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This is the final version of the article. Available from European Geosciences Union (EGU) and Copernicus Publications via the DOI in this record. ; It is often implicitly assumed that over suitably long periods the mean of observations and models should be comparable, even if they have different temporal sampling. We assess the errors incurred due to ignoring temporal sampling and show that they are of similar magnitude as (but smaller than) actual model errors (20–60 %). Using temporal sampling from remote-sensing data sets, the satellite imager MODIS (MODerate resolution Imaging Spectroradiometer) and the ground-based sun photometer network AERONET (AErosol Robotic NETwork), and three different global aerosol models, we compare annual and monthly averages of full model data to sampled model data. Our results show that sampling errors as large as 100 % in AOT (aerosol optical thickness), 0.4 in AE (Ångström Exponent) and 0.05 in SSA (single scattering albedo) are possible. Even in daily averages, sampling errors can be significant. Moreover these sampling errors are often correlated over long distances giving rise to artificial contrasts between pristine and polluted events and regions. Additionally, we provide evidence that suggests that models will underestimate these errors. To prevent sampling errors, model data should be temporally collocated to the observations before any analysis is made. We also discuss how this work has consequences for in situ measurements (e.g. aircraft campaigns or surface measurements) in model evaluation. Although this study is framed in the context of model evaluation, it has a clear and direct relevance to climatologies derived from observational data sets. ; This work was supported by the Natural Environmental Research Council grant nr NE/J024252/1 (Global Aerosol Synthesis And Science Project). Computational resources for the ECHAM-HAM runs were made available by Deutsches Klimarechenzentrum (DKRZ) through support from the Bundesministerium für Bildung und Forschung (BMBF). The ECHAM-HAMMOZ model is developed by a consortium composed of ETH Zurich, Max Planck Institut für Meteorologie, Forschungszentrum Jülich, University of Oxford, the Finnish Meteorological Institute and the Leibniz Institute for Tropospheric Research, and managed by the Center for Climate Systems Modeling (C2SM) at ETH Zurich. P. Stier would like to acknowledge funding from the European Research Council under the European Union's Seventh Framework Programme (FP7/2007-2013) ERC project ACCLAIM (grant agreement no. FP7-280025). HadGEMUKCA was run on the ARCHER UK National Supercomputing Service (http://www.archer.ac.uk). The development of the UKCA model (www.ukca.ac.uk) was supported by the UK's Natural Environment Research Council (NERC) through the NERC Centres for Atmospheric Science (NCAS) initiative. MIROC-SPRINTARS was run on the SX-9 supercomputer at NIES (CGER) in Japan. The figures in this paper were prepared using David W. Fanning's coyote library for IDL. The authors thank an anonymous reviewer and in particular Andrew Sayer for useful comments that helped improve the manuscript.

This is the final version of the article. Available from EGU via the DOI in this record ; Many theories have been proposed detailing how aerosols might impact precipitation, predicting both increases and decreases depending on the prevailing meteorological conditions and aerosol type. In convective clouds, increased aerosol concentrations have been speculated to invigorate convective activity. Previous studies have shown large increases in precipitation with increasing aerosol optical depth, concluding an aerosol effect on precipitation. Our analysis reveals that these studies may have been influenced by cloud effects on the retrieved aerosol, as well as by meteorological covariations. We use a regime-based approach to separate out different cloud regimes, allowing for the study of aerosol–cloud interactions in individual cloud regimes. We account for the influence of cloud properties on the aerosol retrieval and make use of the diurnal sampling of the TRMM satellite and the TRMM merged precipitation product to investigate the precipitation development. We find that whilst there is little effect on precipitation at the time of the aerosol retrieval, in the 6 h after the aerosol retrieval, there is an increase in precipitation from cloud in high-aerosol environments, consistent with the invigoration hypothesis. Increases in lightning flash count with increased aerosol are also observed in this period. The invigoration effect appears to be dependent on the cloud-top temperature, with clouds with tops colder than 0 °C showing increases in precipitation at times after the retrieval, as well as increases in wet scavenging. Warm clouds show little change in precipitation development with increasing aerosol, suggesting ice processes are important for the invigoration of precipitation. ; This work was supported by a UK Natural Environment Research Council (NERC) DPhil studentship and funding from the European Research Council under the European Union's Seventh Framework Programme (FP7/2007-2013)/ERC grant agreement no. FP7-280025.

This is the final version of the article. Available from European Geosciences Union via the DOI in this record. ; Many different interactions between aerosols and clouds have been postulated, based on correlations between satellite retrieved aerosol and cloud properties. Previous studies highlighted the importance of meteorological covariations to the observed correlations. In this work, we make use of multiple temporally-spaced satellite retrievals to observe the development of cloud regimes. The observation of cloud regime development allows us to account for the influences of cloud fraction (CF) and meteorological factors on the aerosol retrieval. By accounting for the aerosol index (AI)-CF relationship, we reduce the influence of meteorological correlations compared to "snapshot" studies, finding that simple correlations overestimate any aerosol effect on CF by at least a factor of two. We find an increased occurrence of transitions into the stratocumulus regime over ocean with increases in MODIS AI, consistent with the hypothesis that aerosols increase stratocumulus persistence. We also observe an increase in transitions into the deep convective regime over land, consistent with the aerosol invigoration hypothesis. We find changes in the transitions from the shallow cumulus regime in different aerosol environments. The strength of these changes is strongly dependent on Low Troposphere Static Stability and 10 m windspeed, but less so on other meteorological factors. Whilst we have reduced the error due to meteorological and CF effects on the aerosol retrieval, meteorological covariation with the cloud and aerosol properties is harder to remove, so these results likely represent an upper bound on the effect of aerosols on cloud development and CF. ; This work was supported by a UK Natural Environment Research Council (NERC) DPhil studentship and funding from the European Research Council under the European Union's Seventh Framework Programme (FP7/2007–2013)/ERC grant agreement no. FP7-280025.

This is the final version of the article. Available from European Geosciences Union (EGU) and Copernicus Publications via the DOI in this record. ; In this study a novel framework for inverse modelling of cloud condensation nuclei (CCN) spectra is developed using Köhler theory. The framework is established by using model-generated synthetic measurements as calibration data for a parametric sensitivity analysis. Assessment of the relative importance of aerosol physicochemical parameters, while accounting for bulk–surface partitioning of surface-active organic species, is carried out over a range of atmospherically relevant supersaturations. By introducing an objective function that provides a scalar metric for diagnosing the deviation of modelled CCN concentrations from synthetic observations, objective function response surfaces are presented as a function of model input parameters. Crucially, for the chosen calibration data, aerosol–CCN spectrum closure is confirmed as a well-posed inverse modelling exercise for a subset of the parameters explored herein. The response surface analysis indicates that the appointment of appropriate calibration data is particularly important. To perform an inverse aerosol–CCN closure analysis and constrain parametric uncertainties, it is shown that a high-resolution CCN spectrum definition of the calibration data is required where single-valued definitions may be expected to fail. Using Köhler theory to model CCN concentrations requires knowledge of many physicochemical parameters, some of which are difficult to measure in situ on the scale of interest and introduce a considerable amount of parametric uncertainty to model predictions. For all partitioning schemes and environments modelled, model output showed significant sensitivity to perturbations in aerosol log-normal parameters describing the accumulation mode, surface tension, organic : inorganic mass ratio, insoluble fraction, and solution ideality. Many response surfaces pertaining to these parameters contain well-defined minima and are therefore good candidates for calibration using a Monte Carlo Markov Chain (MCMC) approach to constraining parametric uncertainties. A complete treatment of bulk–surface partitioning is shown to predict CCN spectra similar to those calculated using classical Köhler theory with the surface tension of a pure water drop, as found in previous studies. In addition, model sensitivity to perturbations in the partitioning parameters was found to be negligible. As a result, this study supports previously held recommendations that complex surfactant effects might be neglected, and the continued use of classical Köhler theory in global climate models (GCMs) is recommended to avoid an additional computational burden. The framework developed is suitable for application to many additional composition-dependent processes that might impact CCN activation potential. However, the focus of this study is to demonstrate the efficacy of the applied sensitivity analysis to identify important parameters in those processes and will be extended to facilitate a global sensitivity analysis and inverse aerosol–CCN closure analysis. ; This work was supported by the UK Natural Environment Research Council grants NE/I020148/1 (AerosolCloud Interactions – A Directed Programme to Reduce Uncertainty in Forcing) and NE/J024252/1 (Global Aerosol Synthesis And Science Project). P. Stier would like to acknowledge funding from the European Research Council under the European Union's Seventh Framework Programme (FP7/2007-2013) ERC project ACCLAIM (grant agreement no. FP7-280025).

This is the final version of the article. Available from European Geosciences Union (EGU) and Copernicus Publications via the DOI in this record. ; The activation of aerosols to form cloud droplets is dependent upon vertical velocities whose local variability is not typically resolved at the GCM grid scale. Consequently, it is necessary to represent the subgrid-scale variability of vertical velocity in the calculation of cloud droplet number concentration.This study uses the UK Chemistry and Aerosols community model (UKCA) within the Hadley Centre Global Environmental Model (HadGEM3), coupled for the first time to an explicit aerosol activation parameterisation, and hence known as UKCA-Activate. We explore the range of uncertainty in estimates of the indirect aerosol effects attributable to the choice of parameterisation of the subgrid-scale variability of vertical velocity in HadGEM-UKCA. Results of simulations demonstrate that the use of a characteristic vertical velocity cannot replicate results derived with a distribution of vertical velocities, and is to be discouraged in GCMs. This study focuses on the effect of the variance (σw2) of a Gaussian pdf (probability density function) of vertical velocity. Fixed values of σw (spanning the range measured in situ by nine flight campaigns found in the literature) and a configuration in which σw depends on turbulent kinetic energy are tested. Results from the mid-range fixed σw and TKE-based configurations both compare well with observed vertical velocity distributions and cloud droplet number concentrations.The radiative flux perturbation due to the total effects of anthropogenic aerosol is estimated at −1.9 W m−2 with σw = 0.1 m s−1, −2.1 W m−2 with σw derived from TKE, −2.25 W m−2 with σw= 0.4 m s−1, and −2.3 W m−2 with σw = 0.7 m s−1. The breadth of this range is 0.4 W m−2, which is comparable to a substantial fraction of the total diversity of current aerosol forcing estimates. Reducing the uncertainty in the parameterisation of σw would therefore be an important step towards reducing the uncertainty in estimates of the indirect aerosol effects. Detailed examination of regional radiative flux perturbations reveals that aerosol microphysics can be responsible for some climate-relevant radiative effects, highlighting the importance of including microphysical aerosol processes in GCMs. ; R. E. L. West and Z. Kipling both acknowledge the support of NERC studentships and receipt of CASE awards from the Met Office during the course of this work. P. Stier's research leading to these results has received funding from the European Research Council under the European Union's Seventh Framework Programme (FP7/2007-2013)/ERC grant agreement no. FP7-280025. A. Jones, C. E. Johnson and N. Bellouin were supported by the Joint DECC/Defra Met Office Hadley Centre Climate Programme (GA01101). Computing resources and support were provided by the Met Office/NERC Joint Weather and Climate Research Programme (JWCRP).

We apply different aerosol and aerosol precursor emission scenarios reflecting possible future control strategies for air pollution in the ECHAM5-HAM model, and simulate the resulting effect on the Earth's radiation budget. We use two opposing future mitigation strategies for the year 2030: one in which emission reduction legislation decided in countries throughout the world are effectively implemented (current legislation; CLE 2030) and one in which all technical options for emissions reductions are being implemented independent of their cost (maximum feasible reduction; MFR 2030). We consider the direct, semi-direct and indirect radiative effects of aerosols. The total anthropogenic aerosol radiative forcing defined as the difference in the top-of-the-atmosphere radiation between 2000 and pre-industrial times amounts to -2.00 W/m². In the future this negative global annual mean aerosol radiative forcing will only slightly change (+0.02 W/m²) under the "current legislation" scenario. Regionally, the effects are much larger: e.g. over Eastern Europe radiative forcing would increase by +1.50 W/m² because of successful aerosol reduction policies, whereas over South Asia it would decrease by -1.10 W/m² because of further growth of emissions. A "maximum feasible reduction" of aerosols and their precursors would lead to an increase of the global annual mean aerosol radiative forcing by +1.13 W/m². Hence, in the latter case, the present day negative anthropogenic aerosol forcing could be more than halved by 2030 because of aerosol reduction policies and climate change thereafter will be to a larger extent be controlled by greenhouse gas emissions. We combined these two opposing future mitigation strategies for a number of experiments focusing on different sectors and regions. In addition, we performed sensitivity studies to estimate the importance of the aerosol microphysical coupling within the range of expected future changes. For changes in oxidant concentrations caused by future air pollution mitigationm we do not ...

International audience ; We apply different aerosol and aerosol precursor emission scenarios reflecting possible future control strategies for air pollution in the ECHAM5-HAM model, and simulate the resulting effect on the Earth's radiation budget. We use two opposing future mitigation strategies for the year 2030: one in which emission reduction legislation decided in countries throughout the world are effectively implemented (current legislation; CLE 2030) and one in which all technical options for emission reductions are being implemented independent of their cost (maximum feasible reduction; MFR 2030). We consider the direct, semi-direct and indirect radiative effects of aerosols. The total anthropogenic aerosol radiative forcing defined as the difference in the top-of-the-atmosphere radiation between 2000 and pre-industrial times amounts to ?2.05 W/m 2 . In the future this negative global annual mean aerosol radiative forcing will only slightly change (+0.02 W/m 2 ) under the "current legislation" scenario. Regionally, the effects are much larger: e.g. over Eastern Europe radiative forcing would increase by +1.50 W/m 2 because of successful aerosol reduction policies, whereas over South Asia it would decrease by ?1.10 W/m 2 because of further growth of emissions. A "maximum feasible reduction" of aerosols and their precursors would lead to an increase of the global annual mean aerosol radiative forcing by +1.13 W/m 2 . Hence, in the latter case, the present day negative anthropogenic aerosol forcing cloud be more than halved by 2030 because of aerosol reduction policies and climate change thereafter will be to a larger extend be controlled by greenhouse gas emissions. We combined these two opposing future mitigation strategies for a number of experiments focusing on different sectors and regions. In addition, we performed sensitivity studies to estimate the importance of future changes in oxidant concentrations and the importance of the aerosol microphysical coupling within the range of expected future ...

This is the final version of the article. Available from EGU via the DOI in this record. ; Aerosol–cloud interactions continue to constitute a major source of uncertainty for the estimate of climate radiative forcing. The variation of aerosol indirect effects (AIE) in climate models is investigated across different dynamical regimes, determined by monthly mean 500 hPa vertical pressure velocity (ω500), lower-tropospheric stability (LTS) and large-scale surface precipitation rate derived from several global climate models (GCMs), with a focus on liquid water path (LWP) response to cloud condensation nuclei (CCN) concentrations. The LWP sensitivity to aerosol perturbation within dynamic regimes is found to exhibit a large spread among these GCMs. It is in regimes of strong large-scale ascent (ω500 0.1 mm day−1) contributes the most to the total aerosol indirect forcing (from 64 to nearly 100 %). Results show that the uncertainty in AIE is even larger within specific dynamical regimes compared to the uncertainty in its global mean values, pointing to the need to reduce the uncertainty in AIE in different dynamical regimes. ; M. Wang acknowledged the support from the Jiangsu Province Specially-appointed professorship grant and the One Thousand Young Talents Program and the National Natural Science Foundation of China (41575073). The contribution from Pacific Northwest National Laboratory was supported by the US Department of Energy (DOE), Office of Science, Decadal and Regional Climate Prediction using Earth System Models (EaSM program). H. Wang acknowledges support by the DOE Earth System Modeling program. The Pacific Northwest National Laboratory is operated for the DOE by Battelle Memorial Institute under contract DE-AC06-76RLO 1830. The ECHAM-HAMMOZ model is developed by a consortium composed of ETH Zurich, Max Planck Institut für Meteorologie, Forschungszentrum Jülich, University of Oxford, the Finnish Meteorological Institute and the Leibniz Institute for Tropospheric Research, and managed by the Center for Climate Systems Modeling (C2SM) at ETH Zurich. D. Neubauer gratefully acknowledges the support by the Austrian Science Fund (FWF): J 3402-N29 (Erwin Schrödinger Fellowship Abroad). The Center for Climate Systems Modeling (C2SM) at ETH Zurich is acknowledged for providing technical and scientific support. This work was supported by a grant from the Swiss National Supercomputing Centre (CSCS) under project ID s431. D. G. Partridge would like to acknowledge support from the UK Natural Environment Research Council project ACID-PRUF (NE/I020148/1) as well as thanks to N. Bellouin for useful discussions during the course of this work. The development of GLOMAP-mode within HadGEM is part of the UKCA project, which is supported by both NERC and the Joint DECC/Defra Met Office Hadley Centre Climate Programme (GA01101). We acknowledge use of the MONSooN system, a collaborative facility supplied under the Joint Weather and Climate Research Programme, a strategic partnership between the Met Office and the Natural Environment Research Council. P. Stier would like to acknowledge support from the European Research Council under the European Union's Seventh Framework Programme (FP7/2007-2013) / ERC grant agreement no. FP7-280025.