Reduced effective radiative forcing from cloud–aerosol interactions (ERF_aci) with improved treatment of early aerosol growth in an Earth system model

Historically, aerosols of anthropogenic origin have offset some of the warming from increased atmospheric greenhouse gas concentrations. The strength of this negative aerosol forcing, however, is highly uncertain – especially the part originating from cloud–aerosol interactions. An important part of this uncertainty originates from our lack of knowledge about pre-industrial aerosols and how many of these would have acted as cloud condensation nuclei (CCN). In order to simulate CCN concentrations in models, we must adequately model secondary aerosols, including new particle formation (NPF) and early growth, which contributes a large part of atmospheric CCN. In this study, we investigate the effective radiative forcing (ERF) from cloud–aerosol interactions (ERFaci) with an improved treatment of early particle growth, as presented in Blichner et al. (2021). We compare the improved scheme to the default scheme, OsloAero, which are both embedded in the atmospheric component of the Norwegian Earth System Model v2 (NorESM2). The improved scheme, OsloAeroSec, includes a sectional scheme that treats the growth of particles from 5–39.6 nm in diameter, which thereafter inputs the particles to the smallest mode in the pre-existing modal aerosol scheme. The default scheme parameterizes the growth of particles from nucleation up to the smallest mode, a process that can take several hours. The explicit treatment of early growth in OsloAeroSec, on the other hand, captures the changes in atmospheric conditions during this growth time in terms of air mass mixing, transport, and condensation and coagulation. We find that the ERFaci with the sectional scheme is −1.16 W m−2, which is 0.13 W m−2 weaker compared to the default scheme. This reduction originates from OsloAeroSec producing more particles than the default scheme in pristine, low-aerosol-concentration areas and fewer NPF particles in high-aerosol areas. We find, perhaps surprisingly, that NPF inhibits cloud droplet activation in polluted and/or high-aerosol-concentration regions because the NPF particles increase the condensation sink and reduce the growth of the larger particles which may otherwise activate. This means that in these high-aerosol regions, the model with the lowest NPF – OsloAeroSec – will have the highest cloud droplet activation and thus more reflective clouds. In pristine and/or low-aerosol regions, however, NPF enhances cloud droplet activation because the NPF particles themselves tend to activate. Lastly, we find that sulfate emissions in the present-day simulations increase the hygroscopicity of secondary aerosols compared to pre-industrial simulations. This makes NPF particles more relevant for cloud droplet activation in the present day than the pre-industrial atmosphere because increased hygroscopicity means they can activate at smaller sizes.

Aerodynamic size-resolved composition and cloud condensation nuclei properties of aerosols in Beijing suburban region

The size-resolved physiochemical properties of aerosols determine their atmospheric lifetime, cloud interactions, and the deposition rate on human respiratory system, however most atmospheric composition studies tend to evaluate these properties in bulk. This study investigated size-resolved constituents of aerosols on mass and number basis, and their droplet activation properties, by coupling a suite of online measurements with an aerosol aerodynamic classifier (AAC) based on aerodynamic diameter (Da) in Pinggu, a suburb of Beijing. While organic matter accounted for a large fraction of mass, a higher contribution of particulate nitrate at larger sizes (Da > 300 nm) was found under polluted cases. By applying the mixing state of refractory black carbon containing particles (rBCc) and composition-dependent densities, aerosols including rBCc were confirmed nearly spherical at Da > 300 nm. Importantly, the number fraction of rBCc was found to increase with Da at all pollution levels. The number fraction of rBC is found to increase from ~3 % at ~90 nm to ~15 % at ~1000 nm, and this increasing rBC number fraction may be caused by the coagulation during atmospheric aging. The droplet activation diameter at a water supersaturation of 0.2 % was 112 ± 6 nm and 193 ± 41 nm for all particles with Da smaller than 1 μm (PM1) and rBCc respectively. As high as 52 ± 6 % of rBCc and 50 ± 4 % of all PM1 particles in number could be activated under heavy pollution due to enlarged particle size, which could be predicted by applying the volume-mixing of substance hygroscopicity within rBCc. As rBCc contributes to the quantity of aerosols at larger particle size, these thickly coated rBC may contribute to the radiation absorption significantly or act as an important source of cloud condensation nuclei (CCN). This size regime may also exert important health effects due to their higher deposition rate.

Droplet activation of moderately surface active organic aerosol predicted with six approaches to surface activity

Surface active compounds (surfactants) found in atmospheric aerosols can decrease droplet surface tension as they adsorb to the droplet surfaces simultaneously depleting the droplet bulk. These processes may influence the activation properties of aerosols into cloud droplets and investigation of their role in cloud microphysics has been ongoing for decades. In this study, we have used six different approaches documented in the literature to represent surface activity in Köhler calculations predicting cloud droplet activation properties for particles consisting of one of three different moderately surface active organics mixed with ammonium sulphate in different ratios. We find that the different models predict comparable activation properties at small organic mass fractions in the dry particles for all three moderately surface active organics tested, even with large differences in the predicted degree of bulk-to-surface partitioning of the surface active component. However, differences between the models regarding both the predicted critical diameter and supersaturation for the same dry particle size increase with the organic fraction in the particles. Comparison with available experimental data shows that assuming complete bulk-to-surface partitioning of the organic component (total depletion of the bulk) along the full droplet growth curve does not adequately represent the activation properties of particles with high moderate surfactant mass fractions. Accounting for the surface tension depression mitigates some of the effect. Models that include the possibility for partial bulk-to-surface partitioning yield comparable results to the experimental data, even at high organic mass fractions in the particles. The study highlights the need for using thermodynamically consistent model frameworks to treat surface activity of atmospheric aerosols and for firm experimental validation of model predictions across a wide range of states relevant to the atmosphere.

Impact of entrainment-mixing and turbulent fluctuations on droplet size distributions in a cumulus cloud: An investigation using Lagrangian microphysics with a sub-grid-scale model

Entrainment-mixing and turbulent fluctuations critically impact cloud droplet size distributions (DSDs) in cumulus clouds. This problem is investigated via a new sophisticated modeling framework using the CM1 LES model and a Lagrangian cloud microphysics scheme – the “super-droplet method” (SDM) – coupled with sub-grid-scale (SGS) schemes for particle transport and supersaturation fluctuations. This modeling framework is used to simulate a cumulus congestus cloud. Average DSDs in different cloud regions show broadening from entrainment and secondary cloud droplet activation (activation above the cloud base). DSD width increases with increasing entrainment-induced dilution as expected from past work, except in the most diluted cloud regions. The new modeling framework with SGS transport and supersaturation fluctuations allows a more sophisticated treatment of secondary activation compared to previous studies. In these simulations, it contributes about 25%of the cloud droplet population and impacts DSDs in two contrastingways: narrowing in extremely diluted regions and broadening in relatively less diluted. SGS supersaturation fluctuations contribute significantly to an increase in DSD width via condensation growth and evaporation. Mixing of super-droplets from SGS velocity fluctuations also broadens DSDs. The relative dispersion (ratio of DSD dispersion and mean radius) negatively correlates with grid-scale vertical velocity in updrafts, but is positively correlated in downdrafts. The latter is from droplet activation driven by positive SGS supersaturation fluctuations in grid-mean subsaturated conditions. Finally, the sensitivity to model grid length is evaluated. The SGS schemes have greater influence as the grid length is increased, and they partially compensate for the reduced model resolution.

Cloud droplet activation in a continental Central European urban environment

Collocated measurements by condensation particle counter, differential mobility particle sizer and cloud condensational nuclei counter instruments were realised in parallel in central Budapest from 15 April 2019 to 14 April 2020 to gain insight into the droplet activation behaviour of urban aerosol particles. The median total particle number concentration was 10.1 × 103 cm−3. The median concentrations of cloud condensation nuclei (CCN) at water vapour supersaturations (Ss) of 0.1, 0.2, 0.3, 0.5 and 1.0 % were 0.59, 1.09, 1.39, 1.80 and 2.5 × 103 cm−3, respectively. They represented from 7 to 27 % of the total particles. The effective critical dry particle diameters (dc,eff) were derived utilising the CCN concentrations and particle number size distributions. Their medians were 207, 149, 126, 105 and 80 nm, respectively. They were all positioned within the accumulation mode of the typical particle number size distribution. Their frequency distributions revealed a single peak, which geometric standard deviation increased monotonically with S. The broadening indicated larger time variability in the activation properties of smaller particles. The frequency distributions also showed a fine structure. Its several compositional elements seemed to change in a tendentious manner with S. They were related to the size-dependent chemical composition and external mixtures of particles. The relationships between the critical S and dc,eff suggested that the urban aerosol particles in Budapest with a diameter larger than approximately 130 nm showed similar hygroscopicity than the continental aerosol in general, while the smaller particles appeared to be less hygroscopic than that. Seasonal cycling of the CCN concentrations and activation fractions implied modest alterations and for the larger Ss only. They likely reflected the changes in particle number concentrations, chemical composition and mixing state of particles. The seasonal dependencies for dc,eff were featureless, which indicated that the urban particles exhibited more or less similar droplet activation properties over the measurement year. This is different from non-urban locations. The hygroscopicity parameters (κ values) were computed without determining time-dependent chemical composition of particles. Their medians were 0.16, 0.10, 0.07, 0.04 and 0.02, respectively. The averages suggested that the larger particles exhibited considerably higher hygroscopicity than the smaller particles. The urban aerosol was characterised by substantially smaller kappa values than for regional or remote locations. All these could be virtually linked to specific source composition in cities. The relatively large variability in the hygroscopicity parameter sets for a given S emphasized that their individual values represented the CCN population in the ambient air, while the averages stood mainly for the particles with a size close to the effective critical dry particle diameters.

Reduced effective radiative forcing from cloud-aerosol interactions (ERF_aci) with improved treatment of early aerosol growth in an Earth System Model

Historically, aerosols of anthropogenic origin have offset some of the warming from increased atmospheric green- house gas concentrations. The strength of this negative aerosol forcing is, however, highly uncertain – especially the part originating from cloud-aerosol interactions. An important part of this uncertainty originates from our lack of knowledge about the pre-industrial aerosols and how many of these would have acted as cloud condensation nuclei (CCN). In order to simulate CCN concentrations in models, we must adequately model secondary aerosols, including new particle formation (NPF) and early growth, which contributes with a large part of atmospheric CCN. In this study, we investigate the effective radiative forcing (ERF) from cloud–aerosol interactions (ERFaci ) with an improved treatment of early particle growth, presented in Blichner et al. (2020). We compare the improved scheme to the default scheme, OsloAero, both part of the atmospheric component of the Norwegian Earth System Model v2 (NorESM2). The improved scheme, OsloAeroSec, includes a sectional scheme that treats the growth of the particles from 5–39.6 nm which thereafter inputs the particles to the smallest mode in the pre-existing, modal aerosol scheme. The default scheme parameterizes the growth of particles from nucleation and up to the smallest mode, a process that can take several hours. The explicit treatment of the early growth in OsloAeroSec on the other hand, captures the changes in atmospheric condition during this growth time both in terms of air mass mixing, transport and condensation and coagulation.We find that the ERF aci with the sectional scheme is −1.16 Wm−2 , which is 0.13 Wm−2 weaker compared to the default scheme. This reduction originates from OsloAeroSec producing more particles than the default scheme in pristine, low-aerosol- concentration areas and less NPF particles in high-aerosol areas. We find, perhaps surprisingly, that NPF inhibits cloud droplet activation in polluted/high-aerosol-concentration regions because the NPF particles increase the condensation sink and reduces the growth of the larger particles which may otherwise activate. This means that in these high-aerosol regions, the model with lowest NPF – OsloAeroSec – will have highest cloud droplet activation and thus more reflective clouds. In pristine/low aerosol regions however, NPF enhances cloud droplet activation, because the NPF particles themselves tend to activate.Lastly, we find that sulphate emissions in the present day simulations increase the hygroscopicity of the secondary aerosols compared to the pre-industrial simulations. This makes NPF particles more relevant for cloud droplet activation in the present day than the pre-industrial atmosphere, because the increased hygroscopicity means they can activate at smaller sizes.