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This study compares aerosol direct radiative effects on numerical weather forecasts made by the NCEP Global Forecast System (GFS) with two different aerosol datasets, the Optical Properties of Aerosols and Clouds (OPAC) and MERRA-2 aerosol climatologies. The underestimation of aerosol optical depth (AOD) by OPAC over northwest Africa, central to East Africa, the Arabian Peninsula, Southeast Asia, and the Indo-Gangetic Plain, and overestimation in the storm-track regions in both hemispheres are reduced by MERRA-2. Surface downward shortwave (SW) and longwave (LW) fluxes and the top-of-the-atmosphere SW and outgoing LW fluxes from model forecasts are compared with CERES satellite observations. Forecasts made with OPAC aerosols have large radiative flux biases, especially in northwest Africa and the storm-track regions. These biases are also reduced in the forecasts made with MERRA-2 aerosols. The improvements from MERRA-2 are most noticeable in the surface downward SW fluxes. GFS medium-range weather forecasts made with the MERRA-2 aerosols demonstrated slightly improved forecast accuracy of sea level pressure and precipitation over the Indian and East Asian summer monsoon region. A stronger Africa easterly jet is produced, associated with a low pressure over the east Atlantic Ocean and west of northwest Africa. Impacts on large-scale skill scores such as 500-hPa geopotential height anomaly correlation are generally positive in the Northern Hemisphere and the Pacific and North American regions in both the winter and summer seasons.

The direct perturbation of anthropogenic aerosols on Earth’s energy balance [i.e., direct aerosol radiative forcing (DARF)] remains uncertain in climate models. These uncertainties critically depend on aerosol optical properties, primarily aerosol optical depth (AOD), single scattering albedo (SSA), and the asymmetry factor g. In this study, we investigate the intermodel spread of DARF across 14 global models within phase 6 of the Coupled Model Intercomparison Project (CMIP6), using unified radiative transfer calculation and aerosol optical parameter assumptions. The global mean DARF for clear sky in 2014 with respect to 1850 is estimated as −0.77 ± 0.52 W m−2 assuming an externally mixed state and −0.68 ± 0.53 W m−2 for an internally mixed state. We further conduct a quantitative analysis and find that globally, for the external mixing assumption, AOD is the dominant factor, whose intermodel spread results in 36% of the total DARF uncertainty. For the internal mixing assumption, SSA becomes the major factor, which also leads to 36% DARF uncertainty. The g parameter and aerosol vertical distribution combined contribute to ∼30% of the DARF uncertainty. Regionally, DARF uncertainty is typically more sensitive to SSA where the absorbing aerosol fraction is high, such as South Asia and central Africa. Substantial differences between model-averaged and observed aerosol optical parameters are still noticed, with external mixing in general yielding closer agreement with observations. Our results highlight the importance of aerosol scattering and absorption properties in DARF estimation.

The direct perturbation of anthropogenic aerosols on Earth’s energy balance [i.e., direct aerosol radiative forcing (DARF)] remains uncertain in climate models. In this study, we investigate the uncertainty of DARF associated with aerosol vertical distribution, using simulation results from 14 global models within phase 6 of the Coupled Model Intercomparison Project (CMIP6). The column mass loading for each aerosol species is first normalized to the multimodel average for each model, which is called the mass-normalization process. The unified radiative transfer model and aerosol optical parameter are used, so that the differences in the calculated DARF are solely attributed to the difference in aerosol vertical profiles. The global mean DARF values in 2014 with respect to 1850 before and after mass normalization are −0.77 ± 0.52 and −0.81 ± 0.12 W m−2 respectively, assuming external mixing, which indicates that the intermodel difference in aerosol vertical distribution accounts for ∼20% of the total DARF uncertainty. We further conduct two separate experiments by normalizing aerosol optical depth (AOD) and aerosol single scattering albedo (SSA) profiles, respectively, and find that the vertical distribution of SSA results in larger DARF uncertainty (0.17 W m−2) than that of AOD (0.10 W m−2). Finally, compared with CALIPSO observation, CMIP6 models tend to produce higher aerosol layers. The bias in modeled aerosol profile with respect to CALIPSO leads to stronger DARF, especially for land regions.

The goal of the Sea2Cloud project is to study the interplay between surface ocean biogeochemical and physical properties, fluxes to the atmosphere, and ultimately their impact on cloud formation under minimal direct anthropogenic influence. Here we present an interdisciplinary approach, combining atmospheric physics and chemistry with marine biogeochemistry, during a voyage between 41° and 47°S in March 2020. In parallel to ambient measurements of atmospheric composition and seawater biogeochemical properties, we describe semicontrolled experiments to characterize nascent sea spray properties and nucleation from gas-phase biogenic emissions. The experimental framework for studying the impact of the predicted evolution of ozone concentration in the Southern Hemisphere is also detailed. After describing the experimental strategy, we present the oceanic and meteorological context including provisional results on atmospheric thermodynamics, composition, and flux measurements. In situ measurements and flux studies were carried out on different biological communities by sampling surface seawater from subantarctic, subtropical, and frontal water masses. Air–Sea-Interface Tanks (ASIT) were used to quantify biogenic emissions of trace gases under realistic environmental conditions, with nucleation observed in association with biogenic seawater emissions. Sea spray continuously generated produced sea spray fluxes of 34% of organic matter by mass, of which 4% particles had fluorescent properties, and which size distribution resembled the one found in clean sectors of the Southern Ocean. The goal of Sea2Cloud is to generate realistic parameterizations of emission flux dependences of trace gases and nucleation precursors, sea spray, cloud condensation nuclei, and ice nuclei using seawater biogeochemistry, for implementation in regional atmospheric models.

El Niño–Southern Oscillation (ENSO) is the leading mode of Earth’s climate variability at interannual time scales with profound ecological and societal impacts, and it is projected to intensify in many climate models as the climate warms under the forcing of increasing CO₂ concentration. Since the preindustrial era, black carbon (BC) emissions have substantially increased in the Northern Hemisphere. But how BC aerosol forcing may influence the occurrence of the extreme ENSO events has rarely been investigated. In this study, using simulations of a global climate model, we show that increases in BC emissions from both the midlatitudes and Arctic weaken latitudinal temperature gradients and northward heat transport, decrease tropical energy divergence, and increase sea surface temperature over the tropical oceans, with a surprising consequential increase in the frequency of extreme ENSO events. A corollary of this study is that reducing BC emissions might serve to mitigate the possible increasing frequency of extreme ENSO events under greenhouse warming, if the modeling result can be translated into the climate in reality.

Road transport significantly contributes to air pollution in cities. Emission regulations have led to significantly reduced emissions in modern vehicles. Particle emissions are controlled by a particulate matter (PM) mass and a solid particle number (SPN) limit. There are concerns that the SPN limit does not effectively control all relevant particulate species and there are instances of semi-volatile particle emissions that are order of magnitudes higher than the SPN emission levels. This overview discusses whether a new metric (total particles, i.e., solids and volatiles) should be introduced for the effective regulation of vehicle emissions. Initially, it summarizes recent findings on the contribution of road transport to particle number concentration levels in cities. Then, both solid and total particle emission levels from modern vehicles are presented and the adverse health effects of solid and volatile particles are briefly discussed. Finally, the open issues regarding an appropriate methodology (sampling and instrumentation) in order to achieve representative and reproducible results are summarized. The main finding of this overview is that, even though total particle sampling and quantification is feasible, details for its realization in a regulatory context are lacking. It is important to define the methodology details (sampling and dilution, measurement instrumentation, relevant sizes, etc.) and conduct inter-laboratory exercises to determine the reproducibility of a proposed method. It is also necessary to monitor the vehicle emissions according to the new method to understand current and possible future levels. With better understanding of the instances of formation of nucleation mode particles it will be possible to identify its culprits (e.g., fuel, lubricant, combustion, or aftertreatment operation). Then the appropriate solutions can be enforced and the right decisions can be taken on the need for new regulatory initiatives, for example the addition of total particles in the tailpipe, decrease of specific organic precursors, better control of inorganic precursors (e.g., NH3, SOx), or revision of fuel and lubricant specifications.

Primary aerosols play a critical role in polar climate systems, influencing cloud formation, precipitation, radiative balance, and surface energy budgets. This paper provides a comprehensive synthesis of primary aerosol sources, transformation and removal processes, and broader atmospheric impacts in polar regions, emphasizing their links to ocean and sea ice biogeochemistry. These aerosols (including sea salt, primary organic aerosol, and primary biological aerosol particles) originate from marine and cryospheric environments and are emitted through physical processes, such as wave breaking, bubble bursting, and blowing snow. Emission sources include seawater, sea ice, snow, and freshwater from river discharge and glacial runoff. Once airborne, these particles can serve as a chemical reservoir, influencing atmospheric composition and reactivity, and as seeds for cloud droplet and ice crystal formation, influencing cloud microphysics and polar climate. Despite their importance, many of the processes governing primary aerosol emissions and transformations remain poorly constrained. The most pressing knowledge gaps pertain to emission processes, limited spatiotemporal observational coverage, instrumentation constraints, parameterization development, and the integration of interdisciplinary expertise. To improve our understanding of primary aerosol drivers and their response to climate, future research efforts should prioritize strategically coordinated and cross-disciplinary process studies, advancements in measurement technologies and coverage, and close collaboration between modelers and observational scientists to inform and refine model parameterizations. As polar regions continue to undergo profound changes marked by increased precipitation, reduced sea and land ice, freshening oceans, and shifting ecosystem dynamics, characterizing present-day primary aerosol populations is vital. Improved understanding will be essential for anticipating future changes in aerosol-radiation and aerosol-cloud interactions and their implications for polar and global climate systems.

To understand the aerosol characteristics in a regional background environment, fine-particle (PM 2.5 , n = 228) samples were collected over a one-year period at the Shangdianzi (SDZ) station, which is a Global Atmospheric Watch regional background station in North China. The chemical and optical characteristics of PM 2.5 were analyzed, including organic carbon, elemental carbon, water-soluble organic carbon, water-soluble inorganic ions, and fluorescent components of water-soluble organic matter. The source factors of major aerosol components are apportioned, and the sources of the fluorescent chromophores are further analyzed. The major chemical components of PM 2.5 at SDZ were NO 3 − , organic matter, SO 4 2− , and NH 4 + . Annually, water-soluble organic carbon contributed 48% ± 15% to the total organic carbon. Secondary formation (52%) and fossil fuel combustion (63%) are the largest sources of water-soluble organic matter and water-insoluble organic matter, respectively. In addition, three humic-like and one protein-like matter were identified via parallel factor analysis for excitation—emission matrices. The fluorescence intensities of the components were highest in winter and lowest in summer, indicating the main impact of burning sources. This study contributes to understanding the chemical and optical characteristics of ambient aerosols in the background atmosphere.

Diesel vehicles are recognized as significant mobile sources of particulate matter emissions. As a renewable and environmentally friendly alternative to conventional fossil diesel, biodiesel offers the benefit of reducing greenhouse gas emissions. However, existing research on biodiesel emissions primarily focuses on primary emissions, with a limited understanding of their impact on secondary organic aerosol (SOA) formation. In this study, a diesel engine test bench was employed under idle conditions using three commonly used biodiesel blends. Exhaust emissions were directly introduced into the HAP-SWFU chamber, a quartz glass smog chamber designed to characterize both primary emissions and SOA formation during the photochemical oxidation process. The black carbon and primary organic aerosol (POA) emission factors for the three biodiesel blends under idle conditions ranged from 0.31 to 0.58 g kg−1 fuel and 0.99 to 1.06 g kg−1 fuel, respectively. The particle size of exhaust particulates peaked between 20 and 30 nm, and nucleation-idle conditions were found to be the dominating mode. The SOA production factor was between 0.92 and 1.15 g kg−1 fuel, and the SOA/POA ratio ranged from 1.35 to 2.37, with an average of 1.86. This study concludes that the POA emission factor for biodiesel under idle conditions is comparable to values reported in previous studies on pure diesel exhaust, with the maximum SOA production factor reduced by 38%.

Submicron atmospheric particles in the Amazon Basin were characterized by a high‐resolution aerosol mass spectrometer during the wet season of 2008. Patterns in the mass spectra closely resembled those of secondary‐organic‐aerosol (SOA) particles formed in environmental chambers from biogenic precursor gases. In contrast, mass spectral indicators of primary biological aerosol particles (PBAPs) were insignificant, suggesting that PBAPs contributed negligibly to the submicron fraction of particles during the period of study. For 40% of the measurement periods, the mass spectra indicate that in‐Basin biogenic SOA production was the dominant source of the submicron mass fraction, contrasted to other periods (30%) during which out‐of‐Basin organic‐carbon sources were significant on top of the baseline in‐Basin processes. The in‐Basin periods had an average organic‐particle loading of 0.6 μg m−3 and an average elemental oxygen‐to‐carbon (O:C) ratio of 0.42, compared to 0.9 μg m−3 and 0.49, respectively, during periods of out‐of‐Basin influence. On the basis of the data, we conclude that most of the organic material composing submicron particles over the Basin derived from biogenic SOA production, a finding that is consistent with microscopy observations made in a concurrent study. This source was augmented during some periods by aged organic material delivered by long‐range transport.