric condition in that season, but alsoprovides nutrient inputs to the Amazon rainforest upon deposition. In thisstudy, we use the chemical transport model GEOS-Chem to investigate theimpact of the export of African mineral dust to the Amazon Basin during theperiod of 2013–2017, constrained by multiple datasets obtained from theAErosol RObotic NETwork (AERONET), MODIS, as well as the Cayenne site and the Amazon Tall Tower Observatory (ATTO) site in the Amazon Basin. With an optimized particle mass size distribution (PMSD) of dust aerosols, the model captures observed aerosol optical depth (AOD) well in terms of both the mean value and the decline rate of the logarithm of AOD over the Atlantic Ocean along the transport path (AOaTP), implying consistency with the observed export efficiency of African dust along the transatlantic transport. With an annual emission of 0.73±0.12 Pg yr−1, African dust entering the Amazon Basin during the wet season accounts for 40±4.5 % (up to 70 %) of surface aerosol mass concentrations over the basin. Observed dust peaks over the Amazon Basin are generally associated with relatively higher African dust emissions (including the Sahara and the Sahel) and longer lifetimes of dust along the transatlantic transport, i.e., higher export efficiency of African dust across the Atlantic Ocean. The frequency of dust events during the wet season is around 18 % when averaged over the Amazon Basin, with maxima of over 60 % at the northeastern coast. During the dust events, AOD over most of the Amazon Basin is dominated by dust. Based on dust deposition, we further estimate annual inputs of 52±8.7, 0.97±0.16, and 21±3.6 mg m−2 yr−1 for iron, phosphorus, and magnesium, respectively, into the Amazon rainforest, which may to some extent compensate for the hydrologic losses of nutrients in the forest ecosystem.

Black carbon (BC) plays an important role in the climate system because of its strong warming effect, yet the magnitude of this effect is highly uncertain owing to the complex mixing state of aerosols. Here we build a unified theoretical framework to describe BC's mixing states, linking dynamic processes to BC coating thickness distribution, and show its self-similarity for sites in diverse environments. The size distribution of BC-containing particles is found to follow a universal law and is independent of BC core size. A new mixing state module is established based on this finding and successfully applied in global and regional models, which increases the accuracy of aerosol climate effect estimations. Our theoretical framework links observations with model simulations in both mixing state description and light absorption quantification.

AbstractSmoke from vegetation fires affects air quality, atmospheric cycling, and the climate in the Amazon rain forest. A major unknown has remained the quantity of long-range transported smoke from Africa in relation to local and regional fire emissions. Here we quantify the abundance, seasonality, and properties of African smoke in central Amazonia. We show that it accounts for ~ 60% of the black carbon concentrations during the wet season and ~ 30% during the dry season. The African smoke influences aerosol-radiation interactions across the entire Amazon, with the strongest impact on the vulnerable eastern basin, a hot spot of climate and land use change. Our findings further suggest that the direct influence of African smoke has been historically relevant for soil fertilization, the carbon and water cycles, and, thus, the development of the Amazon forest ecosystem, even in the pre-industrial era.

Abstract. Nucleation and condensation associated with biogenicvolatile organic compounds (BVOCs) are important aerosol formation pathways,yet their contribution to the upper-tropospheric aerosols remainsinconclusive, hindering the understanding of aerosol climate effects. Here,we develop new schemes describing these organic aerosol formation processesin the WRF-Chem model and investigate their impact on the abundance of cloudcondensation nuclei (CCN) in the upper troposphere (UT) over the AmazonBasin. We find that the new schemes significantly increase the simulated CCNnumber concentrations in the UT (e.g., up to ∼ 400 cm−3at 0.52 % supersaturation) and greatly improve the agreement with theaircraft observations. Organic condensation enhances the simulated CCNconcentration by 90 % through promoting particle growth, while organicnucleation, by replenishing new particles, contributes an additional 14 %.Deep convection determines the rate of these organic aerosol formationprocesses in the UT through controlling the upward transport of biogenicprecursors (i.e., BVOCs). This finding emphasizes the importance of thebiosphere–atmosphere coupling in regulating upper-tropospheric aerosolconcentrations over the tropical forest and calls for attention to itspotential role in anthropogenic climate change.

Airborne transmission by droplets and aerosols is important for the spread of viruses. Face masks are a well-established preventive measure, but their effectiveness for mitigating SARS-CoV-2 transmission is still under debate. We show that variations in mask efficacy can be explained by different regimes of virus abundance and related to population-average infection probability and reproduction number. For SARS-CoV-2, the viral load of infectious individuals can vary by orders of magnitude. We find that most environments and contacts are under conditions of low virus abundance (virus-limited) where surgical masks are effective at preventing virus spread. More advanced masks and other protective equipment are required in potentially virus-rich indoor environments including medical centers and hospitals. Masks are particularly effective in combination with other preventive measures like ventilation and distancing.

Low clouds play a key role in the Earth-atmosphere energy balance and influence agricultural production and solar-power generation. Smoke aloft has been found to enhance marine stratocumulus through aerosol-cloud interactions, but its role in regions with strong human activities and complex monsoon circulation remains unclear. Here we show that biomass burning aerosols aloft strongly increase the low cloud coverage over both land and ocean in subtropical southeastern Asia. The degree of this enhancement and its spatial extent are comparable to that in the Southeast Atlantic, even though the total biomass burning emissions in Southeast Asia are only one-fifth of those in Southern Africa. We find that a synergetic effect of aerosol-cloud-boundary layer interaction with the monsoon is the main reason for the strong semi-direct effect and enhanced low cloud formation in southeastern Asia.

Wildfires inject large amounts of black carbon (BC) particles into the atmosphere, which can reach the lowermost stratosphere (LMS) and cause strong radiative forcing. During a 14-month period of observations on board a passenger aircraft flying between Europe and North America, we found frequent and widespread biomass burning (BB) plumes, influencing 16 of 160 flight hours in the LMS. The average BC mass concentrations in these plumes (∼140 ng·m-3, standard temperature and pressure) were over 20 times higher than the background concentration (∼6 ng·m-3) with more than 100-fold enhanced peak values (up to ∼720 ng·m-3). In the LMS, nearly all BC particles were covered with a thick coating. The average mass equivalent diameter of the BC particle cores was ∼120 nm with a mean coating thickness of ∼150 nm in the BB plume and ∼90 nm with a coating of ∼125 nm in the background. In a BB plume that was encountered twice, we also found a high diameter growth rate of ∼1 nm·h-1 due to the BC particle coatings. The observed high concentrations and thick coatings of BC particles demonstrate that wildfires can induce strong local heating in the LMS and may have a significant influence on the regional radiative forcing of climate.

Polycyclic aromatic hydrocarbons like benzo(a)pyrene (BaP) in atmospheric particulate matter pose a threat to human health because of their high carcinogenicity. In the atmosphere, BaP is mainly degraded through a multiphase reaction with ozone, but the fate and atmospheric transport of BaP are poorly characterized. Earlier modeling studies used reaction rate coefficients determined in laboratory experiments at room temperature, which may overestimate/underestimate degradation rates when applied under atmospheric conditions. Moreover, the effects of diffusion on the particle bulk are not well constrained, leading to large discrepancies between model results and observations. We show how regional and global distributions and transport of BaP can be explained by a new kinetic scheme that provides a realistic description of the temperature and humidity dependence of phase state, diffusivity, and reactivity of BaP-containing particles. Low temperature and humidity can substantially increase the lifetime of BaP and enhance its atmospheric dispersion through both the planetary boundary layer and the free troposphere. The new scheme greatly improves the performance of multiscale models, leading to better agreement with observed BaP concentrations in both source regions and remote regions (Arctic), which cannot be achieved by less-elaborate degradation schemes (deviations by multiple orders of magnitude). Our results highlight the importance of considering temperature and humidity effects on both the phase state of aerosol particles and the chemical reactivity of particulate air pollutants.

Abstract. Polycyclic aromatic hydrocarbons (PAHs) are hazardous pollutants, with increasing emissions in pace with economic development in East Asia, but their distribution and fate in the atmosphere are not yet well understood. We extended the regional atmospheric chemistry model WRF-Chem (Weather Research Forecast model with Chemistry module) to comprehensively study the atmospheric distribution and the fate of low-concentration, slowly degrading semivolatile compounds. The WRF-Chem-PAH model reflects the state-of-the-art understanding of current PAHs studies with several new or updated features. It was applied for PAHs covering a wide range of volatility and hydrophobicity, i.e. phenanthrene, chrysene and benzo[a]pyrene, in East Asia. Temporally highly resolved PAH concentrations and particulate mass fractions were evaluated against observations. The WRF-Chem-PAH model is able to reasonably well simulate the concentration levels and particulate mass fractions of PAHs near the sources and at a remote outflow region of East Asia, in high spatial and temporal resolutions. Sensitivity study shows that the heterogeneous reaction with ozone and the homogeneous reaction with the nitrate radical significantly influence the fate and distributions of PAHs. The methods to implement new species and to correct the transport problems can be applied to other newly implemented species in WRF-Chem.

The allergenic potential of airborne proteins may be enhanced via post-translational modification induced by air pollutants like ozone (O3) and nitrogen dioxide (NO2). The molecular mechanisms and kinetics of the chemical modifications that enhance the allergenicity of proteins, however, are still not fully understood. Here, protein tyrosine nitration and oligomerization upon simultaneous exposure of O3 and NO2 were studied in coated-wall flow-tube and bulk solution experiments under varying atmospherically relevant conditions (5-200 ppb O3, 5-200 ppb NO2, 45-96% RH), using bovine serum albumin as a model protein. Generally, more tyrosine residues were found to react via the nitration pathway than via the oligomerization pathway. Depending on reaction conditions, oligomer mass fractions and nitration degrees were in the ranges of 2.5-25% and 0.5-7%, respectively. The experimental results were well reproduced by the kinetic multilayer model of aerosol surface and bulk chemistry (KM-SUB). The extent of nitration and oligomerization strongly depends on relative humidity (RH) due to moisture-induced phase transition of proteins, highlighting the importance of cloud processing conditions for accelerated protein chemistry. Dimeric and nitrated species were major products in the liquid phase, while protein oligomerization was observed to a greater extent for the solid and semi-solid phase states of proteins. Our results show that the rate of both processes was sensitive towards ambient ozone concentration, but rather insensitive towards different NO2 levels. An increase of tropospheric ozone concentrations in the Anthropocene may thus promote pro-allergic protein modifications and contribute to the observed increase of allergies over the past decades.

There are thousands of volatile organic compound (VOC) species in ambient air, while existing techniques can only detect a small part of them (approximately several hundred). The large number of unmeasured VOCs prevents us from understanding the photochemistry of ozone and aerosols in the atmosphere. The major sources and photochemical effects of these unmeasured VOCs in urban areas remain unclear. The missing VOC reactivity, which is defined as the total OH reactivity of the unmeasured VOCs, is a good indicator for constraining the photochemical effect of unmeasured VOCs. Here, we identified the dominant role of anthropogenic emission sources in the missing VOC reactivity (accounting for up to 70 %) by measuring missing VOC reactivity and tracer-based source analysis in a typical megacity in China. Omitting the missing VOC reactivity from anthropogenic emissions in model simulations will remarkably affect the diagnosis of sensitivity regimes for ozone formation, overestimating the degree of VOC-limited regimes by up to 46 %. Therefore, a thorough quantification of missing VOC reactivity from various anthropogenic emission sources is urgently needed for constraints of air quality models and the development of effective ozone control strategies. [ABSTRACT FROM AUTHOR]