scholarly journals Simulation of particle size distribution with a global aerosol model: contribution of nucleation to aerosol and CCN number concentrations

2009 ◽  
Vol 9 (2) ◽  
pp. 10597-10645 ◽  
Author(s):  
F. Yu ◽  
G. Luo
Keyword(s):  
Particle Number ◽  
Transport Model ◽  
Cloud Condensation Nuclei ◽  
Formation Rate ◽  
Sea Salt ◽  
Condensation Nuclei ◽  
Gaseous Species ◽  
Acid Vapor ◽  
Aerosol Model ◽  
Secondary Particles

Abstract. An advanced particle microphysics model with a number of computationally efficient schemes has been incorporated into a global chemistry transport model (GEOS-Chem) to simulate particle number size distributions and cloud condensation nuclei (CCN) concentrations in the atmosphere. Size-resolved microphysics for secondary particles (i.e., those formed from gaseous species) and sea salt has been treated in the present study. The growth of nucleated particles through the condensation of sulfuric acid vapor and equilibrium uptake of nitrate, ammonium, and secondary organic aerosol is explicitly simulated, along with the scavenging of secondary particles by primary particles (dust, black carbon, organic carbon, and sea salt). We calculate secondary particle formation rate based on ion-mediated nucleation (IMN) mechanism and constrain the parameterizations of primary particle emissions with various observations. Our simulations indicate that secondary particles formed via IMN appear to be able to account for the particle number concentrations observed in many parts of troposphere. A comparison of the simulated annual mean concentrations of condensation nuclei larger than 10 nm (CN10) with those measured values show very good agreement (within a factor of two) in near all 22 sites around the globe that have at least one full year of CN10 measurements. Secondary particles appear to dominate the number abundance in most parts of the troposphere. Calculated CCN concentration at supersaturation of 0.4% (CCN0.4) and the fraction of CCN0.4 that is secondary (fCCNsec) have large spatial variations. Over the middle latitude in the Northern Hemisphere, zonally averaged CCN0.4 decreases from ~400–700 cm−3 in the boundary layer (BL) to below 100 cm−3 above altitude of ~4 km, the corresponding fCCNsec values change from 50–60% to above ~70%. In the Southern Hemisphere, the zonally averaged CCN0.4 is below 200 cm−3 and fCCNsec is generally above 60% except in the BL over the Southern Ocean.

scholarly journals Simulation of particle size distribution with a global aerosol model: contribution of nucleation to aerosol and CCN number concentrations

2009 ◽  
Vol 9 (20) ◽  
pp. 7691-7710 ◽  
Author(s):  
F. Yu ◽  
G. Luo
Keyword(s):  
Particle Number ◽  
Transport Model ◽  
Cloud Condensation Nuclei ◽  
Formation Rate ◽  
Sea Salt ◽  
Condensation Nuclei ◽  
Gaseous Species ◽  
Acid Vapor ◽  
Aerosol Model ◽  
Secondary Particles

Abstract. An advanced particle microphysics model with a number of computationally efficient schemes has been incorporated into a global chemistry transport model (GEOS-Chem) to simulate particle number size distributions and cloud condensation nuclei (CCN) concentrations in the atmosphere. Size-resolved microphysics for secondary particles (i.e., those formed from gaseous species) and sea salt has been treated in the present study. The growth of nucleated particles through the condensation of sulfuric acid vapor and equilibrium uptake of nitrate, ammonium, and secondary organic aerosol is explicitly simulated, along with the scavenging of secondary particles by primary particles (dust, black carbon, organic carbon, and sea salt). We calculate secondary particle formation rate based on ion-mediated nucleation (IMN) mechanism and constrain the parameterizations of primary particle emissions with various observations. Our simulations indicate that secondary particles formed via IMN appear to be able to account for the particle number concentrations observed in many parts of the troposphere. A comparison of the simulated annual mean concentrations of condensation nuclei larger than 10 nm (CN10) with those measured values show very good agreement (within a factor of two) in near all 22 sites around the globe that have at least one full year of CN10 measurements. Secondary particles appear to dominate the number abundance in most parts of the troposphere. Calculated CCN concentration at supersaturation of 0.4% (CCN0.4) and the fraction of CCN0.4 that is secondary (fsecCCN) have large spatial variations. Over the middle latitude in the Northern Hemisphere, zonally averaged CCN0.4 decreases from ~400–700 cm−3 in the boundary layer (BL) to below 100 cm−3 above altitude of ~4 km, the corresponding fsecCCN values change from 50–60% to above ~70%. In the Southern Hemisphere, the zonally averaged CCN0.4 is below 200 cm−3 and fsecCCN is generally above 60% except in the BL over the Southern Ocean.

scholarly journals Effect of aerosol sub-grid variability on aerosol optical depth and cloud condensation nuclei: Implications for global aerosol modelling

2016 ◽  
Author(s):  
N. Weigum ◽  
N. Schutgens ◽  
P. Stier
Keyword(s):  
Aerosol Optical Depth ◽  
Optical Depth ◽  
Spatial Scales ◽  
Cloud Condensation Nuclei ◽  
Convective Transport ◽  
Condensation Nuclei ◽  
Gaseous Species ◽  
Climate Effects ◽  
Aerosol Model ◽  
The Impact

Abstract. A fundamental limitation of grid-based models is their inability to resolve variability on scales smaller than a grid box. Past research has shown that significant aerosol variability exists on scales smaller than these grid-boxes, which can lead to discrepancies in simulated aerosol climate effects between high and low resolution models. This study investigates the impact of neglecting sub-grid variability in present-day global microphysical aerosol models on aerosol optical depth (AOD) and cloud condensation nuclei (CCN). We introduce a novel technique to isolate the effect of aerosol variability from other sources of model variability by varying the resolution of aerosol and trace gas fields while maintaining a constant resolution in the rest of the model. We compare WRF-Chem runs in which aerosol and gases are simulated at 80 km and again at 10 km resolutions; in both simulations the other model components, such as meteorology and dynamics, are kept at the 10 km baseline resolution. We find that AOD is underestimated by 13 % and CCN is overestimated by 27 % when aerosol and gases are simulated at 80 km resolution compared to 10 km. Processes most affected by neglecting aerosol sub-grid variability are gas-phase chemistry and aerosol uptake of water through aerosol/gas equilibrium reactions. The inherent non-linearities in these processes result in large changes in aerosol parameters when aerosol and gaseous species are artificially mixed over large spatial scales. These changes in aerosol and gas concentrations are exaggerated by convective transport, which transports these altered concentrations to altitudes where their effect is more pronounced. These results demonstrate that aerosol variability can have a large impact on simulating aerosol climate effects, even when meteorology and dynamics are held constant. Future aerosol model development should focus on accounting for the effect of sub-grid variability on these processes at global scales in order to improve model predictions of the aerosol effect on climate.

scholarly journals Effect of vehicular traffic, remote sources and new particle formation on the activation properties of cloud condensation nuclei in the megacity of São Paulo, Brazil

2016 ◽  
Vol 16 (22) ◽  
pp. 14635-14656 ◽  
Author(s):  
Carlos Eduardo Souto-Oliveira ◽  
Maria de Fátima Andrade ◽  
Prashant Kumar ◽  
Fábio Juliano da Silva Lopes ◽  
Marly Babinski ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Particle Number ◽  
Cloud Condensation Nuclei ◽  
Activation Parameters ◽  
Particle Formation ◽  
Sea Salt ◽  
Vehicular Emissions ◽  
Vehicular Traffic ◽  
Condensation Nuclei ◽  
The Impact

Abstract. Atmospheric aerosol is the primary source of cloud condensation nuclei (CCN). The microphysics and chemical composition of aerosols can affect cloud development and the precipitation process. Among studies conducted in Latin America, only a handful have reported the impact of urban aerosol on CCN activation parameters such as activation ratio (AR) and activation diameter (Dact). With over 20 million inhabitants, the Metropolitan Area of São Paulo (MASP) is the largest megacity in South America. To our knowledge, this is the first study to assess the impact that remote sources and new particle formation (NPF) events have on CCN activation properties in a South American megacity. The measurements were conducted in the MASP between August and September 2014. We measured the CCN within the 0.2–1.0 % range of supersaturation, together with particle number concentration (PNC) and particle number distribution (PND), as well as trace-element concentrations and black carbon (BC). NPF events were identified on 35 % of the sampling days. Combining multivariate analysis in the form of positive matrix factorization (PMF) with an aerosol profile from lidar and HYSPLIT model analyses allowed us to identify the main contribution of vehicular traffic on all days and sea salt and biomass burning from remote regions on 28 and 21 % of the sampling days, respectively. The AR and Dact parameters showed distinct patterns for daytime with intense vehicular traffic and nighttime periods. For example, CCN activation was lower during the daytime than during the nighttime periods, a pattern that was found to be associated mainly with local road-traffic emissions. A decrease in CCN activation was observed on the NPF event days, mainly due to high concentrations of particles with smaller diameters. We also found that aerosols from sea salt, industrial emissions, and biomass burning had minor effects on Dact. For example, nights with biomass burning and vehicular emissions showed slightly lower CCN activation properties than sea-salt, industrial and non-event nights. Our results show that particulate matter from local vehicular emissions during the daytime has a greater effect on CCN activation parameters than that from remote sources.

scholarly journals Properties of cloud condensation nuclei (CCN) in the trade wind marine boundary layer of the western North Atlantic

2016 ◽  
Vol 16 (4) ◽  
pp. 2675-2688 ◽  
Author(s):  
Thomas B. Kristensen ◽  
Thomas Müller ◽  
Konrad Kandler ◽  
Nathalie Benker ◽  
Markus Hartmann ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Long Range ◽  
North Atlantic ◽  
Particle Number ◽  
Marine Boundary Layer ◽  
Mineral Dust ◽  
Cloud Condensation Nuclei ◽  
Sea Salt ◽  
Condensation Nuclei ◽  
Accumulation Mode

Abstract. Cloud optical properties in the trade winds over the eastern Caribbean Sea have been shown to be sensitive to cloud condensation nuclei (CCN) concentrations. The objective of the current study was to investigate the CCN properties in the marine boundary layer (MBL) in the tropical western North Atlantic, in order to assess the respective roles of inorganic sulfate, organic species, long-range transported mineral dust and sea-salt particles. Measurements were carried out in June–July 2013, on the east coast of Barbados, and included CCN number concentrations, particle number size distributions and offline analysis of sampled particulate matter (PM) and sampled accumulation mode particles for an investigation of composition and mixing state with transmission electron microscopy (TEM) in combination with energy-dispersive X-ray spectroscopy (EDX). During most of the campaign, significant mass concentrations of long-range transported mineral dust was present in the PM, and influence from local island sources can be ruled out. The CCN and particle number concentrations were similar to what can be expected in pristine marine environments. The hygroscopicity parameter κ was inferred, and values in the range 0.2–0.5 were found during most of the campaign, with similar values for the Aitken and the accumulation mode. The accumulation mode particles studied with TEM were dominated by non-refractory material, and concentrations of mineral dust, sea salt and soot were too small to influence the CCN properties. It is highly likely that the CCN were dominated by a mixture of sulfate species and organic compounds.

scholarly journals Effect of aerosol subgrid variability on aerosol optical depth and cloud condensation nuclei: implications for global aerosol modelling

2016 ◽  
Vol 16 (21) ◽  
pp. 13619-13639 ◽  
Author(s):  
Natalie Weigum ◽  
Nick Schutgens ◽  
Philip Stier
Keyword(s):  
Aerosol Optical Depth ◽  
Optical Depth ◽  
Spatial Scales ◽  
Cloud Condensation Nuclei ◽  
Convective Transport ◽  
Condensation Nuclei ◽  
Gaseous Species ◽  
Climate Effects ◽  
Aerosol Model ◽  
The Impact

Abstract. A fundamental limitation of grid-based models is their inability to resolve variability on scales smaller than a grid box. Past research has shown that significant aerosol variability exists on scales smaller than these grid boxes, which can lead to discrepancies in simulated aerosol climate effects between high- and low-resolution models. This study investigates the impact of neglecting subgrid variability in present-day global microphysical aerosol models on aerosol optical depth (AOD) and cloud condensation nuclei (CCN). We introduce a novel technique to isolate the effect of aerosol variability from other sources of model variability by varying the resolution of aerosol and trace gas fields while maintaining a constant resolution in the rest of the model. We compare WRF-Chem (Weather and Research Forecast model) runs in which aerosol and gases are simulated at 80 km and again at 10 km resolutions; in both simulations the other model components, such as meteorology and dynamics, are kept at the 10 km baseline resolution. We find that AOD is underestimated by 13 % and CCN is overestimated by 27 % when aerosol and gases are simulated at 80 km resolution compared to 10 km. The processes most affected by neglecting aerosol subgrid variability are gas-phase chemistry and aerosol uptake of water through aerosol–gas equilibrium reactions. The inherent non-linearities in these processes result in large changes in aerosol properties when aerosol and gaseous species are artificially mixed over large spatial scales. These changes in aerosol and gas concentrations are exaggerated by convective transport, which transports these altered concentrations to altitudes where their effect is more pronounced. These results demonstrate that aerosol variability can have a large impact on simulating aerosol climate effects, even when meteorology and dynamics are held constant. Future aerosol model development should focus on accounting for the effect of subgrid variability on these processes at global scales in order to improve model predictions of the aerosol effect on climate.

scholarly journals Implementation of aerosol–cloud interactions in the regional atmosphere–aerosol model COSMO-MUSCAT(5.0) and evaluation using satellite data

2017 ◽  
Vol 10 (6) ◽  
pp. 2231-2246 ◽  
Author(s):  
Sudhakar Dipu ◽  
Johannes Quaas ◽  
Ralf Wolke ◽  
Jens Stoll ◽  
Andreas Mühlbauer ◽  
...  
Keyword(s):  
Satellite Data ◽  
Transport Model ◽  
Cloud Condensation Nuclei ◽  
Cloud Droplet ◽  
Atmospheric Model ◽  
Horizontal Resolution ◽  
Small Scale ◽  
Aerosol Model ◽  
Aerosol Cloud ◽  
Aerosol Cloud Interactions

Abstract. The regional atmospheric model Consortium for Small-scale Modeling (COSMO) coupled to the Multi-Scale Chemistry Aerosol Transport model (MUSCAT) is extended in this work to represent aerosol–cloud interactions. Previously, only one-way interactions (scavenging of aerosol and in-cloud chemistry) and aerosol–radiation interactions were included in this model. The new version allows for a microphysical aerosol effect on clouds. For this, we use the optional two-moment cloud microphysical scheme in COSMO and the online-computed aerosol information for cloud condensation nuclei concentrations (Cccn), replacing the constant Cccn profile. In the radiation scheme, we have implemented a droplet-size-dependent cloud optical depth, allowing now for aerosol–cloud–radiation interactions. To evaluate the models with satellite data, the Cloud Feedback Model Intercomparison Project Observation Simulator Package (COSP) has been implemented. A case study has been carried out to understand the effects of the modifications, where the modified modeling system is applied over the European domain with a horizontal resolution of 0.25°  ×  0.25°. To reduce the complexity in aerosol–cloud interactions, only warm-phase clouds are considered. We found that the online-coupled aerosol introduces significant changes for some cloud microphysical properties. The cloud effective radius shows an increase of 9.5 %, and the cloud droplet number concentration is reduced by 21.5 %.

scholarly journals Cloud activation properties of aerosol particles in a continental Central European urban environment

2021 ◽  
Vol 21 (14) ◽  
pp. 11289-11302
Author(s):  
Imre Salma ◽  
Wanda Thén ◽  
Máté Vörösmarty ◽  
András Zénó Gyöngyösi
Keyword(s):  
Chemical Composition ◽  
Particle Number ◽  
Cloud Condensation Nuclei ◽  
Aerosol Particles ◽  
Number Concentration ◽  
Urban Aerosol ◽  
Condensation Nuclei ◽  
Frequency Distributions ◽  
Remote Locations ◽  
Cloud Activation

Abstract. Collocated measurements using a condensation particle counter, differential mobility particle sizer and cloud condensation nuclei counter were realised in parallel in central Budapest from 15 April 2019 to 14 April 2020 to gain insight into the cloud activation properties 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 supersaturation (S) values 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. The CCN concentrations represented 7–27 % of all particles. The CCN concentrations were considerably larger but the activation fractions were systematically substantially smaller than observed in regional or remote locations. The effective critical dry particle diameters (dc,eff) were derived utilising the CCN concentrations and particle number size distributions. Their median values at the five supersaturation values considered were 207, 149, 126, 105 and 80 nm, respectively; all of these diameters were positioned within the accumulation mode of the typical particle number size distribution. Their frequency distributions revealed a single peak for which the geometric standard deviation increased monotonically with S. This broadening indicated high time variability in the activating properties of smaller particles. The frequency distributions also showed fine structure, with several compositional elements that seemed to reveal a consistent or monotonical tendency with S. The relationships between the critical S and dc,eff suggest that urban aerosol particles in Budapest with diameters larger than approximately 130 nm showed similar hydroscopicity to corresponding continental aerosol particles, whereas smaller particles in Budapest were less hygroscopic than corresponding continental aerosol particles. Only modest seasonal cycling in CCN concentrations and activation fractions was seen, and only for large S values. This cycling likely reflects changes in the number concentration, chemical composition and mixing state of the particles. The seasonal dependencies of dc,eff were featureless, indicating that the droplet activation properties of the urban particles remained more or less the same throughout the year. This is again different from what is seen in non-urban locations. Hygroscopicity parameters (κ values) were computed without determining the time-dependent chemical composition of the particles. The median values for κ were 0.15, 0.10, 0.07, 0.04 and 0.02, respectively, at the five supersaturation values considered. The averages suggested that the larger particles were considerably more hygroscopic than the smaller particles. We found that the κ values for the urban aerosol were substantially smaller than those previously reported for aerosols in regional or remote locations. All of these characteristics can be linked to the specific source composition of particles in cities. The relatively large variability in the hygroscopicity parameters for a given S emphasises that the individual values represent the CCN population in ambient air while the average hygroscopicity parameter mainly corresponds to particles with sizes close to the effective critical dry particle diameter.

scholarly journals Intercomparison of modal and sectional aerosol microphysics representations within the same 3-D global chemical transport model

2012 ◽  
Vol 12 (1) ◽  
pp. 623-689 ◽  
Author(s):  
G. W. Mann ◽  
K. S. Carslaw ◽  
D. A. Ridley ◽  
D. V. Spracklen ◽  
K. J. Pringle ◽  
...  
Keyword(s):  
Size Distribution ◽  
Transport Model ◽  
Cloud Condensation Nuclei ◽  
Particle Growth ◽  
Free Troposphere ◽  
Chemical Transport Model ◽  
Condensation Nuclei ◽  
Chemistry Transport Model ◽  
Surface Mass ◽  
Cloud Processing

Abstract. A global modal aerosol microphysics module (GLOMAP-mode) is evaluated and improved by comparing against a sectional version (GLOMAP-bin) and observations in the same 3-D global offline chemistry transport model. With both schemes, the model captures the main features of the global particle size distribution, with sub-micron aerosol approximately unimodal in continental regions and bi-modal in marine regions. Initial bin-mode comparisons showed that various size distribution parameter settings (mode widths and inter-modal separation sizes) resulted in clear biases compared to the sectional scheme. By adjusting these parameters in the modal scheme, much better agreement is achieved against the bin scheme and observations. Surface mass of sulphate, sea-salt, black carbon (BC) and organic carbon (OC) are, on the annual mean, within 25 % in the two schemes in nearly all regions. On the annual mean, surface level concentrations of condensation nuclei (CN), cloud condensation nuclei (CCN), surface area density and condensation sink also compare within 25 % in most regions. However, marine CCN concentrations between 30° N and 30° S are systematically higher in the modal scheme, by 25–60 %, which we attribute to differences in size-resolved particle growth or cloud-processing. Larger differences also exist in regions or seasons dominated by biomass burning and in free-troposphere and high-latitude regions. Indeed, in the free-troposphere, GLOMAP-mode BC is a factor 2–4 higher than GLOMAP-bin, likely due to differences in size-resolved scavenging. Nevertheless, in most parts of the atmosphere, we conclude that bin-mode differences are much less than model-observation differences, although some processes are missing in these runs which may pose a bigger challenge to modal schemes (e.g. boundary layer nucleation, ultra-fine sea-spray). The findings here underline the need for a spectrum of complexity in global models, with size-resolved aerosol properties predicted by modal schemes needing to be continually benchmarked and improved against freely evolving sectional schemes and observations.

scholarly journals ModelE2-TOMAS development and evaluation using aerosol optical depths, mass and number concentrations

2014 ◽  
Vol 7 (5) ◽  
pp. 5831-5918 ◽  
Author(s):  
Y. H. Lee ◽  
P. J. Adams ◽  
D. T. Shindell
Keyword(s):  
Organic Matter ◽  
General Circulation ◽  
Mineral Dust ◽  
Cloud Condensation Nuclei ◽  
Circulation Model ◽  
Convective Transport ◽  
Sea Salt ◽  
Computationally Efficient ◽  
Anthropogenic Aerosol ◽  
Aerosol Model

Abstract. The TwO-Moment Aerosol Sectional microphysics model (TOMAS) has been integrated into the state-of-the-art general circulation model, GISS ModelE2. TOMAS has the flexibility to select a size resolution as well as the lower size cutoff. A computationally efficient version of TOMAS is used here, which has 15 size bins covering 3 nm to 10 μm aerosol dry diameter. For each bin, it simulates the total aerosol number concentration and mass concentrations of sulphate, pure elementary carbon (hydrophobic), mixed elemental carbon (hydrophilic), hydrophobic organic matter, hydrophilic organic matter, sea salt, mineral dust, ammonium, and aerosol-associated water. This paper provides a detailed description of the ModelE2-TOMAS model and evaluates the model against various observations including aerosol precursor gas concentrations, aerosol mass and number concentrations, and aerosol optical depths. Additionally, global budgets in ModelE2-TOMAS are compared with those of other global aerosol models, and the TOMAS model is compared to the default aerosol model in ModelE2, which is a bulk aerosol model. Overall, the ModelE2-TOMAS predictions are within the range of other global aerosol model predictions, and the model has a reasonable agreement with observations of sulphur species and other aerosol components as well as aerosol optical depth. However, ModelE2-TOMAS (as well as the bulk aerosol model) cannot capture the observed vertical distribution of sulphur dioxide over the Pacific Ocean possibly due to overly strong convective transport. The TOMAS model successfully captures observed aerosol number concentrations and cloud condensation nuclei concentrations. Anthropogenic aerosol burdens in the bulk aerosol model running in the same host model as TOMAS (ModelE2) differ by a few percent to a factor of 2 regionally, mainly due to differences in aerosol processes including deposition, cloud processing, and emission parameterizations. Larger differences are found for naturally emitted aerosols such as sea salt and mineral dust. With TOMAS, ModelE2 has three different aerosol models (the bulk aerosol model and modal-based aerosol microphysics model, MATRIX) and allows exploration of the uncertainties associated with aerosol modelling within the same host model, NASA GISS ModelE2.

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