Variation of the mixing state of Saharan dust particles with atmospheric transport

Mineral dust is an important aerosol species in the Earth’s atmosphere and has a major source within North Africa, of which the Sahara forms the major part. Aerosol Time of Flight Mass Spectrometry (ATOFMS) is first used to determine the mixing state of dust particles collected from the land surface in the Saharan region, showing low abundance of species such as nitrate and sulphate internally mixed with the dust mineral matrix. These data are then compared with the ATOFMS single particle mass spectra of Saharan dust particles detected in the marine atmosphere in the vicinity of the Cape Verde islands, which are further compared with those from particles with longer atmospheric residence sampled at a coastal station at Mace Head, Ireland. Saharan dust particles collected near the Cape Verde Islands showed increased internally mixed nitrate but no sulphate, whilst Saharan dust particles collected on the coast of Ireland showed a very high degree of internally mixed secondary species including nitrate, sulphate and methanesulphonate. This uptake of secondary species will change the pH and hygroscopic properties of the aerosol dust and thus can influence the budgets of other reactive gases, as well as influencing the radiative properties of the particles and the availability of metals for dissolution.     

Observed chemical characteristics of long-range transported particles at a marine background site in Korea

Deokjeok Island is located off the west coast of the Korean Peninsula and is a suitable place to monitor the long-range transport of air pollutants from the Asian continent. In addition to pollutants, Asian dust particles are also transported to the island during long-range transport events. Episodic transport of dust and secondary particles was observed during intensive measurements in the spring (March 31-April 11) and fall (October 13-26) of 2009. In this study, the chemical characteristics of long-range-transported particles were investigated based on highly time-resolved ionic measurements with a particle-into-liquid system coupled with an online ion chromatograph (PILS-IC) that simultaneously measures concentrations of cations (Li+, Na , NH4+, K+, Ca2+, Mg2+) and anions (F-, C1-, NO3-, SO42-). The aerosol optical thickness (AOT) distribution retrieved by the modified Bremen Aerosol Retrieval (M-BAER) algorithm from moderate resolution imaging spectroradiometer (MODIS) satellite data confirmed the presence of a thick aerosol plume coming from the Asian continent towards the Korean peninsula. Seven distinctive events involving the long-range transport (LRT) of aerosols were identified and studied, the chemical components of which were strongly related to sector sources. Enrichment of acidic secondary aerosols on mineral dust particles, and even of sea-salt components, during transport was observed in this study. Backward trajectory, chemical analyses, and satellite aerosol retrievals identified two distinct events: a distinctively high [Ca2++Mg2]/[Na+] ratio (>2.0), which was indicative of a preprocessed mineral dust transport event, and a low [Ca2++Mg2+]/[Na+] ratio (<2.0), which was indicative of severe aging of sea-salt components on the processed dust particles. Particulate C1- was depleted by up to 85% in spring and 50% in the fall. A consistent fraction of carbonate replacement (FCR) averaged 0.53 in spring and 0.55 in the fall. Supporting evidences of C1- enrichment on the marine boundary layer prior to a dust front were also found. Supplemental materials are available for this article. Go to the publisher's online edition of the Journal of the Air & Waste Management Association for sector and air mass classifications of clean and LRT cases.     

Size-segregated chemistry of particulate dicarboxylic acids in the Arctic atmosphere

Gas–particle interactions of low-molecular-weight dicarboxylic acids were studied at a coastal Arctic site during the summer. Size segregated measurements with a Berner low-pressure impactor displayed up to four modes for ionic compounds: an Aitken mode, an accumulation mode, and two supermicron modes. The lower supermicron mode was ascribed to sea-salt, whereas the upper mode consisted mostly of species associated with continental particles. All four modes could be identified for oxalic acid, with the lower supermicron mode being the dominant. Malonic acid displayed a supermicron mode but was not found in the submicron size range. Succinic acid had an accumulation mode and, in a few samples, a supermicron mode. Glutaric acid displayed sometimes and accumulation mode, sometimes a supermicron mode, and occasionally both. The most probable formation pathway for submicron oxalic and glutaric acid was condensation from the gas phase, even though production in cloud droplets cannot be ruled out either. A slightly different formation pathway may have been important for submicron succinic acid production. Supermicron oxalic acid was probably formed by condensation from the gas-phase, by heterogeneous reactions occurring on the surface of pre-existing sea-salt and continental particles, or in cloud droplets. A larger mass median diameter for supermicron malonic and glutaric acid might be indicative of liquid-phase production in aqueous sea-salt particles. Evidence on possibly substantial sampling artifacts related to measuring dicarboxylic acids using filters were also obtained.     

The aging process of naturally emitted aerosol (sea-salt and mineral aerosol) during long range transport

The aging processes of two representative natural aerosol, sea-salt and mineral aerosol, are investigated by using a box model equipped with a thermodynamic module (SCAPE). The model is shown to successfully describe the aging processes between the gas-phase anthropogenic pollutants (SO₂, NO_x, and NH₃) and primary aerosol particles, including self-neutralization process/chlorine depletion in the sea-salt aerosol; formation/dissipation of carbonate and bicarbonate ions in the mineral aerosol; irreversible dynamic deposition of SO₂ and H₂SO₄; and reversible thermodynamic distribution of inorganic volatile species. It is found that SO₂ and H₂SO₄ tend to deposit onto the mode with the largest surface area, and that ammonia deposition is controlled by preceding SO₂/H₂SO₄ deposition. During the SO₂/H₂SO₄ deposition, chloride and carbonate are continuously released from the sea-salt and mineral dust particles, respectively. The findings by the model predictions are consistent with field and observational studies.     

Ion balances of size-resolved tropospheric aerosol samples: implications for the acidity and atmospheric processing of aerosols

A large set of size-resolved aerosol samples was inspected with regard to their ion balance to shed light on how the aerosol acidity changes with particle size in the lower troposphere and what implications this might have for the atmospheric processing of aerosols. Quite different behaviour between the remote and more polluted environments could be observed. At the remote sites, practically the whole accumulation mode had cation-to-anion ratios clearly below unity, indicating that these particles were quite acidic. The supermicron size range was considerably less acidic and may in some cases have been close to neutral or even alkaline. An interesting feature common to the remote sites was a clear jump in the cation-to-anion ratio when going from the accumulation to the Aitken mode. The most likely reason for this was cloud processing which, via in-cloud sulphate production, makes the smallest accumulation-mode particles more acidic than the non-activated Aitken-mode particles. A direct consequence of the less acidic nature of the Aitken mode is that it can take up semi-volatile, water-soluble gases much easier than the accumulation mode. This feature may have significant implications for atmospheric cloud condensation nuclei production in remote environments. In rural and urban locations, the cation-to-anion ratio was close to unity over most of the accumulation mode, but increased significantly when going to either larger or smaller particle sizes. The high cation-to-anion ratios in the supermicron size range were ascribed to carbonate associated with mineral dust. The ubiquitous presence of carbonate in these particles indicates that they were neutral or alkaline, making them good sites for heterogeneous reactions involving acidic trace gases. The high cation-to-anion ratios in the Aitken mode suggest that these particles contained some water-soluble anions not detected by our chemical analysis. This is worth keeping in mind when investigating the hygroscopic properties or potential health effects of ultrafine particles in polluted environments.     

Halogen production from aqueous tropospheric particles

Box model studies have been performed to study the role of aqueous phase chemistry with regard to halogen activation for marine and urban clouds and the marine aerosol as well. Different chemical pathways leading to halogen activation in diluted cloud droplets and highly concentrated sea salt aerosol particles are investigated. The concentration of halides in cloud droplets is significantly smaller than in sea-salt particles, and hence different reaction sequences control the overall chemical conversions. In diluted droplets radical chemistry involving OH, NO(3), Cl/Cl(2)(-)/ClOH(-), and Br/Br(2)(-)/BrOH(-) gains in importance and pH independent pathways lead to the release of halogens from the particle phase whereas the chemistry in aerosol particles with high electrolyte concentrations is controlled by non-radical reactions at high ionic strengths and relatively low pH values.For the simulation of halogen activation in tropospheric clouds and aqueous aerosol particles in different environments a halogen module was developed including both gas and aqueous phase processes of halogen containing species. This module is coupled to a base mechanism consisting of RACM (Regional Atmospheric Chemistry Mechanism) and the Chemical Aqueous Phase Radical Mechanism CAPRAM 2.4 (MODAC-mechanism). Phase exchange is described by the resistance model by Chemistry of Multiphase Atmospheric Systems, NATO ASI Series, 1986.It can be shown that under cloud conditions the bromine atom is mainly produced by OH initiated reactions, i.e. its concentration maximum is reached at noon. In contrast, the concentration level of chlorine atoms is linked to NO(3) radical chemistry leading to a smaller amplitude between day and night time concentrations.The contribution of radical processes to halogen atom formation in the particle phase is evident, e.g. by halogen atoms which undergo direct phase transfer. Furthermore, the application of the multiphase model for initial concentrations for sea-salt aerosols shows that the particle phase can act as a main source of halogen containing molecules (Cl(2), BrCl, Br(2)) which are photolysed in the gas phase to yield halogen atoms (about 70% of all Cl sources and more than 99% for Br).     

Influence of natural events on the concentration and composition of atmospheric particulate matter

A ten-month field study aimed to determine the contribution of natural events (i.e. sea-salt and mineral dust events) to urban PM concentration was carried out at six sampling sites in Central Italy (Lazio region). Four indicators have been used to identify natural events during the period of the study. The first one is constituted by the ratio between number of particles in the coarse to the accumulation mode. It is simple, cheap, and the information are given in quasi-real time, but the nature of the event (sea-salt or mineral dust) is not detectable. The second indicator relies on the chemical analysis of the collected PM by X-ray fluorescence (XRF) and allows a robust identification of sea-salt and crustal components. The third one is based on diagnostic ratios of elemental fractions: Mg_extractable/Ti_residue for sea-salt and Ti_residue/Sb_residue for mineral dust. It requires skilled staff but it is most accurate and sensible. The last indicator, constructed on the basis of natural radioactivity data, is not diagnostic for the nature of the event but it is able to estimate the increase in PM concentration with respect to the expected concentration in the absence of natural events.The relevance of natural events and the variations in PM concentration and composition during the study are discussed. The joined use of the four indicators allowed the identification of about 20 natural PM episodes. In general, sea-salt aerosol events did not cause exceedance of the daily EU limit value for PM₁₀. Saharan dust events, instead, were in most cases responsible for the exceedance of the limit value at all stations.     

Soil-Atmosphere exchange of radiatively and chemically active gases

Exchanges between the soils and the atmosphere may control or significantly affect the global budgets of many environmentally important trace gases, both natural and man-made. Flux measurements, taken in several ecosystems, show that soils are a substantial source of chloroform (8 ± 4 μg/m²/d) and a sink for methyl chloride (-10 _-3 ⁺⁶ μg/m²/d). The known sources and sinks of these gases are insufficient to explain the observed concentrations. Our findings will help to balance the global budget of chloroform but may put the budget of methyl chloride further out of balance. We also found, consistent with previous research, that soils are a substantial source of nitrous oxide and carbon monoxide and take up hydrogen and methane. The uptake of man-made chlorocarbons was observed, but the rates are small. Observed fluxes of non-methane hydrocarbons showed few patterns except that soils may be a source of ethane and butane.     

Observations and modelling of aerosol growth in marine stratocumulus—case study

Airborne measurements of the growth of the marine accumulation mode after multiple cycles through stratocumulus cloud are presented. The nss-sulphate cloud residual mode was log-normal in spectral shape and it’s mode radius was observed to progressively increase in size from 0.78 to 0.94 μm over 155 min of air parcel evolution through the cloudy marine boundary layer. The primary reason for this observed growth was thought to result from aqueous phase oxidation of SO₂ to aerosol sulphate in activated cloud drops. An aqueous phase aerosol–cloud-chemistry model was used to simulate this case study of aerosol growth and was able to closely reproduce the observed growth. The model simulations illustrate that aqueous phase oxidation of SO₂ in cloud droplets was able to provide enough additional sulphate mass to increase the size of activated aerosol. During a typical cloud cycle simulation, ≈4.6 nmoles kg^-1_air (0.44 μg m^-3) of sulphate mass was produced with ≈70% of sulphate production occurring in cloud droplets activated upon sea-salt nuclei and ≈30% occurring upon nss-sulphate nuclei, even though sea-salt nuclei contributed less than 15% to the activated droplet population. The high fraction of nss-sulphate mass internally mixed with sea-salt aerosol suggests that aqueous phase oxidation of SO₂ in cloud droplets activated upon sea-salt nuclei is the dominant nss-sulphate formation mechanism and that sea-salt aerosol provides the primary chemical sink for SO₂ in the cloudy marine boundary layer.     

Air parcel model simulations of a convective cloud: Bacteria acting as immersion ice nuclei

The effects of bacteria acting as immersion ice nuclei were investigated in numerical sensitivity studies and compared to the efforts of other ice nuclei such as mineral dust and soot particles. An adiabatic air parcel model was employed simulating convective situations with different initial aerosol particle distributions. The maximum fractions of active ice nuclei were based on field measurements of the proportioning of atmospheric aerosol particle types in continental and marine air masses. Recent field measurements of bacteria concentrations in cloud water and in snow samples were used. From the concentrations in bulk samples the concentration in mean sized cloud droplets was estimated. Immersion freezing was described based on laboratory measurements to constrain the freezing fraction versus temperature. The results indicated that the effects of diminutive amounts of bacteria on ice formation in convective clouds, while being significantly less than the effects of mineral dust particles, might be comparable to the expected effects of soot particles acting as ice nuclei. It can be predicted that bacterial ice nuclei would have to be enriched by at least 10⁴ times reported concentrations in cloud water in order to equate to the impact of mineral dust ice nuclei present in 20–25% of all cloud droplets.     

Influence of dust composition on cloud droplet formation

Previous studies suggest that interactions between dust particles and clouds are significant; yet the conditions where dust particles can serve as cloud condensation nuclei (CCN) are uncertain. Since major dust components are insoluble, the CCN activity of dust strongly depends on the presence of minor components. However, many minor components measured in dust particles are overlooked in cloud modeling studies. Some of these compounds are believed to be products of heterogeneous reactions involving carbonates. In this study, we calculate Kohler curves (modified for slightly soluble substances) for dust particles containing small amounts of K⁺, Mg²⁺, or Ca²⁺ compounds to estimate the conditions where reacted and unreacted dust can activate. We also use an adiabatic parcel model to evaluate the influence of dust particles on cloud properties via water competition. Based on their bulk solubilities, K⁺ compounds, MgSO₄·7H₂O, Mg(NO₃)₂·6H₂O, and Ca(NO₃)₂·4H₂O are classified as highly soluble substances, which enable activation of fine dust. Slightly soluble gypsum and MgSO₃·6H₂O, which may form via heterogeneous reactions involving carbonates, enable activation of particles with diameters between about 0.6 and 2 μm under some conditions. Dust particles>2 μm often activate regardless of their composition. Only under very specialized conditions does the addition of a dust distribution into a rising parcel containing fine (NH₄)₂SO₄ particles significantly reduce the total number of activated particles via water competition. Effects of dust on cloud saturation and droplet number via water competition are generally smaller than those reported previously for sea salt. Large numbers of fine dust CCN can significantly enhance the number of activated particles under certain conditions. Improved representations of dust mineralogy and reactions in global aerosol models could improve predictions of the effects of aerosol on climate.     

Dust characteristics over the North Pacific observed through shipboard measurements during the ACE-Asia experiment

To examine the diversity of chemical and physical properties of aerosol particles, in particular dust, over the North Pacific, aerosols were collected along ∼32°N latitude between 140°E and 170°W longitude aboard the NOAA R/V Ronald H. Brown during the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia) in the spring 2001. A total of 11,482 aerosol particles were examined through individual-particle analysis. Results indicate that dust particles over this region were dominated primarily by Si-rich particles, including aluminosilicates that contain Fe. Fe is also present as separate Fe-rich particles. Additional common particle types include Ca- and S-rich particles; many of the later appear to represent soil-derived calcium carbonate and its reaction products whereas the former are predominantly reaction products of sea salt and sulfate. Particles are often aggregates of different types including pollution-derived substances and highly heterogeneous, both internally and externally. Dust particles are non-spherical, having circularities from 1.0 up to 4.5, suggesting the high degree of complexity of particle shape. The majority of dust particles were dominated by particles with median diameters from 0.67 to 1.26 μm. However, dust particles with diameters of 5 μm or even larger do exist associated with those events of dust originated from Asian desert areas. The existence of soot and Fe-rich particles over this region indicates the influence of fossil fuel sources in Asia. Aerosol Fe from both Asian desert and fossil fuel combustion may contribute to the nutrient Fe in the surface waters of the North Pacific basin. Therefore, the transport of Asian dust associated with species of fossil fuel burning in the spring may play an important role in altering the natural composition of aerosols over the North Pacific.     

Heterogeneous loss of HO2 by KCl,synthetic sea salt,and natural seawater aerosol particles

The HO₂ uptake to aerosol particles is potentially significant sink for the HO₂ radical in the marine atmosphere. To assess the heterogeneous loss of HO₂ on marine aerosol particles, we have investigated the uptake coefficients (γ) of HO₂ for submicron aerosol particles of KCl, synthetic sea salt, and natural seawater under ambient conditions (760 Torr and 296 ± 2 K) using an aerosol flow tube (AFT) coupled with a chemical conversion/laser-induced fluorescence (CC/LIF) technique. γ values determined for dry and wet aerosols of KCl were 0.02 ± 0.01 and 0.07 ± 0.03 at 66% and 75% RH, respectively, while γ values for those doped with CuSO₄ was 0.55 ± 0.19 at 75% RH. γ values determined for synthetic sea-salt particles were 0.07 ± 0.03, 0.12 ± 0.04 and 0.13 ± 0.04 at 35%, 50%, 75% RH, respectively, while γ values for natural seawater particles were 0.10 ± 0.03, 0.11 ± 0.02 and 0.10 ± 0.03 at 35%, 50%, 75% RH, respectively. We recommend a HO₂ uptake coefficient in marine areas of 0.1 for modeling and estimated the contribution of heterogeneous loss of HO₂ by sea-salt aerosol particles in marine areas using a box model. Our box-model simulations suggested that daytime maximum HO₂ concentrations decreased to 87–94% of the values without heterogeneous loss.     

Hydrolysis and heat treatment of aluminum dust.

Aluminum dust is a toxic and hazardous byproduct of Al remelting. The present research was performed to characterize and evaluate its behavior in water. The materials obtained by hydrolysis were also characterized, and the gases generated during the process were qualitatively analyzed. The effects of hydrolysis reaction time and temperature on the dust were also explored. The hydrolysis of Al dust is an exothermic reaction that gave rise to a solid composed of aluminum oxide, silicon oxide, and spinel (MgAl2O4). Most of the CH4, NH3, and SH2 gases generated were emitted immediately upon the start of the reaction, though their production continued for a long time. This slow reaction, which was moderately accelerated by temperature, led to the formation of a material less reactive than the untreated dust. On the other hand, heat treatment of the dust gave rise to an inert material composed of spinel, alumina, and magnesium and aluminum silicates.     

The effect of inorganic and organic chlorine on formation of highly chlorinated organic compounds during incineration: Laboratory pilot study

Aliphatic liquid as a basic fuel was incinerated in a laboratory scale pilot plant. Inorganic chlorine and organic chlorine mixed with basic fuel were used as additive chemicals. Sodium chloride (NaCl) and tetrachloroethylene (C₂Cl₄) were used as the sources of inorganic and organic chlorine. Combustion parameters were adjusted for optimum combustion and, consequently, the amount of particles in flue gases was low. The concentrations of chlorine in flue gases were high enough for possible formation reactions of organic chlorinated compounds in all of the chlorine input tests. An increase in chlorine input did not significantly increase the amounts of highly chlorinated organic compounds, like PCDD/Fs. The main result was that chlorophenol concentrations increased in parallel with organic chlorine input. Comparing organic chlorine to inorganic chlorine tests showed that more highly substituted PCDD/F congeners were formed when organic chlorine was the additive chlorine source. The formation of highly chlorinated organic compounds such as PCDD/Fs requires not only chlorine and aliphatic fuel to be formed, but some catalysts are also needed.     

Water uptake characteristics of individual atmospheric particles having coatings

We used an environmental transmission electron microscope to observe deliquescence and hygroscopic growth of atmospheric particles with hygroscopic coatings over the range 0–100% relative humidity (RH). The particles were collected from polluted and clean environments. Types included a sulfate-coated NaCl/silicate aggregate particle, a sulfate-coated sea-salt particle, and a Mg-rich, chloride-coated sea-salt particle. They all exhibited initial water uptake between 50% and 60% RH, although the first major morphological changes occurred at 70% RH. A deliquescence sphere, adjacent to the core particle, formed between 70% and 76% RH when deliquescence occurred or when the liquid phase was able to break out of the solid exterior coating. The deliquescence sphere grew to engulf the particle with increasing RH. Some particles developed a splatter zone associated with a particle coating. Efflorescence occurred over the range 49–44% RH. Our results indicate that some coated particles undergo a multi-step deliquescence process and that composition of the different phases within the coating affects deliquescence and hygroscopic growth below 76% RH. Above 76% RH, the dominant hygroscopic growth was due to water uptake by NaCl. Efflorescence of these particles also was strongly linked to NaCl, although the presence of other phases inhibited formation of a single NaCl crystal. Our results show that the observed coatings can both enhance particle solubility and lower the effective deliquescence RH of the particle. Thus, these coatings cause important phase and size changes for aerosol particles that could feed back into many other chemical and physical processes that contribute to radiative forcing within the atmosphere.     

Factors influencing aerosol solubility during cloud processes

The water-soluble fraction of an aerosol determines its chemical and physical properties and also its behaviour. The origin of the aerosol and its atmospheric transport influence its solubility. Cloud process simulations have been conducted on both Saharan and anthropogenic aerosols. The rate of solubilisation was followed for native and processed aerosol particles; it is controlled by the pH variations due to release of acids or bases. It appears that one condensation/evaporation cycle increases the solubility of aerosol particles. Increasing the number of cloud process simulations does not affect the solubility profile. The solubility depends only on the conditions of the last cloud cycle and, in particular, on the factor controlling pH during this process.     

Assessment of the photochemistry of OH and NO3 on Jeju Island during the Asian-dust-storm period in the spring of 2001

In this study, we examined the influence of the long-range transport of dust particles and air pollutants on the photochemistry of OH and NO3 on Jeju Island, Korea (33.17 degrees N, 126.10 degrees E) during the Asian-dust-storm (ADS) period of April 2001. Three ADS events were observed during the periods of April 10-12, 13-14, and 25-26. Average concentration levels of daytime OH and nighttime NO3 on Jeju Island during the ADS period were estimated to be about 1x10(6) and 2x10(8) moleculescm(-3) ( approximately 9 pptv), respectively. OH levels during the ADS period were lower than those during the non-Asian-dust-storm (NADS) period by a factor of 1.5. This was likely to result from higher CO levels and the significant loading of dust particles, reducing the photolysis frequencies of ozone. Decreases in NO3 levels during the ADS period was likely to be determined mainly by the enhancement of the N2O5 heterogeneous reaction on dust aerosol surfaces. Averaged over 24 h, the reaction between HO2 and NO was the most important source of OH during the study period, followed by ozone photolysis, which contributed more than 95% of the total source. The reactions with CO, NO2, and non-methane hydrocarbons (NMHCs) during the study period were major sinks for OH. The reaction of N2O5 on aerosol surfaces was a more important sink for nighttime NO3 during the ADS due to the significant loading of dust particles. The reaction of NO3 with NMHCs and the gas-phase reaction of N2O5 with water vapor were both significant loss mechanisms during the study period, especially during the NADS. However, dry deposition of these oxidized nitrogen species and a heterogeneous reaction of NO3 were of no importance.     

Optical and chemical properties of marine boundary-layer aerosol around Japan determined from shipboard measurements in 2002

Shipboard measurements of the optical and chemical properties of marine boundary-layer aerosol were made around Japan over the period from 28 August to 25 September 2002. Measurements were conducted aboard the Research Vessel (R/V) Shirase along cruise tracks beginning from Yokosuka, and proceeding on to Hakodate, Sakata, Sasebo, Naha, Kure, and Yokkaichi. This paper describes the results of optical measurements using an Optical Particle Counter (OPC), an Integrating Nephelometer (IN), and a Particle Soot/Absorption Photometer (PSAP), as well as chemical analyses of water-soluble aerosol particles collected by impactor and filter systems. Coulter Multisizer measurements were used for water-insoluble aerosol particles. The complex refractive index (CRI), scattering and absorption coefficients, and size distribution of aerosols were estimated from combined measurements made using OPC, IN, and PSAP. Contrasting aerosol characteristics were observed during different stages of the cruise. Discussion on these differences focuses mainly on two legs: Leg-1 from Yokosuka to Hakodate and Leg-4 from Sasebo to Naha. Backward trajectory analyses indicate that the air sampled during Leg-1 originated from the Pacific Ocean, whereas the air sampled during Leg-4 originated from the Chinese Continent via the Korean Peninsula. For the first half of Leg-1, the number concentration was low and larger particles were relatively predominant. The real and imaginary parts of the CRI were estimated to be 1.38–1.40 and close to zero, respectively. This estimation is consistent with the results of chemical analyses, which show that the sea salt is rich in aerosols sourced from remote ocean areas. In contrast, small particles were predominant during Leg-4, and the real and imaginary parts of the CRI were estimated to be 1.52–1.59 and approximately −0.002, respectively. These findings are also consistent with chemical analyses that reveal a mixture of mineral dust and sulfate aerosol likely transported from China and Korea. The Coulter Multisizer measurements conducted during Leg-4 reveal abundant water-insoluble particles with a mode radius of 1.35 μm.     

A case study of optical and chemical ground apportionment for urban aerosols in Thessaloniki

Urban aerosol characterization gathering ground-based in situ and sunphotometer measurements have been performed for the city of Thessaloniki for two specific days: the 12th and 13th of June 1997. A representative aerosol model for Thessaloniki aerosols was tentatively constructed for each day. Four components have been selected from our chemical measurements: black carbon (BC), particulate organic matter (POM), inorganic fine water soluble particles (WS) and a residue coarse component which mainly contains coarse dust and sea-salt particles (CC). Size distribution and complex refractive index for (WS) and (CC) components were determined from published data. (CC) has been shown to have a small optical effect compared to the submicron components. Size distribution for carbonaceous particles was obtained from sensitivity tests on particulate number and visible Angström exponent. The impact of relative humidity on extinction and scattering coefficients has been calculated on 13 June with Mie theory and Hänel relationships. Parameters needed for this calculation were well known for WS particles only. For POM particles we have used the experimental curve of hygroscopic factors obtained by Hobbs et al. (1997) for urban aerosols sampled on the East coast of United States to determine the hydrophilic dependency of POM particles. Relative humidity has been shown to be an important parameter even for values lower than 50%. Optical apportionment calculation has been realized pointing out that more than 45% of the total extinction coefficient is due to (POM) particles and about 20 and 30% to (WS) and (BC), respectively.