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Anthropogenic emissions of aerosols and precursor compounds are known to significantly affect the energy balance of the Earth–atmosphere system, alter the formation of clouds and precipitation, and have a substantial impact on human health and the environment. Global models are an essential tool for examining the impacts of these emissions. In this study, we examine the sensitivity of model results to the assumed height of SO2 injection, seasonality of SO2 and black carbon (BC) particulate emissions, and the assumed fraction of SO2 emissions that is injected into the atmosphere as particulate phase sulfate (SO4) in 11 climate and chemistry models, including both chemical transport models and the atmospheric component of Earth system models. We find large variation in atmospheric lifetime across models for SO2, SO4, and BC, with a particularly large relative variation for SO2, which indicates that fundamental aspects of atmospheric sulfur chemistry remain uncertain. Of the perturbations examined in this study, the assumed height of SO2 injection had the largest overall impacts, particularly on global mean net radiative flux (maximum difference of −0.35 W m−2), SO2 lifetime over Northern Hemisphere land (maximum difference of 0.8 d), surface SO2 concentration (up to 59 % decrease), and surface sulfate concentration (up to 23 % increase). Emitting SO2 at height consistently increased SO2 and SO4 column burdens and shortwave cooling, with varying magnitudes, but had inconsistent effects across models on the sign of the change in implied cloud forcing. The assumed SO4 emission fraction also had a significant impact on net radiative flux and surface sulfate concentration. Because these properties are not standardized across models this is a source of inter-model diversity typically neglected in model intercomparisons. These results imply a need to ensure that anthropogenic emission injection height and SO4 emission fraction are accurately and consistently represented in global models.

Paul Jozef Crutzen was a pioneer in the atmospheric sciences, a kind-hearted and humorous person with empathy for the private lives of his colleagues and students, and a man who upheld the highest scientific standards for himself and for others. He made fundamental scientific contributions to a wide range of scientific topics in all parts of the atmosphere, from the mesosphere to the stratosphere and from the stratosphere to the troposphere. In particular, he was the first to describe the NOx-driven ozone depletion cycle in the stratosphere, he was among the first to develop the idea of chemical formation of ozone in the troposphere, he provided key concepts to explain the “ozone hole”, and he made fundamental discoveries about the effects of biomass burning on the troposphere. Understanding and addressing the causes of anthropogenic air pollution and climate change were the driving motivations for his scientific work. In his work, he did not shy away from challenge and provocation. His work on smoke from fires after a potential nuclear war inspired new research on a concept now known as “nuclear winter”. He also initiated the reopening of the debate on “geoengineering” – a concept now referred to as “climate intervention”. He also brought the term “Anthropocene” to the popular debate. Moreover, he had a strong influence on atmospheric science through his educational role; there is a very large number of outstanding scientists who started their career with scientific work with Paul. In 2000, Paul was among the founders of the journal Atmospheric Chemistry and Physics, which was unique at the time in providing public discussion of published preprints as well as what we now call “open access” to published articles. Paul's work on human impacts on atmosphere and climate has had a profound impact on the environmental policies of many countries for decades. In the future, his work will continue to be a guide for generations of scientists and environmental policymakers to come.

Despite a large number of studies, out of all drivers of radiative forcing, the effect of aerosols has the largest uncertainty in global climate model radiative forcing estimates. There have been studies of aerosol optical properties in climate models, but the effects of particle number size distribution need a more thorough inspection. We investigated the trends and seasonality of particle number concentrations in nucleation, Aitken, and accumulation modes at 21 measurement sites in Europe and the Arctic. For 13 of those sites, with longer measurement time series, we compared the field observations with the results from five climate models, namely EC-Earth3, ECHAM-M7, ECHAM-SALSA, NorESM1.2, and UKESM1. This is the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five earth system models (ESMs). We found that the trends of particle number concentrations were mostly consistent and decreasing in both measurements and models. However, for many sites, climate models showed weaker decreasing trends than the measurements. Seasonal variability in measured number concentrations, quantified by the ratio between maximum and minimum monthly number concentration, was typically stronger at northern measurement sites compared to other locations. Models had large differences in their seasonal representation, and they can be roughly divided into two categories: for EC-Earth and NorESM, the seasonal cycle was relatively similar for all sites, and for other models the pattern of seasonality varied between northern and southern sites. In addition, the variability in concentrations across sites varied between models, some having relatively similar concentrations for all sites, whereas others showed clear differences in concentrations between remote and urban sites. To conclude, although all of the model simulations had identical input data to describe anthropogenic mass emissions, trends in differently sized particles vary among the models due to assumptions in emission sizes and differences in how models treat size-dependent aerosol processes. The inter-model variability was largest in the accumulation mode, i.e. sizes which have implications for aerosol–cloud interactions. Our analysis also indicates that between models there is a large variation in efficiency of long-range transportation of aerosols to remote locations. The differences in model results are most likely due to the more complex effect of different processes instead of one specific feature (e.g. the representation of aerosol or emission size distributions). Hence, a more detailed characterization of microphysical processes and deposition processes affecting the long-range transport is needed to understand the model variability.

New particle formation (NPF) is a significant source of atmospheric particles, affecting climate and air quality. Understanding the mechanisms involved in urban aerosols is important to develop effective mitigation strategies. However, NPF rates reported in the polluted boundary layer span more than 4 orders of magnitude, and the reasons behind this variability are the subject of intense scientific debate. Multiple atmospheric vapours have been postulated to participate in NPF, including sulfuric acid, ammonia, amines and organics, but their relative roles remain unclear. We investigated NPF in the CLOUD chamber using mixtures of anthropogenic vapours that simulate polluted boundary layer conditions. We demonstrate that NPF in polluted environments is largely driven by the formation of sulfuric acid–base clusters, stabilized by the presence of amines, high ammonia concentrations and lower temperatures. Aromatic oxidation products, despite their extremely low volatility, play a minor role in NPF in the chosen urban environment but can be important for particle growth and hence for the survival of newly formed particles. Our measurements quantitatively account for NPF in highly diverse urban environments and explain its large observed variability. Such quantitative information obtained under controlled laboratory conditions will help the interpretation of future ambient observations of NPF rates in polluted atmospheres.

This paper presents an analysis of the mineral dust aerosol modelled by five Earth system models (ESMs) within the project entitled Coordinated Research in Earth Systems and Climate: Experiments, kNowledge, Dissemination and Outreach (CRESCENDO). We quantify the global dust cycle described by each model in terms of global emissions, together with dry and wet deposition, reporting large differences in the ratio of dry over wet deposition across the models not directly correlated with the range of particle sizes emitted. The multi-model mean dust emissions with five ESMs is 2836 Tg yr−1 but with a large uncertainty due mainly to the difference in the maximum dust particle size emitted. The multi-model mean of the subset of four ESMs without particle diameters larger than 10 µ m is 1664 (σ=651) Tg yr−1. Total dust emissions in the simulations with identical nudged winds from reanalysis give us better consistency between models; i.e. the multi-model mean global emissions with three ESMs are 1613 (σ=278) Tg yr−1, but 1834 (σ=666) Tg yr−1 without nudged winds and the same models. Significant discrepancies in the globally averaged dust mass extinction efficiency explain why even models with relatively similar global dust load budgets can display strong differences in dust optical depth. The comparison against observations has been done in terms of dust optical depths based on MODIS (Moderate Resolution Imaging Spectroradiometer) satellite products, showing global consistency in terms of preferential dust sources and transport across the Atlantic. The global localisation of source regions is consistent with MODIS, but we found regional and seasonal differences between models and observations when we quantified the cross-correlation of time series over dust-emitting regions. To faithfully compare local emissions between models we introduce a re-gridded normalisation method that can also be compared with satellite products derived from dust event frequencies. Dust total deposition is compared with an instrumental network to assess global and regional differences. We find that models agree with observations within a factor of 10 for data stations distant from dust sources, but the approximations of dust particle size distribution at emission contributed to a misrepresentation of the actual range of deposition values when instruments are close to dust-emitting regions. The observed dust surface concentrations also are reproduced to within a factor of 10. The comparison of total aerosol optical depth with AERONET (AErosol RObotic NETwork) stations where dust is dominant shows large differences between models, although with an increase in the inter-model consistency when the simulations are conducted with nudged winds. The increase in the model ensemble consistency also means better agreement with observations, which we have ascertained for dust total deposition, surface concentrations and optical depths (against both AERONET and MODIS retrievals). We introduce a method to ascertain the contributions per mode consistent with the multi-modal direct radiative effects, which we apply to study the direct radiative effects of a multi-modal representation of the dust particle size distribution that includes the largest particles.

Understanding the vertical distribution of aerosol helps to reduce the uncertainty in the aerosol life cycle and therefore in the estimation of the direct and indirect aerosol forcing. To improve our understanding, we use measurements from four deployments of the Atmospheric Tomography (ATom) field campaign (ATom1–4) which systematically sampled aerosol and trace gases over the Pacific and Atlantic oceans with near pole-to-pole coverage. We evaluate the UK Earth System Model (UKESM1) against ATom observations in terms of joint biases in the vertical profile of three variables related to new particle formation: total particle number concentration (NTotal), sulfur dioxide (SO2) mixing ratio and the condensation sink. The NTotal, SO2 and condensation sink are interdependent quantities and have a controlling influence on the vertical profile of each other; therefore, analysing them simultaneously helps to avoid getting the right answer for the wrong reasons. The simulated condensation sink in the baseline model is within a factor of 2 of observations, but the NTotal and SO2 show much larger biases mainly in the tropics and high latitudes. We performed a series of model sensitivity tests to identify atmospheric processes that have the strongest influence on overall model performance. The perturbations take the form of global scaling factors or improvements to the representation of atmospheric processes in the model, for example by adding a new boundary layer nucleation scheme. In the boundary layer (below 1 km altitude) and lower troposphere (1–4 km), inclusion of a boundary layer nucleation scheme (Metzger et al., 2010) is critical to obtaining better agreement with observations. However, in the mid (4–8 km) and upper troposphere (> 8 km), sub-3 nm particle growth, pH of cloud droplets, dimethyl sulfide (DMS) emissions, upper-tropospheric nucleation rate, SO2 gas-scavenging rate and cloud erosion rate play a more dominant role. We find that perturbations to boundary layer nucleation, sub-3 nm growth, cloud droplet pH and DMS emissions reduce the boundary layer and upper tropospheric model bias simultaneously. In a combined simulation with all four perturbations, the SO2 and condensation sink profiles are in much better agreement with observations, but the NTotal profile still shows large deviations, which suggests a possible structural issue with how nucleation or gas/particle transport or aerosol scavenging is handled in the model. These perturbations are well-motivated in that they improve the physical basis of the model and are suitable for implementation in future versions of UKESM.

A global model perturbed parameter ensemble of 60 simulations was used to explore how combinations of six parameters related to secondary organic aerosol (SOA) formation affect particle number concentrations and organic aerosol mass. The parameters represent the formation of organic compounds with different volatilities from biogenic and anthropogenic sources. The most plausible parameter combinations were determined by comparing the simulations against observations of the number concentration of particles larger than 3 nm diameter (N3), the number concentration of particles larger than 50 nm diameter (N50), and the organic aerosol (OA) mass concentration. The simulations expose a high degree of model equifinality in which the skill of widely different parameter combinations cannot be distinguished against observations. We therefore conclude that, based on the observations we have used, a six-parameter SOA scheme is under-determined. Nevertheless, the model skill in simulating N3 and N50 is clearly determined by the low-volatility and extremely low-volatility compounds that affect new particle formation and growth, and the skill in simulating OA mass is determined by the low-volatility and semi-volatile compounds. The biogenic low-volatility class of compounds that grow nucleated clusters and condense on all particles is found to have the strongest effect on the model skill in simulating N3, N50, and OA. The simulations also expose potential structural deficiencies in the model: we find that parameter combinations that are best for N3 and N50 are worst for OA mass, and the ensemble exaggerates the observed seasonal cycle of particle concentrations – a deficiency that we conclude requires an additional anthropogenic source of either primary or secondary particles.

The representations of clouds, aerosols, and cloud–aerosol–radiation impacts remain some of the largest uncertainties in climate change, limiting our ability to accurately reconstruct past climate and predict future climate. The south-east Atlantic is a region where high atmospheric aerosol loadings and semi-permanent stratocumulus clouds are co-located, providing an optimum region for studying the full range of aerosol–radiation and aerosol–cloud interactions and their perturbations of the Earth's radiation budget. While satellite measurements have provided some useful insights into aerosol–radiation and aerosol–cloud interactions over the region, these observations do not have the spatial and temporal resolution, nor the required level of precision to allow for a process-level assessment. Detailed measurements from high spatial and temporal resolution airborne atmospheric measurements in the region are very sparse, limiting their use in assessing the performance of aerosol modelling in numerical weather prediction and climate models. CLARIFY-2017 was a major consortium programme consisting of five principal UK universities with project partners from the UK Met Office and European- and USA-based universities and research centres involved in the complementary ORACLES, LASIC, and AEROCLO-sA projects. The aims of CLARIFY-2017 were fourfold: (1) to improve the representation and reduce uncertainty in model estimates of the direct, semi-direct, and indirect radiative effect of absorbing biomass burning aerosols; (2) to improve our knowledge and representation of the processes determining stratocumulus cloud microphysical and radiative properties and their transition to cumulus regimes; (3) to challenge, validate, and improve satellite retrievals of cloud and aerosol properties and their radiative impacts; (4) to improve the impacts of aerosols in weather and climate numerical models. This paper describes the modelling and measurement strategies central to the CLARIFY-2017 deployment of the FAAM BAe146 instrumented aircraft campaign, summarizes the flight objectives and flight patterns, and highlights some key results from our initial analyses.

We describe Global Atmosphere 7.0 and Global Land 7.0 (GA7.0/GL7.0), the latest science configurations of the Met Office Unified Model (UM) and the Joint UK Land Environment Simulator (JULES) land surface model developed for use across weather and climate timescales. GA7.0 and GL7.0 include incremental developments and targeted improvements that, between them, address four critical errors identified in previous configurations: excessive precipitation biases over India, warm and moist biases in the tropical tropopause layer (TTL), a source of energy non-conservation in the advection scheme and excessive surface radiation biases over the Southern Ocean. They also include two new parametrisations, namely the UK Chemistry and Aerosol (UKCA) GLOMAP-mode (Global Model of Aerosol Processes) aerosol scheme and the JULES multi-layer snow scheme, which improve the fidelity of the simulation and were required for inclusion in the Global Atmosphere/Global Land configurations ahead of the 6th Coupled Model Intercomparison Project (CMIP6). In addition, we describe the GA7.1 branch configuration, which reduces an overly negative anthropogenic aerosol effective radiative forcing (ERF) in GA7.0 whilst maintaining the quality of simulations of the present-day climate. GA7.1/GL7.0 will form the physical atmosphere/land component in the HadGEM3–GC3.1 and UKESM1 climate model submissions to the CMIP6.

We present the results of laboratory measurements of the ion–ion recombination coefficient at different temperatures, relative humidities and concentrations of ozone and sulfur dioxide. The experiments were carried out using the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at CERN, the walls of which are made of conductive material, making it possible to measure small ions. We produced ions in the chamber using a 3.5 GeV c−1 beam of positively charged pions (π+) generated by the CERN Proton Synchrotron (PS). When the PS was switched off, galactic cosmic rays were the only ionization source in the chamber. The range of the ion production rate varied from 2 to 100 cm−3 s−1, covering the typical range of ionization throughout the troposphere. The temperature ranged from −55 to 20 °C, the relative humidity (RH) from 0 to 70 %, the SO2 concentration from 0 to 40 ppb, and the ozone concentration from 200 to 700 ppb. The best agreement of the retrieved ion–ion recombination coefficient with the commonly used literature value of 1.6 × 10−6 cm3 s−1 was found at a temperature of 5 °C and a RH of 40 % (1.5 ± 0.6) × 10−6 cm3 s−1. At 20 °C and 40 % RH, the retrieved ion–ion recombination coefficient was instead (2.3 ± 0.7) × 10−6 cm3 s−1. We observed no dependency of the ion–ion recombination coefficient on ozone concentration and a weak variation with sulfur dioxide concentration. However, we observed a more than fourfold increase in the ion–ion recombination coefficient with decreasing temperature. We compared our results with three different models and found an overall agreement for temperatures above 0 °C, but a disagreement at lower temperatures. We observed a strong increase in the recombination coefficient for decreasing relative humidities, which has not been reported previously.

The literature on atmospheric particulate matter (PM), or atmospheric aerosol, has increased enormously over the last 2 decades and amounts now to some 1500–2000 papers per year in the refereed literature. This is in part due to the enormous advances in measurement technologies, which have allowed for an increasingly accurate understanding of the chemical composition and of the physical properties of atmospheric particles and of their processes in the atmosphere. The growing scientific interest in atmospheric aerosol particles is due to their high importance for environmental policy. In fact, particulate matter constitutes one of the most challenging problems both for air quality and for climate change policies. In this context, this paper reviews the most recent results within the atmospheric aerosol sciences and the policy needs, which have driven much of the increase in monitoring and mechanistic research over the last 2 decades. The synthesis reveals many new processes and developments in the science underpinning climate–aerosol interactions and effects of PM on human health and the environment. However, while airborne particulate matter is responsible for globally important influences on premature human mortality, we still do not know the relative importance of the different chemical components of PM for these effects. Likewise, the magnitude of the overall effects of PM on climate remains highly uncertain. Despite the uncertainty there are many things that could be done to mitigate local and global problems of atmospheric PM. Recent analyses have shown that reducing black carbon (BC) emissions, using known control measures, would reduce global warming and delay the time when anthropogenic effects on global temperature would exceed 2 °C. Likewise, cost-effective control measures on ammonia, an important agricultural precursor gas for secondary inorganic aerosols (SIA), would reduce regional eutrophication and PM concentrations in large areas of Europe, China and the USA. Thus, there is much that could be done to reduce the effects of atmospheric PM on the climate and the health of the environment and the human population. A prioritized list of actions to mitigate the full range of effects of PM is currently undeliverable due to shortcomings in the knowledge of aerosol science; among the shortcomings, the roles of PM in global climate and the relative roles of different PM precursor sources and their response to climate and land use change over the remaining decades of this century are prominent. In any case, the evidence from this paper strongly advocates for an integrated approach to air quality and climate policies.

The release of vast quantities of methane into the atmosphere as a result of clathrate destabilization is a potential mechanism for rapid amplification of global warming. Previous studies have calculated the enhanced warming based mainly on the radiative effect of the methane itself, with smaller contributions from the associated carbon dioxide or ozone increases. Here, we study the effect of strongly elevated methane (CH4) levels on oxidant and aerosol particle concentrations using a combination of chemistry-transport and general circulation models. A 10-fold increase in methane concentrations is predicted to significantly decrease hydroxyl radical (OH) concentrations, while moderately increasing ozone (O3). These changes lead to a 70 % increase in the atmospheric lifetime of methane, and an 18 % decrease in global mean cloud droplet number concentrations (CDNC). The CDNC change causes a radiative forcing that is comparable in magnitude to the longwave radiative forcing ("enhanced greenhouse effect") of the added methane. Together, the indirect CH4-O3 and CH4-OH-aerosol forcings could more than double the warming effect of large methane increases. Our findings may help explain the anomalously large temperature changes associated with historic methane releases.

During a 4-week run in October–November 2006, a pilot experiment was performed at the CERN Proton Synchrotron in preparation for the Cosmics Leaving OUtdoor Droplets (CLOUD) experiment, whose aim is to study the possible influence of cosmic rays on clouds. The purpose of the pilot experiment was firstly to carry out exploratory measurements of the effect of ionising particle radiation on aerosol formation from trace H2SO4 vapour and secondly to provide technical input for the CLOUD design. A total of 44 nucleation bursts were produced and recorded, with formation rates of particles above the 3 nm detection threshold of between 0.1 and 100 cm−3s−1, and growth rates between 2 and 37 nm h−1. The corresponding H2O concentrations were typically around 106 cm−3 or less. The experimentally-measured formation rates and htwosofour concentrations are comparable to those found in the atmosphere, supporting the idea that sulphuric acid is involved in the nucleation of atmospheric aerosols. However, sulphuric acid alone is not able to explain the observed rapid growth rates, which suggests the presence of additional trace vapours in the aerosol chamber, whose identity is unknown. By analysing the charged fraction, a few of the aerosol bursts appear to have a contribution from ion-induced nucleation and ion-ion recombination to form neutral clusters. Some indications were also found for the accelerator beam timing and intensity to influence the aerosol particle formation rate at the highest experimental SO2 concentrations of 6 ppb, although none was found at lower concentrations. Overall, the exploratory measurements provide suggestive evidence for ion-induced nucleation or ion-ion recombination as sources of aerosol particles. However in order to quantify the conditions under which ion processes become significant, improvements are needed in controlling the experimental variables and in the reproducibility of the experiments. Finally, concerning technical aspects, the most important lessons for the CLOUD design include the stringent requirement of internal cleanliness of the aerosol chamber, as well as maintenance of extremely stable temperatures (variations below 0.1 °C

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., (© 2021. The Author(s).)

This corrects the article DOI: 10.1038/sdata.2017.3.

Cloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other international sites over multiple years. Here, harmonized data records from 11 observatories are summarized, spanning 98,677 instrument hours for CCN data, 157,880 for particle number size distributions, and 70,817 for chemical composition data. The observatories represent nine different environments, e.g., Arctic, Atlantic, Pacific and Mediterranean maritime, boreal forest, or high alpine atmospheric conditions. This is a unique collection of aerosol particle properties most relevant for studying aerosol-cloud interactions which constitute the largest uncertainty in anthropogenic radiative forcing of the climate. The dataset is appropriate for comprehensive aerosol characterization (e.g., closure studies of CCN), model-measurement intercomparison and satellite retrieval method evaluation, among others. Data have been acquired and processed following international recommendations for quality assurance and have undergone multiple stages of quality assessment.