Aerosol Emissions Research Articles

Effect of industrialization on the differences in sources and composition of ambient PM2.5 in two Southern Ontario locations

PM2.5 was sampled over a seven-year period (2013–2019) at two locations ∼50 km apart in Southern Ontario (concurrently for five years: 2015–2019). One is a heavily industrialized site (Hamilton), while the other was a rural site (Simcoe). To assess the impact of industrialization on the composition and sources of PM affecting air quality in these two locations, positive matrix factorization coupled with dispersion normalization (DN-PMF) was used to identify six and eight factors at Simcoe and Hamilton, respectively. The Simcoe factors in order of diminishing PM mass contribution were: particulate sulphate (pSO4), secondary organic aerosol (SOA), crustal matter, particulate nitrate (pNO3), biomass burning, and vehicular emissions. At Hamilton, the effects of industrialization were observed by the ∼36% higher average ambient PM2.5 concentration for the study period as well as the presence of factors unique to metallurgy, i.e., coking and steelmaking, compared to Simcoe. The coking and steelmaking factors contributed ∼15% to the PM mass at Hamilton. Seasonal variants of appropriate nonparametric trend tests with the associated slopes (Sen's) were used to assess statistically significant changes in the factor contributions to PM2.5 over time. Specifically at Hamilton, a significant decline in PM contributions was noted for coking (−0.03 μg/m³/yr or −4.1%/yr) while steelmaking showed no statistically significant decline over the study period. Other factors at Hamilton that showed statistically significant declines over the study period were: pSO4 (−0.27 μg/m³/yr or −12.6%/yr), biomass burning (−0.05 μg/m³/yr or −9.02%/yr), crustal matter (−0.03 μg/m³/yr or −5.28%/yr). These factors mainly accounted for the significant decline in PM2.5 over the study period (−0.35 μg/m³/yr or −4.24%/yr). This work shows the importance of long-term monitoring in assessing the unique contributions and temporal changes of industrialization on air quality in Ontario and similarly affected locations.

Aerosol Emissions from Heated Tobacco Products: A Review Focusing on Carbonyls, Analytical Methods, and Experimental Quality.

We provide an extensive review of 17 independent and industry-funded studies targeting carbonyls in aerosol emissions of Heated Tobacco Products (HTPs), focusing on quality criteria based on the reproducibility of experiments, appropriate analytic methods, and puffing regimes. Most revised studies complied with these requirements, but some were unreproducible, while others failed to consider analytical variables that may have affected the results and/or produced unrealistic comparisons. We also provide a review of the literature on the physicochemical properties of heated tobacco and HTP aerosols, as well as the evaluation of HTPs by regulatory agencies, addressing various critiques of their relative safety profile. The outcomes from the revised studies and regulatory evaluations tend to agree with and converge to a general consensus that HTP aerosols expose users to significantly lower levels of toxicity than tobacco smoke.

Primary and Secondary Organic Aerosol Formation from Asphalt Pavements.

Asphalt is ubiquitous across cities and a source of organic compounds spanning a wide range of volatility and may be an overlooked source of urban organic aerosols. The emission rate and composition depend strongly on temperature, but emissions have been observed at both application temperatures and surface temperatures during warm sunny days. Here we report primary organic aerosol (POA) emissions and secondary organic aerosol (SOA) production from asphalt. We reheated real-world asphalt samples to application-relevant temperatures (∼130 °C) and typical summertime road-surface temperatures (∼55 °C) and then flushed the emitted vapors into an environmental oxidation chamber containing ammonium sulfate seed particles. SOA was then formed following the photo-oxidation of emissions under high-NOx conditions typical of urban atmospheres. We find that POA only forms at application temperature as it does not require further oxidation, whereas SOA forms under both conditions; with the resulting POA and SOA both being semi-volatile. While total OA formation rates were substantially greater under the limited time spent under application conditions, SOA formation from passive asphalt heating presents a potential long-term source, as heating continues for the lifetime of the road surface. This suggests that persistent asphalt solar heating is likely a considerable and continued source of summertime SOA in urban environments.

Amplified Interhemispheric Rainfall Contrast in Boreal Summer Due To Reduction in Anthropogenic Emissions Under COVID‐MIP Green Economic‐Recovery Scenarios

AbstractOur study looks at the precipitation responses to two possible future emission‐mitigation pathways, pushed by the Coronavirus Disease 2019 pandemic (COVID‐19) and achieving carbon neutrality in the mid‐21st century. We find that a simultaneous‐reduction in well‐mixed greenhouse gases (WMGHGs) and anthropogenic aerosol emissions results in an enhanced interhemispheric precipitation contrast in the 2040s by amplifying the interhemispheric thermal contrast and strengthening the meridional overturning circulation in the tropics. Reduced aerosol emissions induce generally‐increased precipitation in the Northern Hemisphere (NH) and an amplified intertropical rainfall contrast, while reduced WMGHG emissions dominate decrease in precipitation in the areas away from aerosol emission sources. Further, the above precipitation contrast will be enhanced under stronger emission‐mitigation pathways, mainly attributed to larger precipitation increases in the NH caused by reduced aerosols. More aggressive WMGHGs mitigation policies are necessary to counteract the aerosol‐induced warming in the NH, thereby mitigating the risk of regional drying or wetting due to the asymmetry in interhemispheric energy budgets.

Description and performance of a sectional aerosol microphysical model in the Community Earth System Model (CESM2)

Abstract. We implemented the Community Aerosol and Radiation Model for Atmospheres (CARMA) in both the high- and low-top model versions of the Community Earth System Model Version 2 (CESM2). CARMA is a sectional microphysical model, which we use for aerosol in both the troposphere and stratosphere. CARMA is fully coupled to chemistry, clouds, radiation, and transport routines in CESM2. This development enables the comparison of simulations with a sectional (CARMA) and a modal (MAM4) aerosol microphysical model in the same modeling framework. The new implementation of CARMA has been adopted from previous work, with some additions that align with the current CESM2 Modal Aerosol Model (MAM4) implementation. The main updates include an interactive secondary organic aerosol description in CARMA, using the volatility basis set (VBS) approach, updated wet removal, and the use of transient emissions of aerosols and trace gases. In addition, we implemented an alternative aerosol nucleation scheme in CARMA, which is also used in MAM4. Detailed comparisons of stratospheric aerosol properties after the Mount Pinatubo eruption reveal the importance of prescribing sulfur injections in a larger region rather than in a single column to better represent the observed evolution of aerosols. Both CARMA and MAM4 in CESM2 are able to represent stratospheric and tropospheric aerosol properties reasonably well when compared to observations. Several differences in the performance of the two aerosol models show, in general, an improved representation of aerosols when using the sectional aerosol model in CESM2. These include a better representation of the aerosol size distribution after the Mount Pinatubo volcanic eruption in CARMA compared to MAM4. MAM4 produces on average smaller aerosols and less removal than CARMA, which results in a larger total mass. Both CARMA and MAM4 reproduce the stratospheric aerosol optical depth (AOD) within the error bar of the observations between 2001 and 2020, except for recent larger volcanic eruptions that are overestimated by both model configurations. The CARMA background surface area density and aerosol size distribution in the stratosphere and troposphere compare well to observations, with some underestimation of the Aitken-mode size range. MAM4 shows shortcomings in reproducing coarse-mode aerosol distributions in the stratosphere and troposphere. This work outlines additional development needs for CESM2 CARMA to improve the model compared to observations in both the troposphere and stratosphere.

Impact of regional climate patterns on the biomass burning emissions and transport over Peninsular Southeast Asia, 2000-2019

The regional climate variability in peninsular Southeast Asia (PSEA) can influence springtime biomass burning (BB) aerosol emissions and associated transport patterns. To comprehend the interannual variation of regional climate and its impact on PSEA BB, a diagnostic analysis based on the Modern-Era Retrospective Analysis for Research and Applications version 2 (MERRA-2) dataset and Moderate Resolution Imaging Spectroradiometer (MODIS) observations from 2000 to 2019 has presented. Employing principal component, composite, and correlation analyses, this study identified four climatic factors governing the emission and transport of PSEA BB aerosols: (i) a low-level anticyclone (suppressed monsoon trough) in the Bay of Bengal, (ii) the relative strength of the anticyclone over the South China Sea, (iii) the Pacific subtropical high, and (iv) low-level westerlies from PSEA to Taiwan. Additionally, BB emissions and transport significantly correlate with the El Niño-Southern Oscillation (ENSO). In the El Niño year, increased anticyclones in the Bay of Bengal and South China Sea accompanied the stronger westerlies, which enhanced BB aerosol emission and transport. The diagnostic results of this study can contribute to a better understanding and improved model simulations of aerosol-climate interactions in South and Southeast Asian monsoon regions.

Changes in biogenic volatile organic compound emissions in response to the El Niño–Southern Oscillation

Abstract. Emissions of biogenic volatile organic compounds (BVOCs) from the terrestrial biosphere play a significant role in major atmospheric processes. BVOCs are highly reactive compounds that influence the atmosphere's oxidation capacity and also serve as precursors for the formation of aerosols that influence global radiation budgets. Emissions depend on the response of vegetation to atmospheric conditions (primarily temperature and light), as well as other stresses, e.g. from droughts and herbivory. The El Niño–Southern Oscillation (ENSO) is a naturally occurring cycle arising from anomalies in the sea surface temperature (SST) in the tropical Pacific. ENSO perturbs the natural seasonality of weather systems on both global and regional scales and is considered the most significant driver of climate variability. Several studies have evaluated the sensitivity of BVOC fluxes during ENSO events using historical transient simulations. While this approach employs realistic scenarios, it is difficult to assess the impact of ENSO alone given the multiple types of climate forcing, e.g. from anthropogenic emissions of CO2 and aerosol. In this study, a global atmospheric chemistry–climate model with enabled interactive vegetation was used to conduct two sets of simulations: (1) isolated ENSO event simulations, in which a single ENSO event is used to perturb otherwise baseline conditions, and (2) sustained ENSO simulations, in which the same ENSO conditions are reproduced for an extended period of time. From the isolated ENSO events, we present global and regional BVOC emission changes resulting from the immediate response of vegetation to atmospheric states. More focus is given to the sustained ENSO simulations, which have the benefit of reducing the internal variability for more robust statistics when linking atmospheric and vegetation variables with BVOC flux anomalies. Additionally, these simulations explore long-term changes in the biosphere with potential shifts in vegetation in this possible climate mode, accounting for the prospect of increased intensity and frequency of ENSO with climate change. Our results show that strong El Niño events increase global isoprene emission fluxes by 2.9 % and that one single ENSO event perturbs the Earth system so markedly that BVOC emission fluxes do not return to baseline emissions within several years after the event. We show that persistent ENSO conditions shift the vegetation to a new quasi-equilibrium state, leading to an amplification of BVOC emission changes with up to a 19 % increase in isoprene fluxes over the Amazon. We provide evidence that BVOC-induced changes in plant phenology, such as the leaf area index (LAI), have a significant influence on BVOC emissions in the sustained ENSO climate mode.

Assessment of isoprene and near-surface ozone sensitivities to water stress over the Euro-Mediterranean region

Abstract. Plants emit biogenic volatile organic compounds (BVOCs) in response to changes in environmental conditions (e.g. temperature, radiation, soil moisture). In the large family of BVOCs, isoprene is by far the strongest emitted compound and plays an important role in ozone chemistry, thus affecting both air quality and climate. In turn, climate change may alter isoprene emissions by increasing temperature as well as the occurrence and intensity of severe water stresses that alter plant functioning. The Model of Emissions of Gases and Aerosols from Nature (MEGAN) provides different parameterizations to account for the impact of water stress on isoprene emissions, which essentially reduces emissions in response to the effect of soil moisture deficit on plant productivity. By applying the regional climate–chemistry model RegCM4chem coupled to the Community Land Model CLM4.5 and MEGAN2.1, we thus performed sensitivity simulations to assess the effects of water stress on isoprene emissions and near-surface ozone levels over the Euro-Mediterranean region and across the drier and wetter summers over the 1992–2016 period using two different parameterizations of the impact of water stress implemented in the MEGAN model. Over the Euro-Mediterranean region and across the simulated summers, water stress reduces isoprene emissions on average by nearly 6 %. However, during the warmest and driest selected summers (e.g. 2003, 2010, 2015) and over large isoprene-source areas (e.g. the Balkans), decreases in isoprene emissions range from −20 % to −60 % and co-occur with negative anomalies in precipitation, soil moisture and plant productivity. Sustained decreases in isoprene emissions also occur after prolonged or repeated dry anomalies, as observed for the summers of 2010 and 2012. Although the decrease in isoprene emissions due to water stress may be important, it only reduces near-surface ozone levels by a few percent due to a dominant VOC-limited regime over southern Europe and the Mediterranean Basin. Overall, over the selected analysis region, compared to the old MEGAN parameterization, the new one leads to localized and 25 %–50 % smaller decreases in isoprene emissions and 3 %–8 % smaller reductions in near-surface ozone levels.

Comparing respiratory aerosol emissions between children and adults during sustained phonation

Comparing respiratory aerosol emissions between children and adults during sustained phonation

Emission characteristics of biogenic volatile organic compounds in a subtropical pristine forest of southern China

Emission characteristics of biogenic volatile organic compounds (BVOCs) from dominant tree species in the subtropical pristine forests of China are extremely limited. Here we conducted in situ field measurements of BVOCs emissions from representative mature evergreen trees by using dynamic branch enclosures at four altitude gradients (600–1690 m a.s.l.) in the Nanling Mountains of southern China. Composition characteristics as well as seasonal and altitudinal variations were analyzed. Standardized emission rates and canopy-scale emission factors were then calculated. Results showed that BVOCs emission intensities in the wet season were generally higher than those in the dry season. Monoterpenes were the dominant BVOCs emitted from most broad-leaved trees, accounting for over 70% of the total. Schima superba, Yushania basihirsuta and Altingia chinensis had relatively high emission intensities and secondary pollutant formation potentials. The localized emission factors of isoprene were comparable to the defaults in the Model of Emissions of Gases and Aerosols from Nature (MEGAN), while emission factors of monoterpenes and sesquiterpenes were 2 to 58 times of those in the model. Our results can be used to update the current BVOCs emission inventory in MEGAN, thereby reducing the uncertainties of BVOCs emission estimations in forested regions of southern China.

Char dominates black carbon aerosol emission and its historic reduction in China

Emission factors and inventories of black carbon (BC) aerosols are crucial for estimating their adverse atmospheric effect. However, it is imperative to separate BC emissions into char and soot subgroups due to their significantly different physicochemical properties and potential effects. Here, we present a substantial dataset of char and soot emission factors derived from field and laboratory measurements. Based on the latest results of the char-to-soot ratio, we further reconstructed the emission inventories of char and soot for the years 1960–2017 in China. Our findings indicate that char dominates annual BC emissions and its huge historical reduction, which can be attributable to the rapid changes in energy structure, combustion technology and emission standards in recent decades. Our results suggest that further BC emission reductions in both China and the world should focus on char, which mainly derives from lower-temperature combustion and is easier to decrease compared to soot.

Precipitation regime changes in High Mountain Asia driven by cleaner air.

High Mountain Asia (HMA) has experienced a spatial imbalance in water resources in recent decades, partly because of a dipolar pattern of precipitation changes known as South Drying-North Wetting1. These changes can be influenced by both human activities and internal climate variability2,3. Although climate projections indicate a future widespread wetting trend over HMA1,4, the timing and mechanism of the transition from a dipolar to a monopolar pattern remain unknown. Here we demonstrate that the observed dipolar precipitation change in HMA during summer is primarily driven by westerly- and monsoon-associated precipitation patterns. The weakening of the Asian westerly jet, caused by the uneven emission of anthropogenic aerosols, favoured a dipolar precipitation trend from 1951 to 2020. Moreover, the phase transition of the Interdecadal Pacific Oscillation induces an out-of-phase precipitation change between the core region of the South Asian monsoon and southeastern HMA. Under medium- or high-emission scenarios, corresponding to a global warming of 0.6-1.1 °C compared with the present, the dipolar pattern is projected to shift to a monopolar wetting trend in the 2040s. This shift in precipitation patterns is mainly attributed to the intensified jet stream resulting from reduced emissions of anthropogenic aerosols. These findings underscore the importance of considering the impact of aerosol emission reduction in future social planning by policymakers.

Predictable decadal forcing of the North Atlantic jet speed by sub-polar North Atlantic sea surface temperatures

Abstract. It has been demonstrated that decadal variations in the North Atlantic Oscillation (NAO) can be predicted by current forecast models. While Atlantic Multidecadal Variability (AMV) in sea surface temperatures (SSTs) has been hypothesised as the source of this skill, the validity of this hypothesis and the pathways involved remain unclear. We show, using reanalysis and data from two forecast models, that the decadal predictability of the NAO can be entirely accounted for by the predictability of decadal variations in the speed of the North Atlantic eddy-driven jet, with no predictability of decadal variations in the jet latitude. The sub-polar North Atlantic (SPNA) is identified as the only obvious common source of an SST-based signal across the models and reanalysis, and the predictability of the jet speed is shown to be consistent with a forcing from the SPNA visible already within a single season. The pathway is argued to be tropospheric in nature, with the SPNA-associated heating extending up to the mid-troposphere, which alters the meridional temperature gradient around the climatological jet core. The relative roles of anthropogenic aerosol emissions and the Atlantic Meridional Overturning Circulation (AMOC) at generating predictable SPNA variability are also discussed. The analysis is extensively supported by the novel use of a set of seasonal hindcasts spanning the 20th century and forced with prescribed SSTs.

Rapid saturation of cloud water adjustments to shipping emissions

Abstract. Human aerosol emissions change cloud properties by providing additional cloud condensation nuclei. This increases cloud droplet numbers, which in turn affects other cloud properties like liquid-water content and ultimately cloud albedo. These adjustments are poorly constrained, making aerosol effects the most uncertain part of anthropogenic climate forcing. Here we show that cloud droplet number and water content react differently to changing emission amounts in shipping exhausts. We use information about ship positions and modeled emission amounts together with reanalysis winds and satellite retrievals of cloud properties. The analysis reveals that cloud droplet numbers respond linearly to emission amount over a large range (1–10 kg h−1) before the response saturates. Liquid water increases in raining clouds, and the anomalies are constant over the emission ranges observed. There is evidence that this independence of emissions is due to compensating effects under drier and more humid conditions, consistent with suppression of rain by enhanced aerosol. This has implications for our understanding of cloud processes and may improve the way clouds are represented in climate models, in particular by changing parameterizations of liquid-water responses to aerosol.

Climate responses in China to domestic and foreign aerosol changes due to clean air actions during 2013–2019

In recent years, to improve air quality, significant efforts have been made to reduce regional aerosols including China, Europe and North America, which have potential impacts on climate. In this study, fast and slow climate responses in China to changes in domestic and foreign anthropogenic emissions of aerosols and precursors from 2013 to 2019 are investigated using the Community Earth System Model version 1 (CESM1). Aerosol emissions changes, especially reductions in China, North America and Europe, during 2013–2019 resulted in surface air temperature increases across the Northern Hemisphere. Global aerosol changes induce a regional warming of 0.2 °C in China, equally contributed by domestic and foreign emissions changes. China’s domestic emission reductions lead to a regional average temperature rise of 0.1°C, primarily driven by rapid atmospheric adjustments over eastern China. Foreign aerosol changes, particularly reductions in North America and Europe, also contributed to a 0.1°C warming in China through slow oceanic processes. This warming in China induced by foreign aerosol changes is due to a teleconnection between the aerosol-induced anomalous regional warming in Eastern U.S.-North Atlantic Ocean-Europe and the downstream East Asian climate through anomalous wave trains propagation. The comparable influence of domestic and foreign aerosol changes on climate in China underscores the importance of international collaboration in climate mitigation endeavors.

Technical note: In situ measurements and modelling of the oxidation kinetics in films of a cooking aerosol proxy using a quartz crystal microbalance with dissipation monitoring (QCM-D)

Abstract. Aerosols and films are found in indoor and outdoor environments. How they interact with pollutants, such as ozone, has a direct impact on our environment via cloud droplet formation and the chemical persistence of toxic aerosol constituents. The chemical reactivity of aerosol emissions is typically measured spectroscopically or by techniques such as mass spectrometry, directly monitoring the amount of material during a chemical reaction. We present a study which indirectly measures oxidation kinetics in a common cooking aerosol proxy using a low-cost quartz crystal microbalance with dissipation monitoring (QCM-D). We validated this approach by comparison with kinetics measured both spectroscopically and with high-intensity synchrotron radiation. Using microscopy, we found that the film morphology changed and film rigidity increased during oxidation. There was evidence of surface crust formation on oxidised particles, though this was not consistent for all experiments. Crucially, our kinetic modelling of these experimental data confirmed that the oleic acid decay rate is in line with previous literature determinations, which demonstrates that performing such experiments on a QCM-D does not alter the underlying mechanism. There is clear potential to take this robust and low-cost but sensitive method to the field for in situ monitoring of reactions outdoors and indoors.

Changes in the Global Climate: Atmospheric Angular Momentum and Pacific Ocean Temperatures

Abstract Atmospheric angular momentum (AAM) is used to study the variability of Earth’s atmospheric circulation during the past 45 years, a time of considerable climate change. Using global AAM, two interdecadal states are defined covering the periods 1977–98 (hereinafter P1) and 1999–2022 (P2). Global AAM decreased from P1 to P2 and was accompanied by weakened subtropical jet streams in both hemispheres, strong convection around the northern Maritime Continent, and a strengthened sea surface temperature (SST) gradient across the tropical Pacific Ocean. The period differences project onto 1) internal interdecadal Pacific variability (IPV), 2) a postulated transient ocean thermostat response to greenhouse gas and aerosol emissions, and 3) circulation anomalies related to the ozone hole. During 1977–2023, the first two processes are forcing the climate toward larger Pacific Ocean SST gradients and a poleward expansion of the Indo-Pacific warm pool (IPWP), especially into the Northern Hemisphere. The ozone hole produces its own distinct pattern of anomalies in the Southern Hemisphere that tend to become persistent in the early 1990s. The zonal and vertical mean AAM variations during P1 have frequent westerly wind anomalies between 40°N and 40°S with poleward propagation on interannual time scales. During P2, the circulation is dominated by subtropical easterly wind anomalies, poleward-shifted jets, and weaker propagation. Locally, the zonal mean anomalies manifest as midlatitude ridges that lead to continental droughts. Case studies illustrate the weakened subtropical jet streams of P2 and examine the factors behind a transition to La Niña in early 2020 that maintains the P2 pattern.

Seasonal differences in continental outflows and marine emissions of organic aerosols in the East China Sea: Insight from the variation of saccharides

Water-soluble organic species play an important role in cloud condensation nuclei and cloud formation in marine atmosphere. The present study investigated the influence of continental outflows and marine biogenic emission on organic aerosol in the East China Sea from the perspective of saccharides during a cold season and a warm season in 2019, respectively. Driven by the East Asian continental outflows during the cold season, levoglucosan emitted from biomass burning were the dominant species and were mostly concentrated in fine mode (<2.5 μm). Biogenic species, including primary sugars and sugar alcohols, were the dominant species in warm season, accounting for a high fraction of WSOC with 5.48 ± 3.29%, and were mostly distributed in coarse mode (2.5–10 μm). This trend was consistent with sea salt components (Na+ and Cl−) when air masses originated from oceanic areas, suggesting that marine emissions could be the major sources of saccharides during the warm season. Particularly, a dramatic increase in biogenic saccharides (glucose, sucrose, mannitol and arabitol) was observed when experienced the “Super Typhoon Lekima”. Concentrations of these species were 2 to 5 times higher than that in normal days, illustrating the significant impact of extreme weather events on the emissions of biogenic aerosols in marine area. This study improves the understanding of combined impacts of continental outflows and marine emissions on water-soluble organic species in the East China Sea, again highlighting the important contribution of marine biogenic emissions under extreme weather conditions.

Substantially positive contributions of new particle formation to cloud condensation nuclei under low supersaturation in China based on numerical model improvements

Abstract. New particle formation (NPF) and subsequent particle growth are important sources of condensation nuclei (CN) and cloud condensation nuclei (CCN). While many observations have shown positive contributions of NPF to CCN at low supersaturation, negative NPF contributions were often simulated in polluted environments. Using the observations in a coastal city of Qingdao, Beijing, and Gucheng in north China, we thoroughly evaluate the simulated number concentrations of CN and CCN using an NPF-explicit parameterization embedded in the WRF-Chem model. For CN, the initial simulation shows large biases of particle number concentrations at 10–40 and 40–100 nm. By adjusting the process of gas–particle partitioning, including the mass accommodation coefficient (MAC) of sulfuric acid, the phase changes in primary organic aerosol emissions, and the condensational amount of nitric acid, the improvement of the particle growth process yields substantially reduced overestimation of CN. Regarding CCN, secondary organic aerosol (SOA) formed from the oxidation of semi-volatile and intermediate-volatility organic compounds (S/IVOCs) is called SI-SOA, the yield of which is an important contributor. At default settings, the SI-SOA yield is too high without considering the differences in precursor oxidation rates. Lowering the SI-SOA yield under linear H2SO4 nucleation scheme results in much-improved CCN simulations compared to observations. On the basis of the bias-corrected model, we find substantially positive contributions of NPF to CCN at low supersaturation (∼ 0.2 %) over broad areas of China, primarily due to competing effects of increasing particle hygroscopicity, a result of reductions in SI-SOA amount, surpassing that of particle size decreases. The bias-corrected model is robustly applicable to other schemes, such as the quadratic H2SO4 nucleation scheme, in terms of CN and CCN, though the dependence of CCN on SI-SOA yield is diminished likely due to changes in particle composition. This study highlights potentially much larger NPF contributions to CCN on a regional and even global basis.

Isolating the effect of biomass burning aerosol emissions on 20th century hydroclimate in South America and Southeast Asia

Biomass burning is a significant source of aerosol emissions in some regions and has a considerable impact on regional climate. Earth system model simulations indicate that increased biomass burning aerosol emissions contributed to statistically significant decreases in tropical precipitation over the 20th century. In this study, we use the Community Earth System Model version 1 Large Ensemble (CESM1-LENS) experiment to evaluate the mechanisms by which biomass burning aerosol contributed to decreased tropical precipitation, with a focus on South America and Southeast Asia. We analyze the all-but-one forcing simulations in which biomass burning aerosol emissions are held constant while other forcings (e.g., greenhouse gas concentrations) vary throughout the 20th century. This allows us to isolate the influence of biomass burning aerosol on processes that contribute to decreasing precipitation, including cloud microphysics, the radiative effects of absorbing aerosol particles, and alterations in regional circulation. We also show that the 20th century reduction in precipitation identified in the CESM1-LENS historical and biomass burning experiments is consistent across Coupled Model Intercomparison Project Phase 5 models with interactive aerosol schemes and the CESM2 single-forcing experiment. Our results demonstrate that higher concentrations of biomass burning aerosol increases the quantity of cloud condensation nuclei and cloud droplets, limiting cloud droplet size and precipitation formation. Additionally, absorbing aerosols (e.g., black carbon) contribute to a warmer cloud layer, which promotes cloud evaporation, increases atmospheric stability, and alters regional circulation patterns. Corresponding convectively coupled circulation responses, particularly over the tropical Andes, contribute to further reducing the flow of moisture and moisture convergence over tropical land. These results elucidate the processes that affect the water cycle in regions prone to biomass burning and inform our understanding of how future changes in aerosol emissions may impact tropical precipitation over the 21st century.