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Large biases in climate model simulations of cloud radiative properties over the Southern Ocean cause large errors in modeled sea surface temperatures, atmospheric circulation, and climate sensitivity. Here, we combine cloud-resolving model simulations with estimates of the concentration of ice-nucleating particles in this region to show that our simulated Southern Ocean clouds reflect far more radiation than predicted by global models, in agreement with satellite observations. Specifically, we show that the clouds that are most sensitive to the concentration of ice-nucleating particles are low-level mixed-phase clouds in the cold sectors of extratropical cyclones, which have previously been identified as a main contributor to the Southern Ocean radiation bias. The very low ice-nucleating particle concentrations that prevail over the Southern Ocean strongly suppress cloud droplet freezing, reduce precipitation, and enhance cloud reflectivity. The results help explain why a strong radiation bias occurs mainly in this remote region away from major sources of ice-nucleating particles. The results present a substantial challenge to climate models to be able to simulate realistic ice-nucleating particle concentrations and their effects under specific meteorological conditions.

The rapid adjustment, or semi-direct effect, of marine stratocumulus clouds to elevated layers of absorbing aerosols may enhance or dampen the radiative effect of aerosol–radiation interactions. Here we use large-eddy simulations to investigate the sensitivity of stratocumulus clouds to the properties of an absorbing aerosol layer located above the inversion layer, with a focus on the location, timing, and strength of the radiative heat perturbation. The sign of the daily mean semi-direct effect depends on the properties and duration of the aerosol layer, the properties of the boundary layer, and the model setup. Our results suggest that the daily mean semi-direct effect is more elusive than previously assessed. We find that the daily mean semi-direct effect is dominated by the distance between the cloud and absorbing aerosol layer. Within the first 24 h the semi-direct effect is positive but remains under 2 W m−2 unless the aerosol layer is directly above the cloud. For longer durations, the daily mean semi-direct effect is consistently negative but weakens by 30 %, 60 %, and 95 % when the distance between the cloud and aerosol layer is 100, 250, and 500 m, respectively. Both the cloud response and semi-direct effect increase for thinner and denser layers of absorbing aerosol. Considerable diurnal variations in the cloud response mean that an instantaneous semi-direct effect is unrepresentative of the daily mean and that observational studies may underestimate or overestimate semi-direct effects depending on the observed time of day. The cloud response is particularly sensitive to the mixing state of the boundary layer: well-mixed boundary layers generally result in a negative daily mean semi-direct effect, and poorly mixed boundary layers result in a positive daily mean semi-direct effect. The properties of the boundary layer and model setup, particularly the sea surface temperature, precipitation, and properties of the air entrained from the free troposphere, also impact the magnitude of the semi-direct effect and the timescale of adjustment. These results suggest that the semi-direct effect simulated by coarse-resolution models may be erroneous because the cloud response is sensitive to small-scale processes, especially the sources and sinks of buoyancy.

Convective cloud systems in the maritime tropics play a critical role in global climate, but accurately representing aerosol interactions within these clouds persists as a major challenge for weather and climate modelling. We quantify the effect of ice-nucleating particles (INPs) on the radiative properties of a complex tropical Atlantic deep convective cloud field using a regional model with an advanced double-moment microphysics scheme. Our results show that the domain-mean daylight outgoing radiation varies by up to 18 W m−2 depending on the chosen INP parameterisation. The key distinction between different INP parameterisations is the temperature dependence of ice formation, which alters the vertical distribution of cloud microphysical processes. The controlling effect of the INP temperature dependence is substantial even in the presence of Hallett–Mossop secondary ice production, and the effects of secondary ice formation depend strongly on the chosen INP parameterisation. Our results have implications for climate model simulations of tropical clouds and radiation, which currently do not consider a link between INP particle type and ice water content. The results also provide a challenge to the INP measurement community, as we demonstrate that INP concentration measurements are required over the full mixed-phase temperature regime, which covers around 10 orders of magnitude.

A 1200×1200 km2 area of the tropical South Atlantic Ocean near Ascension Island is studied with the HadGEM climate model at convection-permitting and global resolutions for a 10-day case study period in August 2016. During the simulation period, a plume of biomass burning smoke from Africa moves into the area and mixes into the clouds. At Ascension Island, this smoke episode was the strongest of the 2016 fire season.The region of interest is simulated at 4 km resolution, with no parameterised convection scheme. The simulations are driven by, and compared to, the global model. For the first time, the UK Chemistry and Aerosol model (UKCA) is included in a regional model with prognostic aerosol number concentrations advecting in from the global model at the boundaries of the region.Fire emissions increase the total aerosol burden by a factor of 3.7 and cloud droplet number concentrations by a factor of 3, which is consistent with MODIS observations. In the regional model, the inversion height is reduced by up to 200 m when smoke is included. The smoke also affects precipitation, to an extent which depends on the model microphysics. The microphysical and dynamical changes lead to an increase in liquid water path of 60 g m−2 relative to a simulation without smoke aerosol, when averaged over the polluted period. This increase is uncertain, and smaller in the global model. It is mostly due to radiatively driven dynamical changes rather than precipitation suppression by aerosol.Over the 5-day polluted period, the smoke has substantial direct radiative effects of +11.4 W m−2 in the regional model, a semi-direct effect of −30.5 W m−2 and an indirect effect of −10.1 W m−2. Our results show that the radiative effects are sensitive to the structure of the model (global versus regional) and the parameterization of rain autoconversion. Furthermore, we simulate a liquid water path that is biased high compared to satellite observations by 22 % on average, and this leads to high estimates of the domain-averaged aerosol direct effect and the effect of the aerosol on cloud albedo. With these caveats, we simulate a large net cooling across the region, of −27.6 W m−2.

Changes induced by perturbed aerosol conditions in moderately deep mixed-phase convective clouds (cloud top height ∼ 5 km) developing along sea-breeze convergence lines are investigated with high-resolution numerical model simulations. The simulations utilise the newly developed Cloud–AeroSol Interacting Microphysics (CASIM) module for the Unified Model (UM), which allows for the representation of the two-way interaction between cloud and aerosol fields. Simulations are evaluated against observations collected during the COnvective Precipitation Experiment (COPE) field campaign over the southwestern peninsula of the UK in 2013. The simulations compare favourably with observed thermodynamic profiles, cloud base cloud droplet number concentrations (CDNC), cloud depth, and radar reflectivity statistics. Including the modification of aerosol fields by cloud microphysical processes improves the correspondence with observed CDNC values and spatial variability, but reduces the agreement with observations for average cloud size and cloud top height. Accumulated precipitation is suppressed for higher-aerosol conditions before clouds become organised along the sea-breeze convergence lines. Changes in precipitation are smaller in simulations with aerosol processing. The precipitation suppression is due to less efficient precipitation production by warm-phase microphysics, consistent with parcel model predictions. In contrast, after convective cells organise along the sea-breeze convergence zone, accumulated precipitation increases with aerosol concentrations. Condensate production increases with the aerosol concentrations due to higher vertical velocities in the convective cores and higher cloud top heights. However, for the highest-aerosol scenarios, no further increase in the condensate production occurs, as clouds grow into an upper-level stable layer. In these cases, the reduced precipitation efficiency (PE) dominates the precipitation response and no further precipitation enhancement occurs. Previous studies of deep convective clouds have related larger vertical velocities under high-aerosol conditions to enhanced latent heating from freezing. In the presented simulations changes in latent heating above the 0∘C are negligible, but latent heating from condensation increases with aerosol concentrations. It is hypothesised that this increase is related to changes in the cloud field structure reducing the mixing of environmental air into the convective core. The precipitation response of the deeper mixed-phase clouds along well-established convergence lines can be the opposite of predictions from parcel models. This occurs when clouds interact with a pre-existing thermodynamic environment and cloud field structural changes occur that are not captured by simple parcel model approaches.

We perform a model intercomparison of summertime high Arctic (> 80∘ N) clouds observed during the 2008 Arctic Summer Cloud Ocean Study (ASCOS) campaign, when observed cloud condensation nuclei (CCN) concentrations fell below 1 cm−3. Previous analyses have suggested that at these low CCN concentrations the liquid water content (LWC) and radiative properties of the clouds are determined primarily by the CCN concentrations, conditions that have previously been referred to as the tenuous cloud regime. The intercomparison includes results from three large eddy simulation models (UCLALES-SALSA, COSMO-LES, and MIMICA) and three numerical weather prediction models (COSMO-NWP, WRF, and UM-CASIM). We test the sensitivities of the model results to different treatments of cloud droplet activation, including prescribed cloud droplet number concentrations (CDNCs) and diagnostic CCN activation based on either fixed aerosol concentrations or prognostic aerosol with in-cloud processing. There remains considerable diversity even in experiments with prescribed CDNCs and prescribed ice crystal number concentrations (ICNC). The sensitivity of mixed-phase Arctic cloud properties to changes in CDNC depends on the representation of the cloud droplet size distribution within each model, which impacts autoconversion rates. Our results therefore suggest that properly estimating aerosol–cloud interactions requires an appropriate treatment of the cloud droplet size distribution within models, as well as in situ observations of hydrometeor size distributions to constrain them. The results strongly support the hypothesis that the liquid water content of these clouds is CCN limited. For the observed meteorological conditions, the cloud generally did not collapse when the CCN concentration was held constant at the relatively high CCN concentrations measured during the cloudy period, but the cloud thins or collapses as the CCN concentration is reduced. The CCN concentration at which collapse occurs varies substantially between models. Only one model predicts complete dissipation of the cloud due to glaciation, and this occurs only for the largest prescribed ICNC tested in this study. Global and regional models with either prescribed CDNCs or prescribed aerosol concentrations would not reproduce these dissipation events. Additionally, future increases in Arctic aerosol concentrations would be expected to decrease the frequency of occurrence of such cloud dissipation events, with implications for the radiative balance at the surface. Our results also show that cooling of the sea-ice surface following cloud dissipation increases atmospheric stability near the surface, further suppressing cloud formation. Therefore, this suggests that linkages between aerosol and clouds, as well as linkages between clouds, surface temperatures, and atmospheric stability need to be considered for weather and climate predictions in this region.

Aerosol-cloud interactions are a major source of uncertainty in inferring the climate sensitivity from the observational record of temperature. The adjustment of clouds to aerosol is a poorly constrained aspect of these aerosol-cloud interactions. Here, we examine the response of midlatitude cyclone cloud properties to a change in cloud droplet number concentration (CDNC). Idealized experiments in high-resolution, convection-permitting global aquaplanet simulations with constant CDNC are compared to 13 years of remote-sensing observations. Observations and idealized aquaplanet simulations agree that increased warm conveyor belt (WCB) moisture flux into cyclones is consistent with higher cyclone liquid water path (CLWP). When CDNC is increased a larger LWP is needed to give the same rain rate. The LWP adjusts to allow the rain rate to be equal to the moisture flux into the cyclone along the WCB. This results in an increased CLWP for higher CDNC at a fixed WCB moisture flux in both observations and simulations. If observed cyclones in the top and bottom tercile of CDNC are contrasted it is found that they have not only higher CLWP but also cloud cover and albedo. The difference in cyclone albedo between the cyclones in the top and bottom third of CDNC is observed by CERES to be between 0.018 and 0.032, which is consistent with a 4.6-8.3 Wm(exp -2) in-cyclone enhancement in upwelling shortwave when scaled by annual-mean insolation. Based on a regression model to observed cyclone properties, roughly 60% of the observed variability in CLWP can be explained by CDNC and WCB moisture flux.

We describe and evaluate a system for regional modeling of atmospheric composition with the Met Office Unified Model (UM), suitable for climate, weather forecasting and air quality applications. In this system, named NUMAC (“Nested UM with Aerosols and Chemistry”), a global model provides boundary conditions for regional models nested within it, using the Met Office's Regional Nesting Suite for multi‐scale simulations. The regional models, which can run at convection‐permitting or cloud‐resolving scales, use the same code as the global model. The system includes double‐moment prognostic aerosol microphysics with interactive chemistry of sulfur species, ozone, NOx, and CO as in the UK Earth System Model. Double‐moment prognostic cloud microphysics is optional. To test NUMAC, we compare simulations to surface and aircraft measurements from NASA's Korea‐United States Air Quality campaign over South Korea. The performance of the regional model, which we run at 5 km resolution, is similar to the well‐evaluated global model when the regional and global models use the same emissions. Most species such as ozone, NOx, OH, or PM2.5 are simulated within a factor of 2 of observations most of the time, though they are biased low compared to monitors in polluted areas (observed surface dry PM2.5 averages 28 μgm−3 but we simulate 17 μgm−3). Meteorology and clouds are represented satisfactorily. With higher‐resolution emissions, many of the low model biases are reduced, but a tuning was required to keep NO concentrations realistic, indicating shortcomings in the chemistry scheme. We demonstrate the potential of NUMAC for studies of aerosol‐cloud interactions. Plain Language Summary Unified atmospheric simulation systems, defined as those that are routinely used to represent air quality, weather and climate with the same code, are rare. The UK Met Office Unified Model (UM) is one such system, but until recently, aerosol‐cloud interactions were represented only in global climate simulations. Effects of aerosol‐cloud interactions and atmospheric chemistry on Earth's radiation balance are large and must be included in global and regional climate predictions. However, partly because clouds and emissions are spatially inhomogeneous, their effects on climate are currently poorly understood. Simulations with high grid resolution can help us understand the relevant processes better. We document here a system for representing air quality, weather and climate with the UM, including chemistry‐aerosol‐cloud interactions, at high spatial grid resolution on regional scales. We test our system against surface and aircraft measurements of atmospheric chemical species such as ozone and particulate matter made in May 2016 in Korea. The model represents most species well, but has some shortcomings we must address in future work. Overall, however, we judge that it is ready for studies of how atmospheric chemical species and particulate matter affect air quality, weather and climate, and can be further improved as it is used. Key Points We introduce a system for simulations of regional air quality and aerosol‐climate interactions with the UK Met Office Unified Model We evaluate the model against data from NASA's Korea‐United States Air Quality campaign in 2016 over South Korea Despite shortcomings in the representation of some chemical and aerosol species, the system is ready for application and further development

Aerosols have a potentially large effect on climate, particularly through their interactions with clouds, but the magnitude of this effect is highly uncertain. Large volcanic eruptions produce sulfur dioxide, which in turn produces aerosols; these eruptions thus represent a natural experiment through which to quantify aerosol-cloud interactions. Here we show that the massive 2014-2015 fissure eruption in Holuhraun, Iceland, reduced the size of liquid cloud droplets - consistent with expectations - but had no discernible effect on other cloud properties. The reduction in droplet size led to cloud brightening and global-mean radiative forcing of around minus 0.2 watts per square metre for September to October 2014. Changes in cloud amount or cloud liquid water path, however, were undetectable, indicating that these indirect effects, and cloud systems in general, are well buffered against aerosol changes. This result will reduce uncertainties in future climate projections, because we are now able to reject results from climate models with an excessive liquid-water-path response.

Aerosols play a crucial role in the fog life cycle, as they determine the droplet number concentration and hence droplet size, which in turn controls both the fog's optical thickness and lifespan. Detailed aerosol-microphysics schemes which accurately represent droplet formation and growth are unsuitable for weather forecasting and climate models, as the computational power required to calculate droplet formation would dominate the treatment of the rest of the physics in the model. A simple method to account for droplet formation is the use of an aerosol activation scheme, which parameterises the droplet number concentration based on a change in supersaturation at a given time. Traditionally, aerosol activation parameterisation schemes were designed for convective clouds and assume that supersaturation is reached through adiabatic lifting, with many imposing a minimum vertical velocity (e.g. 0.1 m s−1) to account for the unresolved subgrid ascent. In radiation fog, the measured updraughts during initial formation are often insignificant, with radiative cooling being the dominant process leading to saturation. As a result, there is a risk that many aerosol activation schemes will overpredict the initial fog droplet number concentration, which in turn may result in the fog transitioning to an optically thick layer too rapidly. This paper presents a more physically based aerosol activation scheme that can account for a change in saturation due to non-adiabatic processes. Using an offline model, our results show that the equivalent cooling rate associated with the minimum updraught velocity threshold assumption can overpredict the droplet number by up to 70 % in comparison to a typical cooling rate found in fog formation. The new scheme has been implemented in the Met Office Natural Environment Research Council (NERC) Cloud (MONC) large eddy simulation (LES) model and tested using observations of a radiation fog case study based in Cardington, UK. The results in this work show that using a more physically based method of aerosol activation leads to the calculation of a more appropriate cloud droplet number. As a result, there is a slower transition to an optically thick (well-mixed) fog that is more in line with observations. The results shown in this paper demonstrate the importance of aerosol activation representation in fog modelling and the impact that the cloud droplet number has on processes linked to the formation and development of radiation fog. Unlike the previous parameterisation for aerosol activation, the revised scheme is suitable to simulate aerosol activation in both fog and convective cloud regimes.