Philip Stier

Abstract:

The South-eastern Atlantic Ocean (SEA) is semi-permanently covered by one of the most extensive stratocumulus cloud decks on the planet and experiences about one-third of the global biomass burning emissions from the southern Africa savannah region during the fire season. To get a better understanding of the impact of these biomass burning aerosols on clouds and radiation balance over the SEA, the latest generation of the UK Earth System Model (UKESM1) is employed. Measurements from the CLARIFY and ORACLES flight campaigns are used to evaluate the model, demonstrating that the model has good skill in reproducing the biomass burning plume. To investigate the underlying mechanisms in detail, the effects of biomass burning aerosols on the clouds are decomposed into radiative effects (via absorption and scattering) and microphysical effects (via perturbation of cloud condensation nuclei (CCN) and cloud microphysical processes). The July-August means are used to characterise aerosols, clouds and the radiation balance during the fire season. Results show around 65% of CCN at 0.2% supersaturation in the SEA domain can be attributed to biomass burning. The absorption effect of biomass burning aerosols is the most significant in affecting clouds and radiation. Near the continent, it increases the maximum supersaturation diagnosed by the activation scheme, while further from the continent it reduces the altitude of the maximum supersaturation. As a result, the cloud droplet number concentration responds with a similar pattern to the absorption effect of biomass burning aerosols. The microphysical effect, however, decreases the maximum supersaturation and increases the cloud droplets concentration over the ocean; although this change is relatively small. The liquid water path is also significantly increased over the SEA (mainly caused by the absorption effect of biomass burning aerosols) when biomass burning aerosols are above the stratocumulus cloud deck. The microphysical pathways lead to a slight increase in the liquid water path over the ocean. These changes in cloud properties indicate the significant role of biomass burning aerosols on clouds in this region. Among the effects of biomass burning aerosols on the radiation balance, the semi-direct radiative effects (rapid adjustments induced by biomass burning aerosols radiative effects) have a dominant cooling impact over the SEA, which offset the warming direct radiative effect (radiative forcing from biomass burning aerosol–radiation interactions) and lead to overall net cooling radiative effect in the SEA. However, the magnitude and the sign of the semi-direct effects are sensitive to the relative location of biomass burning aerosols and clouds, reflecting the critical task of the accurate modelling of the biomass burning plume and clouds in this region.

Abstract:

We document and evaluate the aerosol schemes as implemented in the physical and Earth system models, the Global Coupled 3.1 configuration of the Hadley Centre Global Environment Model version 3 (HadGEM3-GC3.1) and the United Kingdom Earth System Model (UKESM1), which are contributing to the sixth Coupled Model Intercomparison Project (CMIP6). The simulation of aerosols in the present-day period of the historical ensemble of these models is evaluated against a range of observations. Updates to the aerosol microphysics scheme are documented as well as differences in the aerosol representation between the physical and Earth system configurations. The additional Earth system interactions included in UKESM1 lead to differences in the emissions of natural aerosol sources such as dimethyl sulfide, mineral dust and organic aerosol and subsequent evolution of these species in the model. UKESM1 also includes a stratospheric–tropospheric chemistry scheme which is fully coupled to the aerosol scheme, while GC3.1 employs a simplified aerosol chemistry mechanism driven by prescribed monthly climatologies of the relevant oxidants. Overall, the simulated speciated aerosol mass concentrations compare reasonably well with observations. Both models capture the negative trend in sulfate aerosol concentrations over Europe and the eastern United States of America (US) although the models tend to underestimate sulfate concentrations in both regions. Interactive emissions of biogenic volatile organic compounds in UKESM1 lead to an improved agreement of organic aerosol over the US. Simulated dust burdens are similar in both models despite a 2-fold difference in dust emissions. Aerosol optical depth is biased low in dust source and outflow regions but performs well in other regions compared to a number of satellite and ground-based retrievals of aerosol optical depth. Simulated aerosol number concentrations are generally within a factor of 2 of the observations, with both models tending to overestimate number concentrations over remote ocean regions, apart from at high latitudes, and underestimate over Northern Hemisphere continents. Finally, a new primary marine organic aerosol source is implemented in UKESM1 for the first time. The impact of this new aerosol source is evaluated. Over the pristine Southern Ocean, it is found to improve the seasonal cycle of organic aerosol mass and cloud droplet number concentrations relative to GC3.1 although underestimations in cloud droplet number concentrations remain. This paper provides a useful characterisation of the aerosol climatology in both models and will facilitate understanding in the numerous aerosol–climate interaction studies that will be conducted as part of CMIP6 and beyond.

Abstract:

The Twomey effect describes the radiative forcing associated with a change in cloud albedo due to an increase in anthropogenic aerosol emissions. It is driven by the perturbation in cloud droplet number concentration (ΔNd, ant) in liquid-water clouds and is currently understood to exert a cooling effect on climate. The Twomey effect is the key driver in the effective radiative forcing due to aerosol–cloud interactions, but rapid adjustments also contribute. These adjustments are essentially the responses of cloud fraction and liquid water path to ΔNd, ant and thus scale approximately with it. While the fundamental physics of the influence of added aerosol particles on the droplet concentration (Nd) is well described by established theory at the particle scale (micrometres), how this relationship is expressed at the large-scale (hundreds of kilometres) perturbation, ΔNd, ant, remains uncertain. The discrepancy between process understanding at particle scale and insufficient quantification at the climate-relevant large scale is caused by co-variability of aerosol particles and updraught velocity and by droplet sink processes. These operate at scales on the order of tens of metres at which only localised observations are available and at which no approach yet exists to quantify the anthropogenic perturbation. Different atmospheric models suggest diverse magnitudes of the Twomey effect even when applying the same anthropogenic aerosol emission perturbation. Thus, observational data are needed to quantify and constrain the Twomey effect. At the global scale, this means satellite data. There are four key uncertainties in determining ΔNd, ant, namely the quantification of (i) the cloud-active aerosol – the cloud condensation nuclei (CCN) concentrations at or above cloud base, (ii) Nd, (iii) the statistical approach for inferring the sensitivity of Nd to aerosol particles from the satellite data and (iv) uncertainty in the anthropogenic perturbation to CCN concentrations, which is not easily accessible from observational data. This review discusses deficiencies of current approaches for the different aspects of the problem and proposes several ways forward: in terms of CCN, retrievals of optical quantities such as aerosol optical depth suffer from a lack of vertical resolution, size and hygroscopicity information, non-direct relation to the concentration of aerosols, difficulty to quantify it within or below clouds, and the problem of insufficient sensitivity at low concentrations, in addition to retrieval errors. A future path forward can include utilising co-located polarimeter and lidar instruments, ideally including high-spectral-resolution lidar capability at two wavelengths to maximise vertically resolved size distribution information content. In terms of Nd, a key problem is the lack of operational retrievals of this quantity and the inaccuracy of the retrieval especially in broken-cloud regimes. As for the Nd-to-CCN sensitivity, key issues are the updraught distributions and the role of Nd sink processes, for which empirical assessments for specific cloud regimes are currently the best solutions. These considerations point to the conclusion that past studies using existing approaches have likely underestimated the true sensitivity and, thus, the radiative forcing due to the Twomey effect.