In-cloud scavenging scheme for sectional aerosol modules – implementation in the framework of the Sectional Aerosol module for Large Scale Applications version 2.0 (SALSA2.0) global aerosol module

In this study we introduce an in-cloud wet deposition scheme for liquid and ice phase clouds for global aerosol–climate models which use a size-segregated aerosol description. For in-cloud nucleation scavenging, the scheme uses cloud droplet activation and ice nucleation rates obtained from the host model. For in-cloud impaction scavenging, we used a method where the removal rate depends on the wet aerosol size and cloud droplet radii. We used the latest release version of ECHAM-HAMMOZ (ECHAM6.3-HAM2.3-MOZ1.0) with the Sectional Aerosol module for Large Scale Applications version 2.0 (SALSA) microphysics package to test and compare our scheme. The scheme was compared to a scheme that uses fixed scavenging coefficients. The comparison included vertical profiles and mass and number distributions of wet deposition fluxes of different aerosol compounds and for different latitude bands. Using the scheme presented here, mass concentrations for black carbon, organic carbon, sulfate, and the number concentration of particles with diameters larger than 100 nm are higher than using fixed scavenging coefficients, with the largest differences in the vertical profiles in the Arctic. On the other hand, the number concentrations of particles smaller than 100 nm in diameter show a decrease, especially in the Arctic region. These results could indicate that, compared to fixed scavenging coefficients, nucleation scavenging is less efficient, resulting in an increase in the number concentration of particles larger than 100 nm. In addition, changes in rates of impaction scavenging and new particle formation (NPF) can be the main cause of reduction in the number concentrations of particles smaller than 100 nm. Without further adjustments in the host model, our wet deposition scheme produced unrealistically high aerosol concentrations, especially at high altitudes. This also leads to a spuriously long lifetime of black carbon aerosol. To find a better setup for simulating aerosol vertical profiles and transport, sensitivity simulations were conducted where aerosol emission distribution and hygroscopicity were altered. Vertical profiles of aerosol species simulated with the scheme which uses fixed scavenging rates and the abovementioned sensitivity simulations were evaluated against vertical profiles from aircraft observations. The lifetimes of different aerosol compounds were also evaluated against the ensemble mean of models involved in the Aerosol Comparisons between Observations and Models (AEROCOM) project. The best comparison between the observations and the model was achieved with our wet deposition scheme when black carbon was emitted internally mixed with soluble compounds instead of keeping it externally mixed. This also produced atmospheric lifetimes for the other species which were comparable to the AEROCOM model means.

In-cloud scavenging scheme for aerosol modules

In this study we introduce an in-cloud wet deposition scheme for liquid and ice phase clouds for global aerosol-climate models which use a size-segregated aerosol description. For in-cloud nucleation scavenging, the scheme uses cloud droplet activation and ice nucleation rates obtained from the host model. For in-cloud impaction scavenging, we used a method where the removal rate depends on the aerosol size and cloud droplet radii. The scheme was compared to a scheme that uses fixed scavenging coefficients. The comparison included vertical profiles and mass and number distributions of wet deposition fluxes of different aerosol compounds and for different latitude bands. Using the scheme presented here, mass concentrations for black carbon, organic carbon, sulfate, and the number concentration of particles with diameters larger than 100 nm are higher than using fixed scavenging coefficients, with the largest differences in the vertical profiles in the Arctic. On the other hand, the number concentrations of small particles show a decrease, especially in the Arctic region. These results indicate that, compared to using fixed scavenging coefficients, nucleation scavenging is less efficient and impaction scavenging is increased in the scheme introduced here. Without further adjustments in the host model, our wet deposition scheme produced unrealistically high aerosol concentrations, especially at high altitudes. This also leads to a spuriously long lifetime of black carbon aerosol. To find a better setup for simulating aerosol vertical profiles and transport, sensitivity simulations were conducted where aerosol emission distribution and hygroscopicity were altered. The simulated vertical profiles of aerosol in these sensitivity studies were evaluated against aircraft observations. The lifetimes of different aerosol compounds were also evaluated against the ensemble mean of models involved in the Aerosol Comparisons between Observations and Models (AEROCOM) project. The best comparison between the observations and the model was achieved with the new wet deposition scheme when black carbon was emitted internally mixed with soluble compounds instead of keeping it externally mixed. This also produced atmospheric lifetimes for the other species which were comparable to the AEROCOM model means.

Size-dependent wet removal of black carbon in Canadian biomass burning plumes

Wet deposition is the dominant mechanism for removing black carbon (BC) from the atmosphere and is key in determining its atmospheric lifetime, vertical gradient and global transport. Despite the importance of BC in the climate system, especially in terms of its ability to modulate the radiative energy budget, there are few quantitative case studies of wet removal in ambient environments. We present a case study of BC wet removal by examining aerosol size distributions and BC coating properties sampled in three Canadian boreal biomass burning plumes, one of which passed through a precipitating cloud. This depleted the majority of the plume's BC mass, and the largest and most coated BC-containing particles were found to be preferentially removed, suggesting that nucleation scavenging was likely the dominant mechanism. Calculated single-scattering albedo (SSA) showed little variation, as a large number of non-BC particles were also present in the precipitation-affected plume. The remaining BC cores were smaller than those observed in previous studies of BC in post-precipitation outflow over Asia, possibly due to the thick coating by hydrophilic compounds associated with the Canadian biomass burning particles. This study provides measurements of BC size, mixing state and removal efficiency to constrain model parameterisations of BC wet removal in biomass burning regions, which will help to reduce uncertainty in radiative forcing calculations.

A global process-based study of marine CCN trends and variability

Low-level clouds have a strong climate-cooling effect in oceanic regions due to the much lower albedo of the underlying sea surface. Marine clouds typically have low droplet concentrations, making their radiative properties susceptible to changes in cloud condensation nucleus (CCN) concentrations. Here, we use the global aerosol model GLOMAP to investigate the processes that determine variations in marine CCN concentrations, and focus especially on the effects of previously identified wind speed trends in recent decades. Although earlier studies have found a link between linear wind speed trends and CCN concentration, we find that the effects of wind speed trends identified using a dynamic linear model in the Northern Equatorial Pacific (0.56 m s−1 per decade in the period 1990–2004) and the North Atlantic (−0.21 m s−1 per decade) are largely dampened by other processes controlling the CCN concentration, namely nucleation scavenging and transport of continental pollution. A CCN signal from wind speed change is seen only in the most pristine of the studied regions, i.e. over the Southern Ocean, where we simulate 3.4 cm−3 and 0.17 m s−1 increases over the 15-year period in the statistical mean levels of CCN and wind speed, respectively. Our results suggest that future changes in wind-speed-driven aerosol emissions from the oceans can probably have a climate feedback via clouds only in the most pristine regions. On the other hand, a feedback mechanism via changing precipitation patterns and intensities could take place over most oceanic regions, as we have shown that nucleation scavenging has by far the largest absolute effect on CCN concentrations.

Size-dependent wet removal of black carbon in Canadian biomass burning plumes

Wet deposition is the dominant mechanism for removing black carbon (BC) from the atmosphere, and is key in determining its atmospheric lifetime, vertical gradient and global transport. Despite the importance of BC in the climate system, especially in terms of its ability to modulate the radiative energy budget, there are few quantitative case studies of wet removal in ambient environments. We present a case study of BC wet removal by examining aerosol size distributions and BC coating properties sampled in three Canadian boreal biomass burning plumes, one of which passed through a precipitating cloud. In this plume, the largest and most coated BC particles were found to be preferentially removed, suggesting that nucleation scavenging was the likely dominant mechanism. Calculated mass absorption coefficient (MAC) in the plumes showed no significant variation, as the shifts to smaller BC cores and thinner coatings had opposing effects. Similarly, calculated single-scatter albedo (SSA) showed little variation, as a large number of non-BC particles were also present in the precipitation-affected plume. The remaining BC cores were smaller than those observed in previous studies of BC in post-precipitation outflow over Asia, possibly due to the thick coatings associated with the biomass burning particles. This study provides important constraints to model parameterisations of BC wet removal in biomass burning regions, which will help to reduce uncertainty in radiative forcing calculations.

A global process-based study of marine CCN trends and variability

Low-level clouds have a strong climate-cooling effect in oceanic regions due to the much lower albedo of the underlying sea surface. Marine clouds typically have low droplet concentrations, making their radiative properties susceptible to changes in cloud condensation nucleus (CCN) concentrations. Here, we use the global aerosol model GLOMAP to investigate the processes that determine variations in marine CCN concentrations, and focus especially on the effects of previously identified wind speed trends in recent decades. Although earlier studies have found a link between linear wind speed trends and CCN concentration, we find that the effects of wind speed trends identified using a dynamic linear model in the Northern Equatorial Pacific (0.56 m s−1 per decade in the period 1990–2004) and the North Atlantic (−0.21 m s−1 per decade) are largely dampened by other processes controlling the CCN concentration, namely nucleation scavenging and transport of continental pollution. A CCN signal from wind speed change is seen only in the most pristine of the studied regions, i.e. over the Southern Ocean, where we simulate 3.4 cm−3 and 0.17 m s−1 increases over the fifteen-year period in the statistical mean levels of CCN and wind speed, respectively. Our results suggest that future changes in wind-speed-driven aerosol emissions from the oceans can probably have a climate feedback via clouds only in the most pristine regions. On the other hand, a feedback mechanism via changing precipitation patterns and intensities could take place over most oceanic regions, as we have shown that nucleation scavenging has by far the largest absolute effect on CCN concentrations.

Estimating bacteria emissions from inversion of atmospheric transport: sensitivity to modelled particle characteristics

Model-simulated transport of atmospheric trace components can be combined with observed concentrations to obtain estimates of ground-based sources using various inversion techniques. These approaches have been applied in the past primarily to obtain source estimates for long-lived trace gases such as CO2. We consider the application of similar techniques to source estimation for atmospheric aerosols, using as a case study the estimation of bacteria emissions from different ecosystem regions in the global atmospheric chemistry and climate model ECHAM5/MESSy-Atmospheric Chemistry (EMAC). Source estimation via Markov Chain Monte Carlo is applied to a suite of sensitivity simulations, and the global mean emissions are estimated for the example problem of bacteria-containing aerosol particles. We present an analysis of the uncertainties in the global mean emissions, and a partitioning of the uncertainties that are attributable to particle size, activity as cloud condensation nuclei (CCN), the ice nucleation scavenging ratios for mixed-phase and cold clouds, and measurement error. For this example, uncertainty due to CCN activity or to a 1 μm error in particle size is typically between 10% and 40% of the uncertainty due to observation uncertainty, as measured by the 5–95th percentile range of the Monte Carlo ensemble. Uncertainty attributable to the ice nucleation scavenging ratio in mixed-phase clouds is as high as 10–20% of that attributable to observation uncertainty. Taken together, the four model parameters examined contribute about half as much to the uncertainty in the estimated emissions as do the observations. This was a surprisingly large contribution from model uncertainty in light of the substantial observation uncertainty, which ranges from 81–870% of the mean for each of ten ecosystems for this case study. The effects of these and other model parameters in contributing to the uncertainties in the transport of atmospheric aerosol particles should be treated explicitly and systematically in both forward and inverse modelling studies.

Impact of modelled particle characteristics on emissions inferred by inversion of tracer transport

Model-simulated transport of atmospheric trace components can be combined with observed concentrations to obtain estimates of ground-based sources using various inversion techniques. These approaches have been applied in the past primarily to obtain source estimates for long-lived trace gases such as CO2. We consider the application of similar techniques to source estimation for atmospheric aerosols, using as a case study the estimation of bacteria emissions from different ecosystem regions in the global atmospheric chemistry and climate model ECHAM5/MESSy-Atmospheric Chemistry (EMAC). Source estimation via Monte Carlo Markov Chain is applied to a suite of sensitivity simulations and the global mean emissions are estimated. We present an analysis of the uncertainties in the global mean emissions, and a partitioning of the uncertainties that are attributable to particle size, activity as cloud condensation nuclei (CCN), the ice nucleation scavenging ratios for mixed-phase and cold clouds, and measurement error. Uncertainty due to CCN activity or to a 1 μm error in particle size is typically between 10% and 40% of the uncertainty due to observation uncertainty, as measured by the 5%-ile to 95%-ile range of the Monte Carlo ensemble. Uncertainty attributable to the ice nucleation scavenging ratio in mixed-phase clouds is as high as 10% to 20% of that attributable to observation uncertainty. Taken together, the four model parameters examined contribute about half as much to the uncertainty in the estimated emissions as do the observations. This was a surprisingly large contribution from model uncertainty in light of the substantial observation uncertainty, which ranges from 81% to 870% of the mean for each of ten ecosystems for this case study. The effects of these and other model parameters in contributing to the uncertainties in the transport of atmospheric aerosol particles should be treated explicitly and systematically in both forward and inverse modelling studies.