Mean Cloud Condensation Nuclei Research Articles

Developing a climatological simplification of aerosols to enter the cloud microphysics of a global climate model

Abstract. Aerosol particles influence cloud formation and properties. Hence climate models that aim for a physical representation of the climate system include aerosol modules. In order to represent more and more processes and aerosol species, their representation has grown increasingly detailed. However, depending on one's modelling purpose, the increased model complexity may not be beneficial, for example because it hinders understanding of model behaviour. Hence we develop a simplification in the form of a climatology of aerosol concentrations. In one approach, the climatology prescribes properties important for cloud droplet and ice crystal formation, the gateways for aerosols to enter the model cloud microphysics scheme. Another approach prescribes aerosol mass and number concentrations in general. Both climatologies are derived from full ECHAM-HAM simulations and can serve to replace the HAM aerosol module and thus drastically simplify the aerosol treatment. The first simplification reduces computational model time by roughly 65 %. However, the naive mean climatological treatment needs improvement to give results that are satisfyingly close to the full model. We find that mean cloud condensation nuclei (CCN) concentrations yield an underestimation of cloud droplet number concentration (CDNC) in the Southern Ocean, which we can reduce by allowing only CCN at cloud base (which have experienced hygroscopic growth in these conditions) to enter the climatology. This highlights the value of the simplification approach in pointing to unexpected model behaviour and providing a new perspective for its study and model development.

CCN activation in homogeneous isotropic turbulence: Response to particle characteristics and environmental conditions

Direct Numerical Simulation (DNS) of turbulent cloud parcels are presented where particles evolve in response to the local values in supersaturation (s) led by turbulent fluctuations. A pseudo-spectral DNS is modified to incorporate aerosol particles and Cloud Condensation Nuclei (CCN) activation applying a droplet growth equation based on κ-Köhler theory that works for the whole range of warm cloud particles, from un-activated deliquesced aerosol particles to activated cloud droplets, that grow by condensation. The Lagrangian microphysics applied ensures that each particle experiences a supersaturation (fluctuations added to the mean) corresponding to its near-particle gas phase surroundings, which differs from the uniform parcel view where an average value of supersaturation, s¯, is applied to every particle in the domain. A non-turbulent Lagrangian parcel model with similar mean thermodynamics and CCN properties is compared with turbulent DNS parcels of varying fluctuation intensities to distinguish the impact of turbulence on CCN activation. It is shown that, in a given distribution, a subset of aerosols respond to fluctuations rather than the mean thermodynamics allowing particles of similar dry size to co-exist as un-activated haze particles as well as cloud droplets. The cloud microphysical properties are analysed in a series of DNS experiments with contrasting thermodynamic and aerosol properties. DNS results agrees with the general understanding of aerosol activation and cloud droplets evolution in response to various background conditions such as pristine and polluted aerosol distributions, composition of CCN with respect to organic - inorganic components and magnitude of vertical velocity. DNS considers turbulence-microphysics interactions in such problems providing additional knowledge on the role of turbulence in clouds. It is argued that incorporating turbulent fluctuations in simulating the CCN activation and droplet growth is well reasoned and a constructive way forward.

Distribution Characteristics of Aerosol Size and CCN during the Summer on Mt. Tian and Their Influencing Factors

The aerosol size distribution and cloud condensation nuclei (CCN) number concentration were measured using a wide-range particle spectrometer (WPS) and a cloud condensation nuclei counter (CCNC) on Mt. Tian from 31 July to 9 September, 2019. Combined with meteorological data, distribution characteristics of aerosol size and CCN and their influencing factors were analyzed. The results indicated that the mean aerosol number concentration was 5475.6 ± 5636.5 cm−3. The mean CCN concentrations were 183.7 ± 114.5 cm−3, 729.8 ± 376.1 cm−3, 1630.5 ± 980.5 cm−3, 2162.5 ± 1345.3 cm−3, and 2575.7 ± 1632.9 cm−3 at supersaturation levels of 0.1%, 0.2%, 0.4%, 0.6%, and 0.8%, respectively. The aerosol number size distribution is unimodal, and the dominant particle size is 30–60 nm. Affected by the height of the boundary layer and the valley wind, the diurnal variation in aerosol number concentration shows a unimodal distribution with a peak at 17:00, and the CCN number concentration showed a bimodal distribution with peaks at 18:00 and 21:00. The particle size distribution and supersaturation have a major impact on the activation of the aerosol into CCN. At 0.1% supersaturation (S), the 300–500 nm particles are most likely to activate to CCN. Particles of 100–300 nm are most easily activated at 0.2% (S), while particles of 60–80 nm are most likely activated at high supersaturation (≥0.4%). The concentrations of aerosol and CCN are higher in the northerly wind. Ambient relative humidity (RH) has little relationship with the aerosol activation under high supersaturation. According to N = CSk fitting the CCN spectrum, C = 3297 and k = 0.90 on Mt. Tian, characteristic of the clean continental type.

Broadening of Cloud Droplet Size Spectra by Stochastic Condensation: Effects of Mean Updraft Velocity and CCN Activation

Abstract The authors study the condensational growth of cloud droplets in homogeneous isotropic turbulence by means of a large-eddy simulation (LES) approach. The authors investigate the role of a mean updraft velocity and of the chemical composition of the cloud condensation nuclei (CCN) on droplet growth. The results show that a mean constant updraft velocity superimposed onto a turbulent field reduces the broadening of the droplet size spectra induced by the turbulent fluctuations alone. Extending the authors’ previous results regarding stochastic condensation, the authors introduce a new theoretical estimation of the droplet size spectrum broadening that accounts for this updraft velocity effect. A similar reduction of the spectra broadening is observed when the droplets reach their critical size, which depends on the chemical composition of CCN. The analysis of the square of the droplet radius distribution, proportional to the droplet surface, shows that for large particles the distribution is purely Gaussian, while it becomes strongly non-Gaussian for smaller particles, with the left tail characterized by a peak around the haze activation radius. This kind of distribution can significantly affect the later stages of the droplet growth involving turbulent collisions, since the collision probability kernel depends on the droplet size, implying the need for new specific closure models to capture this effect.

Impacts of organic aerosols and its oxidation level on CCN activity from measurement at a suburban site in China

Abstract. This study is concerned with the impacts of organic aerosols on cloud condensation nuclei (CCN) activity based on field measurements made at a suburban site in Northern China. The sensitivity of the estimated CCN number concentration (NCCN) to both volume fraction of organic material (xorg) and aerosol oxidation level (using f44, the fraction of m∕z 44 in aerosol organic material) are examined. A strong dependence of CCN number concentration (NCCN) on the xorg and f44 was noted. The sensitivity of NCCN to volume fraction of organics increased with increasing xorg. The impacts of the aerosol particles oxidization or aging level on estimating NCCN were also very significant. When the particles were mostly composed of organics (xorg > 60 %), the NCCN at the supersaturation of 0.075 and 0.13 % was underestimated by 46 and 44 %, respectively, if aerosol particles were freshly emitted with primary organics (f44 < 11 %); the underestimation decreased to 32 and 23 % at the corresponding supersaturations, however, if the particles were with more hygroscopic secondary organics (f44 > 15 %). The NCCN at the supersaturation of 0.76 % was underestimated by 11 and 4 %, respectively, at f44 < 11 and f44 > 15 %. However, for the particles composed of low organics (e.g., xorg < 40 %), the effect caused by the f44 was quite insignificant both at high and low supersaturations. This is because the overall hygroscopicity of the particles is dominated by inorganics such as sulfate and nitrate, which are more hygroscopic than organic compounds. Our results indicated that it would decrease the uncertainties in estimating NCCN and lead to a more accurate estimation of NCCN to increase the proportion of secondary organics, especially when the composition of the aerosols is dominated by organics. The applicability of the CCN activation spectrum obtained at Xinzhou to the Xianghe site, about 400 km to the northeast of Xinzhou, was investigated, with the aim of further examining the sensitivity of NCCN to aerosol type. Overall, the mean CCN efficiency spectrum derived from Xinzhou performs well at Xianghe when the supersaturation levels are > 0.2 % (overestimation of 2–4 %). However, NCCN was overestimated by ∼ 20 % at supersaturation levels of < 0.1 %. This suggests that the overestimation is mainly due to the smaller proportion of aged and oxidized organic aerosols present at Xianghe compared to Xinzhou.

Optical properties and CCN activity of aerosols in a high‐altitude Himalayan environment: Results from RAWEX‐GVAX

AbstractThe seasonality and mutual dependence of aerosol optical properties and cloud condensation nuclei (CCN) activity under varying meteorological conditions at the high‐altitude Nainital site (~2 km) in the Indo‐Gangetic Plains were examined using nearly year‐round measurements (June 2011 to March 2012) at the Atmospheric Radiation Measurement mobile facility as part of the Regional Aerosol Warming Experiment–Ganges Valley Aerosol Experiment of the Indian Space Research Organization and the U.S. Department of Energy. The results from collocated measurements provided enhanced aerosol scattering and absorption coefficients, CCN concentrations, and total condensation nuclei concentrations during the dry autumn and winter months. The CCN concentration (at a supersaturation of 0.46) was higher during the periods of high aerosol absorption (single scattering albedo (SSA) < 0.80) than during the periods of high aerosol scattering (SSA > 0.85), indicating that the aerosol composition seasonally changes and influences the CCN activity. The monthly mean CCN activation ratio (at a supersaturation of 0.46) was highest (>0.7) in late autumn (November); this finding is attributed to the contribution of biomass‐burning aerosols to CCN formation at high supersaturation conditions.

The magnitude and causes of uncertainty in global model simulations of cloud condensation nuclei

Abstract. Aerosol–cloud interaction effects are a major source of uncertainty in climate models so it is important to quantify the sources of uncertainty and thereby direct research efforts. However, the computational expense of global aerosol models has prevented a full statistical analysis of their outputs. Here we perform a variance-based analysis of a global 3-D aerosol microphysics model to quantify the magnitude and leading causes of parametric uncertainty in model-estimated present-day concentrations of cloud condensation nuclei (CCN). Twenty-eight model parameters covering essentially all important aerosol processes, emissions and representation of aerosol size distributions were defined based on expert elicitation. An uncertainty analysis was then performed based on a Monte Carlo-type sampling of an emulator built for each model grid cell. The standard deviation around the mean CCN varies globally between about ±30% over some marine regions to ±40–100% over most land areas and high latitudes, implying that aerosol processes and emissions are likely to be a significant source of uncertainty in model simulations of aerosol–cloud effects on climate. Among the most important contributors to CCN uncertainty are the sizes of emitted primary particles, including carbonaceous combustion particles from wildfires, biomass burning and fossil fuel use, as well as sulfate particles formed on sub-grid scales. Emissions of carbonaceous combustion particles affect CCN uncertainty more than sulfur emissions. Aerosol emission-related parameters dominate the uncertainty close to sources, while uncertainty in aerosol microphysical processes becomes increasingly important in remote regions, being dominated by deposition and aerosol sulfate formation during cloud-processing. The results lead to several recommendations for research that would result in improved modelling of cloud–active aerosol on a global scale.

Anthropogenic contribution to cloud condensation nuclei and the first aerosol indirect climate effect

Atmospheric particles influence the climate indirectly by acting as cloud condensation nuclei (CCN). The first aerosol indirect radiative forcing (FAIRF) constitutes the largest uncertainty among the radiative forcings quantified by the latest IPCC report (IPCC2007) and is a major source of uncertainty in predicting climate change. Here, we investigate the anthropogenic contribution to CCN and associated FAIRF using a state-of-the-art global chemical transport and aerosol model (GEOS-Chem/APM) that contains a number of advanced features (including sectional particle microphysics, online comprehensive chemistry, consideration of all major aerosol species, online aerosol–cloud–radiation calculation, and usage of more accurate assimilated meteorology). The model captures the absolute values and spatial distributions of CCN concentrations measured in situ around the globe. We show that anthropogenic emissions increase the global mean CCN in the lower troposphere by ∼60–80% and cloud droplet number concentration by ∼40%. The global mean FAIRF based on GEOS-Chem/APM is −0.75 W m−2, close to the median values of both IPCC2007 and post-IPCC2007 studies. To the best of our knowledge, this is the first time that a global sectional aerosol model with full online chemistry and considering all major aerosol species (including nitrate, ammonium, and second organic aerosols) has been used used to calculate FAIRF.

Low sensitivity of cloud condensation nuclei to changes in the sea-air flux of dimethyl-sulphide

Abstract. The emission of dimethyl-sulphide (DMS) gas by phytoplankton and the subsequent formation of aerosol has long been suggested as an important climate regulation mechanism. The key aerosol quantity is the number concentration of cloud condensation nuclei (CCN), but until recently global models did not include the necessary aerosol physics to quantify CCN. Here we use a global aerosol microphysics model to calculate the sensitivity of CCN to changes in DMS emission using multiple present-day and future sea-surface DMS climatologies. Calculated annual fluxes of DMS to the atmosphere for the five model-derived and one observations based present day climatologies are in the range 15.1 to 32.3 Tg a−1 sulphur. The impact of DMS climatology on surface level CCN concentrations was calculated in terms of summer and winter hemispheric mean values of ΔCCN/ΔFluxDMS, which varied between −43 and +166 cm−3/(mg m−2 day−1 sulphur), with a mean of 63 cm−3/(mg m−2 day−1 sulphur). The range is due to CCN production in the atmosphere being strongly dependent on the spatial distribution of the emitted DMS. The relative sensitivity of CCN to DMS (i.e. fractional change in CCN divided by fractional change in DMS flux) depends on the abundance of non-DMS derived aerosol in each hemisphere. The relative sensitivity averaged over the five present day DMS climatologies is estimated to be 0.02 in the northern hemisphere (i.e. a 0.02% change in CCN for a 1% change in DMS) and 0.07 in the southern hemisphere where aerosol abundance is lower. In a globally warmed scenario in which the DMS flux increases by ~1% relative to present day we estimate a ~0.1% increase in global mean CCN at the surface. The largest CCN response occurs in the Southern Ocean, contributing to a Southern Hemisphere mean annual increase of less than 0.2%. We show that the changes in DMS flux and CCN concentration between the present day and global warming scenario are similar to interannual differences due to variability in windspeed. In summary, although DMS makes a significant contribution to global marine CCN concentrations, the sensitivity of CCN to potential future changes in DMS flux is very low. This finding, together with the predicted small changes in future seawater DMS concentrations, suggests that the role of DMS in climate regulation is very weak.

The impact of the 1783–1784 AD Laki eruption on global aerosol formation processes and cloud condensation nuclei

Abstract. The 1783–1784 AD Laki flood lava eruption commenced on 8 June 1783 and released 122 Tg of sulphur dioxide gas over the course of 8 months into the upper troposphere and lower stratosphere above Iceland. Previous studies have examined the impact of the Laki eruption on sulphate aerosol and climate using general circulation models. Here, we study the impact on aerosol microphysical processes, including the nucleation of new particles and their growth to cloud condensation nuclei (CCN) using a comprehensive Global Model of Aerosol Processes (GLOMAP). Total particle concentrations in the free troposphere increase by a factor ~16 over large parts of the Northern Hemisphere in the 3 months following the onset of the eruption. Particle concentrations in the boundary layer increase by a factor 2 to 5 in regions as far away as North America, the Middle East and Asia due to long-range transport of nucleated particles. CCN concentrations (at 0.22% supersaturation) increase by a factor 65 in the upper troposphere with maximum changes in 3-month zonal mean concentrations of ~1400 cm−3 at high northern latitudes. 3-month zonal mean CCN concentrations in the boundary layer at the latitude of the eruption increase by up to a factor 26, and averaged over the Northern Hemisphere, the eruption caused a factor 4 increase in CCN concentrations at low-level cloud altitude. The simulations show that the Laki eruption would have completely dominated as a source of CCN in the pre-industrial atmosphere. The model also suggests an impact of the eruption in the Southern Hemisphere, where CCN concentrations are increased by up to a factor 1.4 at 20° S. Our model simulations suggest that the impact of an equivalent wintertime eruption on upper tropospheric CCN concentrations is only about one-third of that of a summertime eruption. The simulations show that the microphysical processes leading to the growth of particles to CCN sizes are fundamentally different after an eruption when compared to the unperturbed atmosphere, underlining the importance of using a fully coupled microphysics model when studying long-lasting, high-latitude eruptions.

Cloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China – Part 1: Size-resolved measurements and implications for the modeling of aerosol particle hygroscopicity and CCN activity

Abstract. Atmospheric aerosol particles serving as Cloud Condensation Nuclei (CCN) are key elements of the hydrological cycle and climate. We measured and characterized CCN in polluted air and biomass burning smoke during the PRIDE-PRD2006 campaign from 1–30 July 2006 at a rural site ~60 km northwest of the mega-city Guangzhou in southeastern China. CCN efficiency spectra (activated fraction vs. dry particle diameter; 20–290 nm) were recorded at water vapor supersaturations (S) in the range of 0.068% to 1.27%. The corresponding effective hygroscopicity parameters describing the influence of particle composition on CCN activity were in the range of κ≈0.1–0.5. The campaign average value of κ=0.3 equals the average value of κ for other continental locations. During a strong local biomass burning event, the average value of κ dropped to 0.2, which can be considered as characteristic for freshly emitted smoke from the burning of agricultural waste. At low S (≤0.27%), the maximum activated fraction remained generally well below one, indicating substantial portions of externally mixed CCN-inactive particles with much lower hygroscopicity – most likely soot particles (up to ~60% at ~250 nm). The mean CCN number concentrations (NCCN,S) ranged from 1000 cm−3 at S=0.068% to 16 000 cm−3 at S=1.27%, which is about two orders of magnitude higher than in pristine air. Nevertheless, the ratios between CCN concentration and total aerosol particle concentration (integral CCN efficiencies) were similar to the ratios observed in pristine continental air (~6% to ~85% at S=0.068% to 1.27%). Based on the measurement data, we have tested different model approaches for the approximation/prediction of NCCN,S. Depending on S and on the model approach, the relative deviations between observed and predicted NCCN,S ranged from a few percent to several hundred percent. The largest deviations occurred at low S with a simple power law. With a Köhler model using variable κ values obtained from individual CCN efficiency spectra, the relative deviations were on average less than ~10% and hardly exceeded 20%, confirming the applicability of the κ-Köhler model approach for efficient description of the CCN activity of atmospheric aerosols. Note, however, that different types of κ-parameters must be distinguished for external mixtures of CCN-active and -inactive aerosol particles (κa, κt, κcut). Using a constant average hygroscopicity parameter (κ=0.3) and variable size distributions as measured, the deviations between observed and predicted CCN concentrations were on average less than 20%. In contrast, model calculations using variable hygroscopicity parameters as measured and constant size distributions led to much higher deviations: ~70% for the campaign average size distribution, ~80% for a generic rural size distribution, and ~140% for a generic urban size distribution. These findings confirm earlier studies suggesting that aerosol particle number and size are the major predictors for the variability of the CCN concentration in continental boundary layer air, followed by particle composition and hygroscopicity as relatively minor modulators. Depending on the required and applicable level of detail, the information and parameterizations presented in this study should enable efficient description of the CCN activity of atmospheric aerosols in detailed process models as well as in large-scale atmospheric and climate models.

Influence of oceanic dimethyl sulfide emissions on cloud condensation nuclei concentrations and seasonality over the remote Southern Hemisphere oceans: A global model study

We use a global chemical transport model with size‐resolved aerosol microphysics to investigate the sources of cloud condensation nuclei (CCN) in the Southern Hemisphere remote marine boundary layer (MBL). Long‐term observations of CCN number at Cape Grim (40°41′S, 144°41′E) show a clear seasonal cycle with a 2–3 times higher concentration in summer than in winter, which has been attributed to seasonal changes in the dimethyl sulfide (DMS) ocean‐to‐atmosphere flux. We find that this cycle at Cape Grim and also throughout the 30°–45°S latitude band is caused mostly by changes in the regional‐scale DMS ocean water concentration. In this latitude band, DMS emissions increase the simulated CCN concentrations from November to April, with a maximum effect of 46% in January (calculated at 0.23% supersaturation). Farther south, the impact of DMS on CCN is apparent only from December to February and increases the CCN concentration at most by 18% at 45°–60°S and by 40% at 60°–75°S. These model‐derived contributions of DMS to Southern Ocean summertime CCN are smaller than the 80% derived from correlations between satellite‐observed chlorophyll and column CCN, which we explain in terms of nonlinear behavior of CCN from the free troposphere (FT). We show that the main microphysical pathway of DMS influence on CCN number is nucleation of DMS‐derived H2SO4 in the FT and subsequent growth of formed particles by condensation and coagulation during entrainment into the MBL. Our simulations suggest that >90% of the increase in MBL CCN when DMS is added to the model is formed in this way. The growth of ultrafine sea spray particles to CCN sizes due to condensation of DMS‐derived H2SO4 in the MBL affects the simulated CCN concentrations by less than 6%. Overall, entrainment of nucleated sulfate aerosol into the MBL from the FT accounts for 43–65% of the summer zonal mean CCN concentrations but only 7–20% of the winter CCN over the Southern Hemisphere oceans.

Contribution of particle formation to global cloud condensation nuclei concentrations

We use a global aerosol microphysics model to predict the contribution of boundary layer (BL) particle formation to regional and global distributions of cloud condensation nuclei (CCN). Including an observationally derived particle formation scheme, where the formation rate of molecular clusters is proportional to gas‐phase sulfuric acid to the power one, improves modeled particle size distribution and total particle number concentration at three continental sites in Europe. Particle formation increases springtime BL global mean CCN (0.2% supersaturation) concentrations by 3–20% and CCN (1%) by 5–50%. Uncertainties in particle formation and growth rates must be reduced before the accuracy of these predictions can be improved. These results demonstrate the potential importance of BL particle formation as a global source of CCN.

Atmospheric aerosol major ion composition and cloud condensation nuclei over the northeast Atlantic

Concentrations of the major soluble ions, non‐sea‐salt (nss) sulfate, nitrate, chloride, and ammonium have been measured in aerosol samples collected at various locations and altitudes over the North Atlantic Ocean. Concentrations of nss sulfate, nitrate, and ammonium were found to be fairly uniform within the maritime boundary layer in an air mass aged in the Azores anticyclone; average values obtained were 0.36 ± 0.11, 0.18 ± 0.03, and 0.16 ± 0.06 μg m−3, respectively. The mean cloud condensation nuclei (CCN) concentration at 1% supersaturation was 368 cm−3, corresponding to air containing the major ion concentrations above. Incursion of continental air with a travel time of about 3 days over the sea led to an increase of around fivefold in nss sulfate, nitrate, and ammonium concentrations, while CCN concentrations increased less than threefold to 1076 cm−3. Two air samples collected during the clean air period above the marine boundary layer showed much reduced concentrations of soluble ions, but a mean CCN concentration of 358 cm−3. Regression analysis of all air sample data indicates that the nss sulfate and nitrate data are correlated to the observed CCN number density. While these ions are clearly making a significant contribution to CCN activity, the degree of correlation indicates that other chemical species also play a role as CCN.