Sensitivity of sulphate aerosol size distributions and CCN concentrations over North America to SOx emissions and H2O2 concentrations

Salzen, Knut von; Leighton, H.G.; Ariya, Parisa A.; Barrie, Leonard A.; Gong, Sunling; Blanchet, J.; Spaček, Ľuboš; Lohmann, Ulrike; Kleinman, Lawrence I.

doi:10.1029/2000jd900027

Cited by 55 publications

(61 citation statements)

References 75 publications

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“…The model accounts for in-cloud oxidation in deep and shallow convection, and stratiform clouds with hydrogen peroxide (H 2 O 2 ) and ozone (O 3 ) as oxidants (von Salzen et al, 2000). The oxidation rates depend on the pH of the cloud water (Table 2), which is calculated from an ion balance for the dissolution of the chemical species SO 2 , ammonia (NH 3 ), nitric acid (HNO 3 ), and carbon dioxide (CO 2 ) in could droplets (von Salzen et al, 2000).…”

Section: Tracer Horizontal Diffusionmentioning

confidence: 99%

“…The oxidation rates depend on the pH of the cloud water (Table 2), which is calculated from an ion balance for the dissolution of the chemical species SO 2 , ammonia (NH 3 ), nitric acid (HNO 3 ), and carbon dioxide (CO 2 ) in could droplets (von Salzen et al, 2000). For in-cloud oxidation in deep convection, the cumulus cloud fraction is calculated from the precipitation flux (Slingo, 1987).…”

Section: Tracer Horizontal Diffusionmentioning

confidence: 99%

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The Canadian Fourth Generation Atmospheric Global Climate Model (CanAM4). Part I: Representation of Physical Processes

et al. 2013

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The Canadian Centre for Climate Modelling and Analysis (CCCma) has developed the fourth generation of the Canadian Atmospheric Global Climate Model (CanAM4). The new model includes substantially modified physical parameterizations compared to its predecessor. In particular, the treatment of clouds, cloud radiative effects, and precipitation has been modified. Aerosol direct and indirect effects are calculated based on a bulk aerosol scheme. Simulation results for present-day global climate are analyzed, with a focus on cloud radiative effects and precipitation. Good overall agreement is found between climatological mean short-and longwave cloud radiative effects and observations from the Clouds and Earth's Radiant Energy System (CERES) experiment. An analysis of the responses of cloud radiative effects to variations in climate will be presented in a companion paper.RÉSUMÉ [Traduit par la rédaction] Le Centre canadien de la modélisation et de l'analyse climatique (CCmaC) a mis au point la quatrième génération du modèle canadien de circulation générale de l'atmosphère (CanAM4). Le nouveau modèle comprend des paramétrisations physiques passablement modifiées comparativement à son prédé-cesseur. En particulier, le traitement des nuages, des effets radiatifs des nuages et des précipitations a été modifié. Les effets directs et indirects des aérosols sont calculés à l'aide d'un schéma d'aérosols en bloc. Nous analysons des résultats de simulation pour le climat général du jour présent en mettant l'accent sur les effets radiatifs des nuages et les précipitations. Nous trouvons un bon accord général entre la moyenne climatologique des effets radiatifs des nuages pour les courtes et les grandes longueurs d'onde et les observations de l'expérience CERES (Clouds and Earth's Radiant Energy System). Une analyse de la réponse des effets radiatifs des nuages aux variations du climat sera présentée dans un article connexe.

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Section: Tracer Horizontal Diffusionmentioning

confidence: 99%

Section: Tracer Horizontal Diffusionmentioning

confidence: 99%

The Canadian Fourth Generation Atmospheric Global Climate Model (CanAM4). Part I: Representation of Physical Processes

et al. 2013

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“…The sulphate mass produced by the scheme in clouds is over the activated aerosol spectrum, i.e. cloud droplets [von Salzen et al, 2000]. Since the oxidation chemistry of sulphur species depends on droplet pH, size-dependent chemistry may yield more realistic results.…”

Section: Cloud Chemistrymentioning

confidence: 99%

Canadian Aerosol Module: A size‐segregated simulation of atmospheric aerosol processes for climate and air quality models 1. Module development

Gong¹,

et al. 2003

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[1] A size-segregated multicomponent aerosol algorithm, the Canadian Aerosol Module (CAM), was developed for use with climate and air quality models. It includes major aerosol processes in the atmosphere: generation, hygroscopic growth, coagulation, nucleation, condensation, dry deposition/sedimentation, below-cloud scavenging, aerosol activation, a cloud module with explicit microphysical processes to treat aerosol-cloud interactions and chemical transformation of sulphur species in clear air and in clouds. The numerical solution was optimized to efficiently solve the complicated size-segregated multicomponent aerosol system and make it feasible to be included in global and regional models. An internal mixture is assumed for all types of aerosols except for soil dust and black carbon which are assumed to be externally mixed close to sources. To test the algorithm, emissions to the atmosphere of anthropogenic and natural aerosols are simulated for two aerosol types: sea salt and sulphate. A comparison was made of two numerical solutions of the aerosol algorithm: process splitting and ordinary differential equation (ODE) solver. It was found that the process-splitting method used for this model is within 15% of the more accurate ODE solution for the total sulphate mass concentration and <1% accurate for sea-salt concentration. Furthermore, it is computationally more than 100 times faster. The sensitivity of the simulated size distributions to the number of size bins was also investigated. The diffusional behavior of each individual process was quantitatively characterized by the difference in the mode radius and standard deviation of a lognormal curve fit of distributions between the approximate solution and the 96-bin reference solution. Both the number and mass size distributions were adequately predicted by a sectional model of 12 bins in many situations in the atmosphere where the sink for condensable matter on existing aerosol surface area is high enough that nucleation of new particles is negligible. Total mass concentration was adequately simulated using lower size resolution of 8 bins. However, to properly resolve nucleation mode size distributions and minimize the numerical diffusion, a sectional model of 18 size bins or greater is needed. The number of size bins is more important in resolving the nucleation mode peaks than in reducing the diffusional behavior of aerosol processes. Application of CAM in a study of the global cycling of sea-salt mass accompanies this paper [Gong et al., 2002].

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“…A variation on this approach is the quadrature method of moments (McGraw, 1997) which does not make any assumption about the functional form of the aerosol size distribution, instead solving for the moments of the distribution using a Gaussian quadrature approximation to the integral growth term in the ADEs (Wright et al, 2000;Wright and Kasibhatla, 2001;Wright et al, 2002;Yu et al, 2003;McGraw and Wright, 2003). An alternative approach is to describe the size distribution in terms of discrete size sections (Tegen and Fung, 1994;Gong et al, 1997;Jacobson, 2001a;von Salzen et al, 2000;Jacobson, 2001b;Adams and Seinfeld, 2002;. The sectional approach is relatively computationally expensive because at least 20 size sections are needed to represent the distribution.…”

Section: Introductionmentioning

confidence: 99%

“…Early sectional schemes used a single-moment sectional method (von Salzen et al, 2000) in which the particle number in each size section is simulated. Later sectional schemes used a two-moment sectional method in which the mass per particle in each section is also simulated.…”

Section: Introductionmentioning

confidence: 99%

A global off-line model of size-resolved aerosol microphysics: I. Model development and prediction of aerosol properties

et al. 2005

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Abstract.A GLObal Model of Aerosol Processes (GLOMAP) has been developed as an extension to the TOMCAT 3-D Eulerian off-line chemical transport model. GLOMAP simulates the evolution of the global aerosol size distribution using a sectional two-moment scheme and includes the processes of aerosol nucleation, condensation, growth, coagulation, wet and dry deposition and cloud processing. We describe the results of a global simulation of sulfuric acid and sea spray aerosol. The model captures features of the aerosol size distribution that are well established from observations in the marine boundary layer and free troposphere. Modelled condensation nuclei (CN >3 nm) vary between about 250-500 cm −3 in remote marine boundary layer regions and are generally in good agreement with observations. Modelled continental CN concentrations are lower than observed, which may be due to lack of some primary aerosol sources or the neglect of nucleation mechanisms other than binary homogeneous nucleation of sulfuric acidwater particles. Remote marine CN concentrations increase to around 2000-10 000 cm −3 (at standard temperature and pressure) in the upper troposphere, which agrees with typical observed vertical profiles. Cloud condensation nuclei (CCN) at 0.2% supersaturation vary between about 1000 cm −3 in polluted regions and between 10 and 500 cm −3 in the remote marine boundary layer. New particle formation through sulfuric acid-water binary nucleation occurs predominantly in the upper troposphere, but the model results show that these particles contribute greatly to aerosol concentrations in the marine boundary layer. For this sulfur-sea salt system it is estimated that sea spray emissions account for only ∼10% of CCN in the tropical marine boundary layer, but between 20 and 75% in the mid-latitude Southern Ocean. In a run with only natural sulfate and sea salt emissions the global mean surface CN concentration is more than 60% of that from a run Correspondence to: D. V. Spracklen (dominick@env.leeds.ac.uk) with 1985 anthropogenic sulfur emissions, although the natural emissions comprise only 27% of total sulfur emissions. Southern hemisphere marine boundary layer CN are more than 90% natural in origin, while polluted continental CN are more than 90% anthropogenic in origin, although these numbers will change when other anthropogenic CN sources are included in the model.

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Sensitivity of sulphate aerosol size distributions and CCN concentrations over North America to SO_x emissions and H₂O₂ concentrations

Cited by 55 publications

References 75 publications

The Canadian Fourth Generation Atmospheric Global Climate Model (CanAM4). Part I: Representation of Physical Processes

The Canadian Fourth Generation Atmospheric Global Climate Model (CanAM4). Part I: Representation of Physical Processes

Canadian Aerosol Module: A size‐segregated simulation of atmospheric aerosol processes for climate and air quality models 1. Module development

A global off-line model of size-resolved aerosol microphysics: I. Model development and prediction of aerosol properties

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