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Abstract 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 HNO₃probably 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. 

Abstract Atmospheric aerosol and chemistry modules are key elements in Earth system models (ESMs), as they predict air pollutant concentrations and properties that can impact human health, weather, and climate. The current uncertainty in climate projections is partly due to the inaccurate representation of aerosol direct and indirect forcing. Aerosol/chemistry parameterizations used within ESMs and other atmospheric models span large structural and parameter uncertainties that are difficult to assess independently of their host models. Moreover, there is a strong need for a standardized interface between aerosol/chemistry modules and the host model to facilitate portability of aerosol/chemistry parameterizations from one model to another, allowing not only a comparison between different parameterizations within the same modeling framework, but also quantifying the impact of different model frameworks on aerosol/chemistry predictions. To address this need, we have initiated a new community effort to coordinate the construction of a Generalized Aerosol/Chemistry Interface (GIANT) for use across weather and climate models. We aim to organize a series of community workshops and hackathons to design and build GIANT, which will serve as the interface between a range of aerosol/chemistry modules and the physics and dynamics components of atmospheric host models. GIANT will leverage ongoing efforts at the U.S. modeling centers focused on building next-generation ESMs and the international AeroCom initiative to implement this common aerosol/chemistry interface. GIANT will create transformative opportunities for scientists and students to conduct innovative research to better characterize structural and parametric uncertainties in aerosol/chemistry modules, and to develop a common set of aerosol/chemistry parameterizations. 

Abstract. One of the challenges inrepresenting warm rain processes in global climate models (GCMs) is relatedto the representation of the subgrid variability of cloud properties, such ascloud water and cloud droplet number concentration (CDNC), and the effectthereof on individual precipitation processes such as autoconversion. Thiseffect is conventionally treated by multiplying the resolved-scale warm rainprocess rates by an enhancement factor (E_q) which is derived fromintegrating over an assumed subgrid cloud water distribution. The assumedsubgrid cloud distribution remains highly uncertain. In this study, we derivethe subgrid variations of liquid-phase cloud properties over the tropicalocean using the satellite remote sensing products from Moderate ResolutionImaging Spectroradiometer (MODIS) and investigate the correspondingenhancement factors for the GCM parameterization of autoconversion rate. Wefind that the conventional approach of using only subgrid variability ofcloud water is insufficient and that the subgrid variability of CDNC, as wellas the correlation between the two, is also important for correctlysimulating the autoconversion process in GCMs. Using the MODIS data whichhave near-global data coverage, we find that E_q shows a strongdependence on cloud regimes due to the fact that the subgrid variability ofcloud water and CDNC is regime dependent. Our analysis shows a significantincrease of E_q from the stratocumulus (Sc) to cumulus (Cu) regions.Furthermore, the enhancement factor E_N due to the subgrid variation ofCDNC is derived from satellite observation for the first time, and resultsreveal several regions downwind of biomass burning aerosols (e.g., Gulf ofGuinea, east coast of South Africa), air pollution (i.e., East China Sea),and active volcanos (e.g., Kilauea, Hawaii, and Ambae, Vanuatu), where theE_N is comparable to or even larger than E_q, suggesting an importantrole of aerosol in influencing the E_N. MODIS observations suggest thatthe subgrid variations of cloud liquid water path (LWP) and CDNC aregenerally positively correlated. As a result, the combined enhancementfactor, including the effect of LWP and CDNC correlation, is significantlysmaller than the simple product of E_q⋅E_N. Given the importanceof warm rain processes in understanding the Earth's system dynamics and watercycle, we conclude that more observational studies are needed to provide abetter constraint on the warm rain processes in GCMs. 

Abstract. Aerosol–cloud interactions (ACIs) are considered to be the most uncertaindriver of present-day radiative forcing due to human activities. Thenonlinearity of cloud-state changes to aerosol perturbations make itchallenging to attribute causality in observed relationships of aerosolradiative forcing. Using correlations to infer causality can be challengingwhen meteorological variability also drives both aerosol and cloud changesindependently. Natural and anthropogenic aerosol perturbations from well-defined sources provide “opportunistic experiments” (also known as natural experiments) to investigate ACI in cases where causality may be more confidently inferred. These perturbations cover a wide range of locations and spatiotemporal scales, including point sources such as volcanic eruptions or industrial sources, plumes from biomass burning or forest fires, and tracks from individual ships or shipping corridors. We review the different experimental conditions and conduct a synthesis of the available satellite datasets and field campaigns to place these opportunistic experiments on a common footing, facilitating new insights and a clearer understanding of key uncertainties in aerosol radiative forcing. Cloud albedo perturbations are strongly sensitive to background meteorological conditions. Strong liquid water path increases due to aerosol perturbations are largely ruled out by averaging across experiments. Opportunistic experiments have significantly improved process-level understanding of ACI, but it remains unclear how reliably the relationships found can be scaled to the global level, thus demonstrating a need for deeper investigation in order to improve assessments of aerosol radiative forcing and climate change. 

Abstract. Satellite cloud observations have become an indispensable tool for evaluatinggeneral circulation models (GCMs). To facilitate the satellite and GCMcomparisons, the CFMIP (Cloud Feedback Model Inter-comparison Project)Observation Simulator Package (COSP) has been developed and is nowincreasingly used in GCM evaluations. Real-world clouds and precipitation canhave significant sub-grid variations, which, however, are often ignored oroversimplified in the COSP simulation. In this study, we use COSP cloudsimulations from the Super-Parameterized Community Atmosphere Model (SPCAM5)and satellite observations from the Moderate Resolution ImagingSpectroradiometer (MODIS) and CloudSat to demonstrate the importance ofconsidering the sub-grid variability of cloud and precipitation when usingthe COSP to evaluate GCM simulations. We carry out two sensitivity tests:SPCAM5 COSP and SPCAM5-Homogeneous COSP. In the SPCAM5 COSP run, the sub-gridcloud and precipitation properties from the embeddedcloud-resolving model (CRM) of SPCAM5 are used to drive the COSP simulation, while inthe SPCAM5-Homogeneous COSP run only grid-mean cloud and precipitationproperties (i.e., no sub-grid variations) are given to the COSP. We find thatthe warm rain signatures in the SPCAM5 COSP run agree with the MODIS andCloudSat observations quite well. In contrast, the SPCAM5-Homogeneous COSPrun which ignores the sub-grid cloud variations substantially overestimatesthe radar reflectivity and probability of precipitation compared to thesatellite observations, as well as the results from the SPCAM5 COSP run. Thesignificant differences between the two COSP runs demonstrate that it isimportant to take into account the sub-grid variations of cloud andprecipitation when using COSP to evaluate the GCM to avoid confusing andmisleading results.