One of the least understood aspects in atmospheric chemistry is how urban emissions influence the formation of natural organic aerosols, which affect Earth’s energy budget. The Amazon rainforest, during its wet season, is one of the few remaining places on Earth where atmospheric chemistry transitions between preindustrial and urban-influenced conditions. Here, we integrate insights from several laboratory measurements and simulate the formation of secondary organic aerosols (SOA) in the Amazon using a high-resolution chemical transport model. Simulations show that emissions of nitrogen-oxides from Manaus, a city of ~2 million people, greatly enhance production of biogenic SOA by 60–200% on average with peak enhancements of 400%, through the increased oxidation of gas-phase organic carbon emitted by the forests. Simulated enhancements agree with aircraft measurements, and are much larger than those reported over other locations. The implication is that increasing anthropogenic emissions in the future might substantially enhance biogenic SOA in pristine locations like the Amazon.

A key challenge in aerosol pollution studies and climate change assessment is to understand how atmospheric aerosol particles are initially formed^1,2. Although new particle formation (NPF) mechanisms have been described at specific sites^3–6, in most regions, such mechanisms remain uncertain to a large extent because of the limited ability of atmospheric models to simulate critical NPF processes^1,7. Here we synthesize molecular-level experiments to develop comprehensive representations of 11 NPF mechanisms and the complex chemical transformation of precursor gases in a fully coupled global climate model. Combined simulations and observations show that the dominant NPF mechanisms are distinct worldwide and vary with region and altitude. Previously neglected or underrepresented mechanisms involving organics, amines, iodine oxoacids and HNO₃ probably dominate NPF in most regions with high concentrations of aerosols or large aerosol radiative forcing; such regions include oceanic and human-polluted continental boundary layers, as well as the upper troposphere over rainforests and Asian monsoon regions. These underrepresented mechanisms also play notable roles in other areas, such as the upper troposphere of the Pacific and Atlantic oceans. Accordingly, NPF accounts for different fractions (10–80%) of the nuclei on which cloud forms at 0.5% supersaturation over various regions in the lower troposphere. The comprehensive simulation of global NPF mechanisms can help improve estimation and source attribution of the climate effects of aerosols.

Due to U.S. air pollution regulations, aerosol and precursor emissions have decreased during recent decades, while changes in emissions in other regions of the world also influence U.S. aerosol trends through long‐range transport. We examine here the relative roles of these domestic and foreign emission changes on aerosol concentrations and direct radiative forcing at the top of the atmosphere over the continental United States. Long‐term (1980–2014) trends and aerosol source apportionment are quantified in this study using a global aerosol‐climate model equipped with an explicit aerosol source tagging technique. Due to U.S. emission control policies, the annual mean near‐surface concentration of particles, consisting of sulfate, black carbon, and primary organic aerosol, decreases by about −1.1 (±0.1)/−1.4 (±0.1) μg/m³ in western United States and −3.3 (±0.2)/−2.9 (±0.2) μg/m³ in eastern United States during 2010–2014, as compared to those in 1980–1984. Meanwhile, decreases in U.S. emissions lead to a warming of +0.48 (±0.03)/+0.46 (±0.03) W/m² in western United States and +1.41 (±0.07)/+1.32 (±0.09) W/m² in eastern United States through changes in aerosol direct radiative forcing. Increases in emissions from East Asia generally have a modest impact on U.S. air quality but mitigated the warming effect induced by reductions in U.S. emissions by 25% in western United States and 7% in eastern United States. As U.S. domestic aerosol and precursor emissions continue to decrease, foreign emissions may become increasingly important to radiative forcing over the United States.

Black carbon (BC) has previously been found to intensify haze in China by stabilizing the planetary boundary layer. With ocean, sea ice and cloud feedbacks included in a global aerosol‐climate model, we show that BC emitted from the North China Plain can be transported to the oceans, which in turn changes cloud structure and land‐sea thermal contrast. As a result, East Asian winter monsoon wind speeds decrease over the North China Plain. This decrease causes air stagnation that can further intensify haze. Our results suggest that, in addition to the local BC‐induced interactions between aerosol and the planetary boundary layer, BC can also amplify haze in the North China Plain by weakening East Asian winter monsoon through ocean, sea ice and cloud feedbacks. It implies that reducing BC emissions could have significant indirect benefits for air quality in the North China Plain.

Aerosols have significantly affected health, environment, and climate in Europe. Aerosol concentrations have been declining since the 1980s in Europe, mainly owing to a reduction of local aerosol and precursor emissions. Emissions from other source regions of the world, which have been changing rapidly as well, may also perturb the historical and future trends of aerosols and change their radiative impact in Europe. This study examines trends of aerosols in Europe during 1980–2018 and quantifies contributions from 16 source regions using the Community Atmosphere Model version 5 with Explicit Aerosol Source Tagging (CAM5-EAST). The simulated near-surface total mass concentration of sulfate, black carbon, and primary organic carbon had a 62 % decrease during 1980–2018. The majority of which was contributed to reductions of local emissions in Europe, and 8 %–9 % was induced by a decrease in emissions from Russia–Belarus–Ukraine. With the decreases in the fractional contribution of local emissions, aerosols transported from other source regions are increasingly important for air quality in Europe. During 1980–2018, the decrease in sulfate loading led to a warming effect of 2.0 W m⁻² in Europe, with 12 % coming from changes in non-European sources, especially from North America and Russia–Belarus–Ukraine. According to the Shared Socioeconomic Pathways (SSP) scenarios, contributions to the sulfate radiative forcing over Europe from both local European emissions and non-European emissions should decrease at a comparable rate in the next 3 decades, suggesting that future changes in non-European emissions are as important as European emissions for causing possible regional climate change associated with aerosols in Europe.

We use a simple model of a spherical biomass burning aerosol particle containing an internal mixture of black carbon (BC) and organic carbon (OC) with an effective refractive index calculated as a volume fraction‐weighted mean of refractive indices. Brown carbon (BrC) is considered to be an OC with an imaginary part of refractive index at the blue end of the solar spectrum higher (in absolute value) than at the red end. Mie‐scattering formalism is employed to calculate absorption Ångström exponent (AAE) as a function of single‐scattering albedo (SSA) for a set of BC refractive indices, BC volume fraction, and a set of effective refractive indices of BC and BrC mixtures. Ambient plumes are characterized by their mean SSA at 405 nm wavelength and two‐wavelength (405 and 781 nm) AAE values. Comparing observed and model‐calculated AAE and SSA values identifies the BC refractive index and its volume fraction and an effective refractive index of the BC and BrC mixture. From these values, the imaginary part of BrC refractive index is calculated. For observed southwestern ambient fires, the imaginary part of BrC refractive index is ≤0.016. In contrast, fires in the Amazon and from Africa are dominated by BC. We also use the Mie scattering model to establish the upper limit on AAE of BC (AAE ≤ 1.4) and the upper limit of the BC and OC mixture (AAE ≤ 1.7). Any AAE(405/781) > 1.7 requires the presence of BrC. We derive several relationships between AAE, SSA, BC fractions, and an imaginary part of BrC refractive index of ambient fires.