A newly developed multi-spectral radiative-transfer code is used to investigate the important features of the direct radiative forcing of sulphate and soot aerosol; the indirect effect of both aerosol species is not investigated in this study. The direct radiative forcing is presented for different surface albedos, solar zenith angles, relative humidities and aerosol vertical profiles together with effects upon the surface irradiance and long-wave radiative forcing. The effect of subgrid-scale variations in relative humidity are examined using idealized relative humidity distributions. The results show that subgrid-scale variations in relative humidity and the spatial correlation between cloud and areas of high relative humidity should be considered in future general-circulation model calculations of the direct forcing due to sulphate aerosol. A comparison of the direct forcing obtained by adjusting the surface albedo to that using the full multi-spectral column calculation is performed; the results indicate that recent estimates of the climate response to the direct forcing of sulphate may be too large. The contribution to the direct forcing from cloudy-sky regions appears to be negligible for sulphate aerosol but there is a considerable enhancement of the forcing due to soot aerosol if soot exists within or above clouds. These calculations show that a small amount of soot, relative to the sulphate mass loading, can cause a significant positive direct forcing and emphasize that the vertical profile of soot aerosol relative to cloud must be established to enable accurate assessment of the direct radiative effects of anthropogenic emissions of soot aerosol.

We describe the historical evolution of the conceptualization, formulation, quantification, application, and utilization of “radiative forcing” (RF) of Earth’s climate. Basic theories of shortwave and longwave radiation were developed through the nineteenth and twentieth centuries and established the analytical framework for defining and quantifying the perturbations to Earth’s radiative energy balance by natural and anthropogenic influences. The insight that Earth’s climate could be radiatively forced by changes in carbon dioxide, first introduced in the nineteenth century, gained empirical support with sustained observations of the atmospheric concentrations of the gas beginning in 1957. Advances in laboratory and field measurements, theory, instrumentation, computational technology, data, and analysis of well-mixed greenhouse gases and the global climate system through the twentieth century enabled the development and formalism of RF; this allowed RF to be related to changes in global-mean surface temperature with the aid of increasingly sophisticated models. This in turn led to RF becoming firmly established as a principal concept in climate science by 1990. The linkage with surface temperature has proven to be the most important application of the RF concept, enabling a simple metric to evaluate the relative climate impacts of different agents. The late 1970s and 1980s saw accelerated developments in quantification, including the first assessment of the effect of the forcing due to the doubling of carbon dioxide on climate (the “Charney” report). The concept was subsequently extended to a wide variety of agents beyond well-mixed greenhouse gases (WMGHGs; carbon dioxide, methane, nitrous oxide, and halocarbons) to short-lived species such as ozone. The WMO and IPCC international assessments began the important sequence of periodic evaluations and quantifications of the forcings by natural (solar irradiance changes and stratospheric aerosols resulting from volcanic eruptions) and a growing set of anthropogenic agents (WMGHGs, ozone, aerosols, land surface changes, contrails). From the 1990s to the present, knowledge and scientific confidence in the radiative agents acting on the climate system have proliferated. The conceptual basis of RF has also evolved as both our understanding of the way radiative forcing drives climate change and the diversity of the forcing mechanisms have grown. This has led to the current situation where “effective radiative forcing” (ERF) is regarded as the preferred practical definition of radiative forcing in order to better capture the link between forcing and global-mean surface temperature change. The use of ERF, however, comes with its own attendant issues, including challenges in its diagnosis from climate models, its applications to small forcings, and blurring of the distinction between rapid climate adjustments (fast responses) and climate feedbacks; this will necessitate further elaboration of its utility in the future. Global climate model simulations of radiative perturbations by various agents have established how the forcings affect other climate variables besides temperature (e.g., precipitation). The forcing–response linkage as simulated by models, including the diversity in the spatial distribution of forcings by the different agents, has provided a practical demonstration of the effectiveness of agents in perturbing the radiative energy balance and causing climate changes. The significant advances over the past half century have established, with very high confidence, that the global-mean ERF due to human activity since preindustrial times is positive (the 2013 IPCC assessment gives a best estimate of 2.3 W m−2, with a range from 1.1 to 3.3 W m−2; 90% confidence interval). Further, except in the immediate aftermath of climatically significant volcanic eruptions, the net anthropogenic forcing dominates over natural radiative forcing mechanisms. Nevertheless, the substantial remaining uncertainty in the net anthropogenic ERF leads to large uncertainties in estimates of climate sensitivity from observations and in predicting future climate impacts. The uncertainty in the ERF arises principally from the incorporation of the rapid climate adjustments in the formulation, the well-recognized difficulties in characterizing the preindustrial state of the atmosphere, and the incomplete knowledge of the interactions of aerosols with clouds. This uncertainty impairs the quantitative evaluation of climate adaptation and mitigation pathways in the future. A grand challenge in Earth system science lies in continuing to sustain the relatively simple essence of the radiative forcing concept in a form similar to that originally devised, and at the same time improving the quantification of the forcing. This, in turn, demands an accurate, yet increasingly complex and comprehensive, accounting of the relevant processes in the climate system.

Abstract. Volcanic eruptions can cause significant disruption to society, and numerical models are crucial for forecasting the dispersion of erupted material. Here we assess the skill and limitations of the Met Office's Numerical Atmospheric-dispersion Modelling Environment (NAME) in simulating the dispersion of the sulfur dioxide (SO2) cloud from the 21–22 June 2019 eruption of the Raikoke volcano (48.3∘ N, 153.2∘ E). The eruption emitted around 1.5±0.2 Tg of SO2, which represents the largest volcanic emission of SO2 into the stratosphere since the 2011 Nabro eruption. We simulate the temporal evolution of the volcanic SO2 cloud across the Northern Hemisphere (NH) and compare our model simulations to high-resolution SO2 measurements from the TROPOspheric Monitoring Instrument (TROPOMI) and the Infrared Atmospheric Sounding Interferometer (IASI) satellite SO2 products. We show that NAME accurately simulates the observed location and horizontal extent of the SO2 cloud during the first 2–3 weeks after the eruption but is unable, in its standard configuration, to capture the extent and precise location of the highest magnitude vertical column density (VCD) regions within the observed volcanic cloud. Using the structure–amplitude–location (SAL) score and the fractional skill score (FSS) as metrics for model skill, NAME shows skill in simulating the horizontal extent of the cloud for 12–17 d after the eruption where VCDs of SO2 (in Dobson units, DU) are above 1 DU. For SO2 VCDs above 20 DU, which are predominantly observed as small-scale features within the SO2 cloud, the model shows skill on the order of 2–4 d only. The lower skill for these high-SO2-VCD regions is partly explained by the model-simulated SO2 cloud in NAME being too diffuse compared to TROPOMI retrievals. Reducing the standard horizontal diffusion parameters used in NAME by a factor of 4 results in a slightly increased model skill during the first 5 d of the simulation, but on longer timescales the simulated SO2 cloud remains too diffuse when compared to TROPOMI measurements. The skill of NAME to simulate high SO2 VCDs and the temporal evolution of the NH-mean SO2 mass burden is dominated by the fraction of SO2 mass emitted into the lower stratosphere, which is uncertain for the 2019 Raikoke eruption. When emitting 0.9–1.1 Tg of SO2 into the lower stratosphere (11–18 km) and 0.4–0.7 Tg into the upper troposphere (8–11 km), the NAME simulations show a similar peak in SO2 mass burden to that derived from TROPOMI (1.4–1.6 Tg of SO2) with an average SO2 e-folding time of 14–15 d in the NH. Our work illustrates how the synergy between high-resolution satellite retrievals and dispersion models can identify potential limitations of dispersion models like NAME, which will ultimately help to improve dispersion modelling efforts of volcanic SO2 clouds.

Aerosols interact with radiation and clouds. Substantial progress made over the past 40 years in observing, understanding, and modeling these processes helped quantify the imbalance in the Earth's radiation budget caused by anthropogenic aerosols, called aerosol radiative forcing, but uncertainties remain large. This review provides a new range of aerosol radiative forcing over the industrial era based on multiple, traceable, and arguable lines of evidence, including modeling approaches, theoretical considerations, and observations. Improved understanding of aerosol absorption and the causes of trends in surface radiative fluxes constrain the forcing from aerosol-radiation interactions. A robust theoretical foundation and convincing evidence constrain the forcing caused by aerosol-driven increases in liquid cloud droplet number concentration. However, the influence of anthropogenic aerosols on cloud liquid water content and cloud fraction is less clear, and the influence on mixed-phase and ice clouds remains poorly constrained. Observed changes in surface temperature and radiative fluxes provide additional constraints. These multiple lines of evidence lead to a 68% confidence interval for the total aerosol effective radiative forcing of -1.6 to -0.6 W m −2 , or -2.0 to -0.4 W m −2 with a 90% likelihood. Those intervals are of similar width to the last Intergovernmental Panel on Climate Change assessment but shifted toward more negative values. The uncertainty will narrow in the future by continuing to critically combine multiple lines of evidence, especially those addressing industrial-era changes in aerosol sources and aerosol effects on liquid cloud amount and on ice clouds. Plain Language SummaryHuman activities emit into the atmosphere small liquid and solid particles called aerosols. Those aerosols change the energy budget of the Earth and trigger climate changes, by scattering and absorbing solar and terrestrial radiation and playing important roles in the formation of

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Abstract. Between 27 June and 14 July 2019 aerosol layers were observed by the United Kingdom (UK) Raman lidar network in the upper troposphere and lower stratosphere. The arrival of these aerosol layers in late June caused some concern within the London Volcanic Ash Advisory Centre (VAAC) as according to dispersion simulations the volcanic plume from the 21 June 2019 eruption of Raikoke was not expected over the UK until early July. Using dispersion simulations from the Met Office Numerical Atmospheric-dispersion Modelling Environment (NAME), and supporting evidence from satellite and in situ aircraft observations, we show that the early arrival of the stratospheric layers was not due to aerosols from the explosive eruption of the Raikoke volcano but due to biomass burning smoke aerosols associated with intense forest fires in Alberta, Canada, that occurred 4 d prior to the Raikoke eruption. We use the observations and model simulations to describe the dispersion of both the volcanic and forest fire aerosol clouds and estimate that the initial Raikoke ash aerosol cloud contained around 15 Tg of volcanic ash and that the forest fires produced around 0.2 Tg of biomass burning aerosol. The operational monitoring of volcanic aerosol clouds is a vital capability in terms of aviation safety and the synergy of NAME dispersion simulations, and lidar data with depolarising capabilities allowed scientists at the Met Office to interpret the various aerosol layers over the UK and attribute the material to their sources. The use of NAME allowed the identification of the observed stratospheric layers that reached the UK on 27 June as biomass burning aerosol, characterised by a particle linear depolarisation ratio of 9 %, whereas with the lidar alone the latter could have been identified as the early arrival of a volcanic ash–sulfate mixed aerosol cloud. In the case under study, given the low concentration estimates, the exact identification of the aerosol layers would have made little substantive difference to the decision-making process within the London VAAC. However, our work shows how the use of dispersion modelling together with multiple observation sources enabled us to create a more complete description of atmospheric aerosol loading.

Global mean lower stratosphere temperatures rose abruptly in January 2020 reaching values not experienced since the early 1990s. Anomalously high lower stratospheric temperatures were recorded for 4 months at highly statistically significant levels. Here, we use a combination of satellite and surface-based remote sensing observations to derive a time-series of stratospheric biomass burning aerosol optical depths originating from intense SouthEastern Australian wildfires and use these aerosol optical depths in a state-of-the-art climate model. We show that the S.E. Australian wildfires are the cause of this lower stratospheric warming. We also investigate the radiatively-driven dynamical response to the observed stratospheric ozone perturbation and find a significant strengthening of the springtime Antarctic polar vortex suggesting that biomass burning aerosols play a significant role in the observed anomalous longevity of the ozone hole in 2020.

<p><strong>Abstract.</strong> Here we show results from Earth System Model simulations from the marine cloud brightening experiment G4cdnc of the Geoengineering Model Intercomparison Project (GeoMIP). The nine contributing models prescribe a 50 % increase in the cloud droplet number concentration (CDNC) of low clouds over the global oceans, with the purpose of counteracting the radiative forcing due to anthropogenic greenhouse gases under the RCP4.5 scenario. The model ensemble median effective radiative forcing (ERF) amounts to −1.9 Wm<sup>−2</sup>, with a substantial inter-model spread of −0.6 to −2.5 Wm<sup>−2</sup>. The large spread is partly related to the considerable differences in clouds and their representation between the models, with an underestimation of low clouds in several of the models. All models predict a statistically significant temperature decrease with a median of (for years 2020–2060) −0.95 [−0.18 to −1.19] K relative to the RCP4.5 scenario, with particularly strong cooling over low-latitude continentss. Globally averaged there is a weak but significant precipitation decrease of −2.24 [−0.49 to −2.90] % due to a colder climate, but at low latitudes there is a 1.20 % increase over land. This increase is part of a circulation change where a strong negative TOA short-wave forcing over subtropical oceans, caused by increased albedo associated with the increasing CDNC, is compensated by rising motion and positive TOA long-wave signals over adjacent land regions.</p>