Microscopic Evidence for Phase Separation of Organic Species and Inorganic Salts in Fine Ambient Aerosol Particles
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Phase separation is an important microscopic phenomenon in aerosol particles and reflects the surface properties of particles and the aging degree of organic components. However, few data are available to directly reveal phase separation in ambient aerosol particles, although there are abundant data from laboratory experiments. In this study, different state-of-the-art microscopic technologies were used to study the phase separation of organic matter (OM) and inorganic salts in individual particles collected from different atmospheric environments, with one type of surrogate particles prepared in the laboratory. We found that most of the collected particles with an equivalent sphere diameter of >100 nm have a secondary inorganic aerosol core with OM coating in the continental atmosphere. In addition, secondary inorganic aerosol and OM phase separation are more frequent in rural particles than suburban particles, suggesting that particle aging enhances the phase separation. Our results show that the phase separation is a frequent phenomenon that forms organic coatings on inorganic particles of individual particles (>100 nm), and their number abundances depend on the particle size and OM aging degree. The resulting morphology shows that OM is an important particle surface in the atmosphere, which influences gas partitioning, optical and hygroscopic properties, and cloud condensation nuclei formation activities.Keywords:
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Abstract. This paper assesses the impact of aerosol properties on the formation and the development of radiation fog. Simulations were performed using the Meso-NH meteorological model including the ORILAM aerosol scheme coupled with a two-moment microphysical cloud scheme (number concentration of cloud droplets and cloud water content). The activation scheme used was taken from the work of Abdul-Razzak and Ghan (2004). "Off-line" sensitivity analysis of CCN (Cloud Condensation Nuclei) activation was performed on number, median diameter and chemical compounds of aerosols. During this "off-line" study, the interactions with the other physical processes (e.g. radiative) were not taken into account since the cooling rate was imposed. Different regimes of CCN activation and a critical value of aerosol number concentration were found. This critical aerosol number corresponds to the maximum of activated cloud droplets for a given cooling rate and given aerosol chemical properties. As long as the aerosol number concentration is below this critical value, the cloud droplet number increases when the aerosol number increases. But when the aerosol number concentration exceeds this critical value, the cloud droplet number decreases when aerosol number increases. A sensitivity study on aerosol chemical composition showed that the CCN activation was limited in the case of hydrophilic aerosol composed of material with a solubility in the 10% range. An event observed during the ParisFOG field experiment was simulated. This case took place in the polluted sub-urban area of Paris (France) characterized by particle concentrations of 17 000 aerosols per cm3. 1D simulations successfully reproduced the observed temporal evolution of the fog layer. Beyond the initial fog formation at the surface, cloud droplet formation occurred at the top of the fog layer where the cooling rate was maximum, reaching more than −10 K h−1. These simulations confirm that the aerosol particle number concentration is a key parameter for the accurate prediction of the microphysical properties of a fog layer and also influences the vertical development of fog. The important of the interaction between microphysical and radiative processes is illustrated, showing how the life cycle of a fog layer is determined by the CCN number concentration and chemical properties.
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Abstract. An aerosol model was used to simulate the generation and transport of aerosols over Germany during the HD(CP)2 Observational Prototype Experiment (HOPE) field campaign of 2013. The aerosol number concentrations and size distributions were evaluated against observations, which shows satisfactory agreement in the magnitude and temporal variability of the main aerosol contributors to cloud condensation nuclei (CCN) concentrations. From the modelled aerosol number concentrations, number concentrations of CCN were calculated as a function of vertical velocity using a comprehensive aerosol activation scheme which takes into account the influence of aerosol chemical and physical properties on CCN formation. There is a large amount of spatial variability in aerosol concentrations; however the resulting CCN concentrations vary significantly less over the domain. Temporal variability is large in both aerosols and CCN. A parameterization of the CCN number concentrations is developed for use in models. The technique involves defining a number of best fit functions to capture the dependence of CCN on vertical velocity at different pressure levels. In this way, aerosol chemical and physical properties as well as thermodynamic conditions are taken into account in the new CCN parameterization. A comparison between the parameterization and the CCN estimates from the model data shows excellent agreement. This parameterization may be used in other regions and time periods with a similar aerosol load; furthermore, the technique demonstrated here may be employed in regions dominated by different aerosol species.
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Abstract. This paper explores the impacts of primary carbonaceous aerosol on cloud condensation nuclei (CCN) concentrations in a global climate model with size-resolved aerosol microphysics. Organic matter (OM) and elemental carbon (EC) from two emissions inventories were incorporated into a preexisting model with sulfate and sea-salt aerosol. The addition of primary carbonaceous aerosol increased CCN(0.2%) concentrations by 65–90% in the globally averaged surface layer depending on the carbonaceous emissions inventory used. Sensitivity studies were performed to determine the relative importance of organic solubility/hygroscopicity in predicting CCN. In a sensitivity study where carbonaceous aerosol was assumed to be completely insoluble, concentrations of CCN(0.2%) still increased by 40–50% globally over the no carbonaceous simulation because primary carbonaceous emissions were able to become CCN via condensation of sulfuric acid. This shows that approximately half of the contribution of primary carbonaceous particles to CCN in our model comes from the addition of new particles (seeding effect) and half from the contribution of organic solute (solute effect). The solute effect tends to dominate more in areas where there is less inorganic aerosol than organic aerosol and the seeding effect tends to dominate in areas where there is more inorganic aerosol than organic aerosol. It was found that an accurate simulation of the number size distribution is necessary to predict the CCN concentration but assuming an average chemical composition will generally give a CCN concentration within a factor of 2. If a "typical" size distribution is assumed for each species when calculating CCN, such as is done in bulk aerosol models, the mean error relative to a simulation with size resolved microphysics is on the order of 35%. Predicted values of carbonaceous aerosol mass and aerosol number were compared to observations and the model showed average errors of a factor of 3 for carbonaceous mass and a factor of 4 for total aerosol number; however, errors in the accumulation mode concentrations were found to be lower in comparisons with European and marine observations.. The errors in CN and carbonaceous mass may be reduced by improving the emission size distributions of both primary sulfate and primary carbonaceous aerosol.
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This paper describes the effect of the presence of water-soluble organic compounds (WSOC) in aerosol particles on the aerosol critical supersaturation as defined by the Köhler theory and on cloud condensation nuclei (CCN) number concentration. Taking into account both the soluble mass increase and the surface tension depression due to WSOC, we calculated a substantial decrease of the aerosol critical supersaturation, which results in a large increase in CCN number concentration. CCN supersaturation spectra were computed for three different aerosol types: marine, rural and urban. The increase of CCN number concentration in the presence of WSOC (with respect to the case when only the inorganic aerosol compounds are considered) varies with aerosol type, with an increase up to 13% in the marine case, up to 97% in the rural case, and up to 110% in the urban case, for the supersaturation range typical of atmospheric conditions.
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Abstract. This paper explores the impacts of carbonaceous aerosol on cloud condensation nuclei (CCN) concentrations in a global climate model with size-resolved aerosol microphysics. Organic matter (OM) and elemental carbon (EC) from two emissions inventories were incorporated into a preexisting model with sulfate and sea-salt aerosol. The addition of carbonaceous aerosol increased CCN(0.2%) concentrations by 65–90% in the globally averaged surface layer depending on the carbonaceous emissions inventory used. Sensitivity studies were performed to determine the relative importance of the organic "solute effect", in which CCN concentrations increase because of the added soluble carbonaceous material, versus the "seeding effect", in which CCN concentrations increase because of increased particle number concentrations. In a sensitivity study where carbonaceous aerosol was assumed to be completely insoluble, concentrations of CCN(0.2%) still increased by 40–50% globally over the no carbonaceous simulation because primary carbonaceous emissions were able to become CCN via condensation of sulfuric acid. This shows that approximately half of the contribution of carbonaceous particles to CCN comes from the "seeding effect" and half from the "solute effect". The solute effect tends to dominate more in areas where there is less inorganic aerosol than organic aerosol and the seeding effect tends to dominate in areas where is more inorganic aerosol than organic aerosol. It was found that an accurate simulation of the number size distribution is necessary to predict the CCN concentration but assuming an average chemical composition will generally give a CCN concentration within a factor of 2. If a "typical" size distribution is assumed for each species when calculating CCN, such as is done in bulk aerosol models, the mean error relative to a simulation with size resolved microphysics is on the order of 35%. Predicted values of carbonaceous aerosol mass and aerosol number were compared to observations and the model showed average errors of a factor of 3 for carbonaceous mass and a factor of 4 for total aerosol number. These errors may be reduced by improving the emission size distributions of both primary sulfate and primary carbonaceous aerosol.
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Abstract. An aerosol model was used to simulate the generation and transportation of aerosols over Germany during the HD(CP)2 Observational Prototype Experiment (HOPE) field campaign of 2013. The aerosol number concentrations and size distributions were evaluated against observations, which shows satisfactory agreement in the magnitude and temporal variability of the main aerosol contributors to cloud condensation nuclei (CCN) concentrations. From the modelled aerosol number concentrations, number concentrations of CCN were calculated as a function of vertical velocity using a comprehensive aerosol activation scheme which takes into account the influence of aerosol chemical and physical properties on CCN formation. There is a large amount of spatial variability in aerosol concentrations, however the resulting CCN concentrations vary significantly less over the domain. Temporal variability is large in both aerosols and CCN. A parameterisation of the CCN number concentrations is developed for use in models. The technique involves defining a number of best fit functions to capture the dependence of CCN on vertical velocity at different pressure levels. In this way, aerosol chemical and physical properties as well as thermodynamic conditions are taken into account in the new CCN parameterisation. A comparison between the parameterisation and the CCN estimates from the model data shows excellent agreement. This parameterisation may be used in other regions and time periods with a similar aerosol load, and furthermore, this technique demonstrated here may be employed in regions dominated by different aerosol species.
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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.
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This paper describes the effect of the presence of water-soluble organic compounds (WSOC) in aerosol particles on the aerosol critical supersaturation as defined by the Köhler theory and on cloud condensation nuclei (CCN) number concentration. Taking into account both the soluble mass increase and the surface tension depression due to WSOC, we calculated a substantial decrease of the aerosol critical supersaturation, which results in a large increase in CCN number concentration. CCN supersaturation spectra were computed for three different aerosol types: marine, rural and urban. The increase of CCN number concentration in the presence of WSOC (with respect to the case when only the inorganic aerosol compounds are considered) varies with aerosol type, with an increase up to 13% in the marine case, up to 97% in the rural case, and up to 110% in the urban case, for the supersaturation range typical of atmospheric conditions.
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Abstract Formation of secondary organic aerosols (SOA) through the atmospheric oxidation of organic vapors has potential to enable particle growth to cloud condensation nuclei (CCN)‐relevant sizes. In this work, we constrain a global aerosol model by using aircraft measurements to reveal the global importance of SOA formation in CCN production. Our improved model, with explicit size‐resolved aerosol microphysics and parametrizations of semivolatile organic oxidation products, presents a state‐of‐the‐art performance in simulating both particle number concentrations and organic aerosol concentrations dominated (80–95%) by SOA in the remote atmosphere, which have been challenges in previous modeling studies. The SOA formation in concert with aerosol nucleation contributes to more than 50% of CCN concentrations in those pristine environments featuring low background aerosol concentrations. We estimate that the SOA‐derived CCN alters the magnitude of cloud radiative forcing by ∼0.1 W m −2 . Our findings underscore the necessity for aerosol‐climate models to represent controls on CCN concentrations by SOA production.
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