Abstract. With low concentrations of tropospheric aerosol, the Southern Ocean offers a “natural laboratory” for studies of aerosol–cloud interactions. Aerosols over the Southern Ocean are produced from biogenic activity in the ocean, which generates sulfate aerosol via dimethylsulfide (DMS) oxidation, and from strong winds and waves that lead to bubble bursting and sea spray emission. Here, we evaluate the representation of Southern Ocean aerosols in the Hadley Centre Global Environmental Model version 3, Global Atmosphere 7.1 (HadGEM3-GA7.1) chemistry–climate model. Compared with aerosol optical depth (AOD) observations from two satellite instruments (the Moderate Resolution Imaging Spectroradiometer, MODIS-Aqua c6.1, and the Multi-angle Imaging Spectroradiometer, MISR), the model simulates too-high AOD during winter and too-low AOD during summer. By switching off DMS emission in the model, we show that sea spray aerosol is the dominant contributor to AOD during winter. In turn, the simulated sea spray aerosol flux depends on near-surface wind speed. By examining MODIS AOD as a function of wind speed from the ERA-Interim reanalysis and comparing it with the model, we show that the sea spray aerosol source function in HadGEM3-GA7.1 overestimates the wind speed dependency. We test a recently developed sea spray aerosol source function derived from measurements made on a Southern Ocean research voyage in 2018. In this source function, the wind speed dependency of the sea spray aerosol flux is less than in the formulation currently implemented in HadGEM3-GA7.1. The new source function leads to good agreement between simulated and observed wintertime AODs over the Southern Ocean; however, it reveals partially compensating errors in DMS-derived AOD. While previous work has tested assumptions regarding the seawater climatology or sea–air flux of DMS, we test the sensitivity of simulated AOD, cloud condensation nuclei and cloud droplet number concentration to three atmospheric sulfate chemistry schemes. The first scheme adds DMS oxidation by halogens and the other two test a recently developed sulfate chemistry scheme for the marine troposphere; one tests gas-phase chemistry only, while the second adds extra aqueous-phase sulfate reactions. We show how simulated sulfur dioxide and sulfuric acid profiles over the Southern Ocean change as a result and how the number concentration and particle size of the soluble Aitken, accumulation and coarse aerosol modes are affected. The new DMS chemistry scheme leads to a 20 % increase in the number concentration of cloud condensation nuclei and cloud droplets, which improves agreement with observations. Our results highlight the importance of atmospheric chemistry for simulating aerosols and clouds accurately over the Southern Ocean.

<p><strong>Abstract.</strong> With low concentrations of tropospheric aerosol, the Southern Ocean offers a <q>natural laboratory</q> for studies of aerosol-cloud interactions. Aerosols over the Southern Ocean are produced from biogenic activity in the ocean, which generates sulfate aerosol via dimethylsulfide (DMS) oxidation, and from strong winds and waves that lead to bubble bursting and sea-spray emission. Here we evaluate the representation of Southern Ocean aerosols in the HadGEM3-GA7.1 chemistry-climate model. Compared with aerosol optical depth (AOD) observations from two satellite instruments (the Moderate Resolution Imaging Spectroradiometer, MODIS-Aqua c6.1 and the Multi-angle Imaging Spectroradiometer, MISR), the model simulates too-high AOD during winter and too-low AOD during summer. By switching off DMS emission in the model, we show that sea spray aerosol is the dominant contributor to AOD during winter. In turn, the simulated sea spray aerosol flux depends on near-surface wind speed. By examining MODIS AOD as a function of wind speed from the ERA-Interim reanalysis and comparing it with the model, we show that the sea spray aerosol source function in HadGEM3-GA7.1 overestimates the wind speed dependency. We test a recently-developed sea spray aerosol source function derived from measurements made on a Southern Ocean research voyage in 2018. In this source function the wind speed dependency of the sea spray aerosol flux is less than in the formulation currently implemented in HadGEM3-GA7.1. The new source function leads to good agreement between simulated and observed wintertime AOD over the Southern Ocean, however reveals partially compensating errors in DMS-derived AOD. While previous work has tested assumptions regarding the seawater climatology or sea-air flux of DMS, we test the sensitivity of simulated AOD, cloud condensation nuclei and cloud droplet number concentration to three atmospheric sulfate chemistry schemes. The first scheme adds DMS oxidation by halogens and the other two test a recently-developed sulfate chemistry scheme for the marine troposphere; one tests gas-phase chemistry only while the second adds extra aqueous-phase sulfate reactions. We show how simulated sulfur dioxide and sulfuric acid profiles over the Southern Ocean change as a result, and how the number concentration and particle size of the soluble Aitken, accumulation and coarse aerosol modes are affected. The new DMS chemistry scheme leads to a 20 % increase in the number concentration of cloud condensation nuclei and cloud droplets, which improves agreement with observations. Our results highlight the importance of atmospheric chemistry for simulating aerosols and clouds accurately over the Southern Ocean.</p>

Abstract. Wetlands are the largest global natural methane (CH4) source, and emissions between 50 and 70° N latitude contribute 10–30 % to this source. Predictive capability of land models for northern wetland CH4 emissions is still low due to limited site measurements, strong spatial and temporal variability in emissions, and complex hydrological and biogeochemical dynamics. To explore this issue, we compare wetland CH4 emission predictions from the Community Land Model 4.5 (CLM4.5-BGC) with site- to regional-scale observations. A comparison of the CH4 fluxes with eddy flux data highlighted needed changes to the model's estimate of aerenchyma area, which we implemented and tested. The model modification substantially reduced biases in CH4 emissions when compared with CarbonTracker CH4 predictions. CLM4.5 CH4 emission predictions agree well with growing season (May–September) CarbonTracker Alaskan regional-level CH4 predictions and site-level observations. However, CLM4.5 underestimated CH4 emissions in the cold season (October–April). The monthly atmospheric CH4 mole fraction enhancements due to wetland emissions are also assessed using the Weather Research and Forecasting-Stochastic Time-Inverted Lagrangian Transport (WRF-STILT) model coupled with daily emissions from CLM4.5 and compared with aircraft CH4 mole fraction measurements from the Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE) campaign. Both the tower and aircraft analyses confirm the underestimate of cold-season CH4 emissions by CLM4.5. The greatest uncertainties in predicting the seasonal CH4 cycle are from the wetland extent, cold-season CH4 production and CH4 transport processes. We recommend more cold-season experimental studies in high-latitude systems, which could improve the understanding and parameterization of ecosystem structure and function during this period. Predicted CH4 emissions remain uncertain, but we show here that benchmarking against observations across spatial scales can inform model structural and parameter improvements.

Southern Ocean (SO) shortwave (SW) radiation biases are a common problem in contemporary general circulation models (GCMs), with most models exhibiting a tendency to absorb too much incoming SW radiation. These biases have been attributed to deficiencies in the representation of clouds during the austral summer months, either due to cloud cover or cloud optical thickness being too low. The problem has been the focus of many studies, most of which utilised satellite datasets for model evaluation. We use multi-year ship based observations and the CERES spaceborne radiation budget measurements to 5 contrast cloud representation and SW radiation in the atmospheric component Global Atmosphere (GA) version 7.0 and 7.1 of the HadGEM3 GCM and the MERRA-2 reanalysis. We find that MERRA-2 is biased in the opposite direction to GA (reflects too much SW radiation). In addition, MERRA-2 performs better in terms of absolute SW bias than nudged runs of GA7.0 and GA7.1 in the 60-70 • S latitude band. GA7.1 reduces the SO SW radiation biases relative to GA7.0, but significant errors remain at up to 20 Wm −2 between 60 and 70 • S in the austral summer months. Using ship-based ceilometer observations, we find low 10 cloud below 2 km to be predominant in the Ross Sea and the Indian Ocean sector of the SO. Utilising a novel surface lidar simulator developed for this study, derived from an existing COSP-ACTSIM spaceborne lidar simulator, we find that GA7.0 and MERRA-2 both underestimate low cloud occurrence relative to the ship observations by 18-25% on average, though the cloud cover in MERRA-2 is closer to observations by about 7%. Based on radiosonde observations, we also find the low cloud to be strongly linked to boundary-layer atmospheric stability and the sea surface temperature. GA7.0 and MERRA-2 agree 15 well with observations in terms of boundary-layer stability, suggesting that subgrid-scale parametrisations do not generate enough cloud in response to the thermodynamic profile of the atmosphere and the surface temperature. Our analysis shows that MERRA-2 has a much greater proportion of cloud liquid water in the SO in January than GA7.0, a likely key contributor to the difference in SW radiation. We show that boundary-layer stability and relative humidity fields are very similar in GA7.0 and Atmos. Chem. Phys. Discuss., https://doi.

Abstract. Southern Ocean (SO) shortwave (SW) radiation biases are a common problem in contemporary general circulation models (GCMs), with most models exhibiting a tendency to absorb too much incoming SW radiation. These biases have been attributed to deficiencies in the representation of clouds during the austral summer months, either due to cloud cover or cloud albedo being too low. The problem has been the focus of many studies, most of which utilised satellite datasets for model evaluation. We use multi-year ship-based observations and the CERES spaceborne radiation budget measurements to contrast cloud representation and SW radiation in the atmospheric component Global Atmosphere (GA) version 7.1 of the HadGEM3 GCM and the MERRA-2 reanalysis. We find that the prevailing bias is negative in GA7.1 and positive in MERRA-2. GA7.1 performs better than MERRA-2 in terms of absolute SW bias. Significant errors of up to 21 W m−2 (GA7.1) and 39 W m−2 (MERRA-2) are present in both models in the austral summer. Using ship-based ceilometer observations, we find low cloud below 2 km to be predominant in the Ross Sea and the Indian Ocean sectors of the SO. Utilising a novel surface lidar simulator developed for this study, derived from an existing Cloud Feedback Model Intercomparison Project (CFMIP) Observation Simulator Package (COSP) – active remote sensing simulator (ACTSIM) spaceborne lidar simulator, we find that GA7.1 and MERRA-2 both underestimate low cloud and fog occurrence relative to the ship observations on average by 4 %–9 % (GA7.1) and 18 % (MERRA-2). Based on radiosonde observations, we also find the low cloud to be strongly linked to boundary layer atmospheric stability and the sea surface temperature. GA7.1 and MERRA-2 do not represent the observed relationship between boundary layer stability and clouds well. We find that MERRA-2 has a much greater proportion of cloud liquid water in the SO in austral summer than GA7.1, a likely key contributor to the difference in the SW radiation bias. Our results suggest that subgrid-scale processes (cloud and boundary layer parameterisations) are responsible for the bias and that in GA7.1 a major part of the SW radiation bias can be explained by cloud cover underestimation, relative to underestimation of cloud albedo.