The chemical composition of rainwater over Büyükçekmece Lake, Istanbul

In the present study, the precipitation near Büyükçekmece Lake, which is one of the important drinking water sources of Istanbul city, was studied during October 2001–July 2002. Seventy-nine bulk precipitation samples were collected at two sampling stations near the Lake (41°2′35″N, 28°35′25″E and 41°5′30″N, 28°37′7″E). The study comprised the determination of H⁺, Cl⁻, NO₃⁻, SO₄²⁻, NH₄⁺, Na, K, Mg, Ca, Al, Ba, Fe, Cu and Mn concentrations in bulk deposition rain event samples. The average volume-weighted pH value was found to be 4.81, which points out that the rain is slightly acidic. High sulfate concentrations were observed together with high H⁺ ion values. Sulfur emissions were the major cause for the observed high hydrogen ion levels. On the basis of factor analysis and correlation matrix analysis, it has been found that in this region, acid neutralization is brought about by calcium rather than the ammonium ion. The varimax rotated factor analysis grouped the variables into four factors, which are crustal, marine and two anthropogenic sources.     

Chemical and strontium isotope characterization of rainwater at an urban site in Loess Plateau, Northwest China

Major ion concentrations and strontium isotopic ratios (⁸⁷Sr/⁸⁶Sr) were measured in rainwater samples collected at the urban site of Lanzhou, a city located on the Loess Plateau in the arid and semi-arid areas of northwest China. The rainwater samples possessed alkaline pH, at a reference level of 5.6, with a range of 6.82 to 8.28 and a volume-weighted mean (VWM) pH value of 7.70. The alkaline character of rainwater in Lanzhou is due to the result of neutralization caused by the alkaline soil dusts which contain large amount of CaCO₃. It was observed that Ca²⁺ was the most abundant cation with a VWM value of 886 µeq l^− 1 (115–2184 µeq l^− 1), accounting for 87.8% of the total cations. Without considering HCO₃⁻, SO₄²⁻ and NO₃⁻ were dominant among the anions, accounting for 64.2% and 23.0%, respectively, of the total measured anions. Using Na as an indicator of marine origin and Al for terrestrial inputs, the proportions of sea salt and non-sea-salt elements were estimated from elemental ratios. The precipitation in this region has typical continental characteristics. The Sr concentrations varied from 0.004 to 0.885 µmol l^− 1, and strontium isotopic ratios (⁸⁷Sr/⁸⁶Sr) lay in the range of 0.71025–0.71302, with an average of 0.71143. The ⁸⁷Sr/⁸⁶Sr ratios of Lanzhou rainwater are higher than that of seawater, which reflects contributions from the radiogenic Sr sources of the aerosols. The most suitable candidate for the source would be the soil dust originating from local and distant loess and desert areas. The ⁸⁷Sr/⁸⁶Sr ratios were used to characterize different sources of base cations in rainwater, suggesting that the samples could be interpreted in terms of combinations of at least three components: soil dust derived from the Loess Plateau and desert areas in northwest China (with ⁸⁷Sr/⁸⁶Sr ~ 0.7130), seawater (with ⁸⁷Sr/⁸⁶Sr ~ 0.70917), and anthropogenic inputs (with ⁸⁷Sr/⁸⁶Sr ~ 0.7103). The high ⁸⁷Sr/⁸⁶Sr ratio and Ca and Sr content in the rainwater from Lanzhou can be attributed to the dissolution of calcium carbonate in soil dust.     

Changes of cloud water chemical composition in the Western Sudety Mountains, Poland

The changing chemical composition of cloud water and precipitation in the Western Sudety Mountains are discussed against the background of air-pollution changes in the Black Triangle since the 1980s until September 2004. A marked reduction of sulphur dioxide emissions between the early 1990's and the present (from almost 2 million tons to around 0.2 million tons) has been observed, with a substantial decline of sulphate and hydrogen concentration in cloud water (SO₄²⁻ from more than 200 to around 70 μmol l^− 1; H⁺ from 150 to 50 μmol l^− 1) and precipitation (SO₄²⁻ from around 80 to 20–30 μmol l^− 1; H⁺ from around 60 to 10–15 μmol l^− 1) samples. At some sites, where fog/cloud becomes the major source of pollutants, deposition hot spots are still observed where, for example, nitrogen deposition can exceed 20 times the relevant critical load. The results show that monitoring of cloud water chemistry can be a sensitive indicator of pollutant emissions.     

Atmospheric deposition of nitrogen, sulfur and chloride in Thessaloniki, Greece

In the present study, the wet and dry depositions of particulate NO₃⁻, SO₄²⁻, Cl⁻ and NH₄⁺ were measured using a wet/dry sampler as a surrogate surface. Gas phase compounds of nitrogen, sulfur and chloride (HNO₃, NH₃, SO₂ and HCl) were measured by an annular denuder system (ADS) equipped with a back up filter for the collection of particles with diameter ≤ 5 μm. Ambient concentrations of NO, NO₂ and SO₂ were also taken into consideration. Sampling was conducted at an urban site in the center of the city of Thessaloniki, northern Greece. The presence of the aerosol species was examined by cold/warm period and the possible compounds in dry deposits were also considered. Dry deposition fluxes were found to be well correlated with ambient particle concentrations in order to be used for the calculation of particle deposition velocity. Average particulate deposition velocities calculated were 0.36, 0.20, 0.20 and 0.10 cm s^− 1 for Cl⁻, NO₃⁻, SO₄²⁻ and NH₄⁺, respectively. Total dry deposition fluxes (gas and particles) were estimated at 3.24 kg ha^− 1 year^− 1 for chloride (HCl + p-Cl), 9.97 kg ha^− 1 year^− 1 for nitrogen oxidized (NO + NO₂ + HNO₃ + p-NO₃), 5.32 kg ha^− 1 year^− 1 for nitrogen reduced (NH₃ + p-NH₄) and 15.77 kg ha^− 1 year^− 1 for sulfur (SO₂ + p-SO₄). 70–90% total dry deposition was due to gaseous species deposition. The contribution of dry deposition to the total (wet + dry) was at the level of 60–70% for sulfur and nitrogen (oxidized and reduced), whereas dry chloride deposition contributed 35% to the total. The dry-to-wet deposition ratio of all the studied species was found to be significantly associated with the precipitation amount, with nitrogen species being better and higher correlated. Wet, dry and total depositions measured in Thessaloniki, were compared with other countries of Europe, US and Asia.     

Resources of the ionized atmosphere as an aerosol source

The potential resources on the ion-stimulated syntheses effects of aerosol particles of lower troposphere in test sites in the arctic, mountain, arid and forest areas as the function of irradiation time and gas-precursor concentration were experimentally and theoretically evaluated. The dust-free outdoor air was irradiated with an ionization current of 10^− 6 A by α-rays from isotope ²³⁹Pu. The total output of radiolytic aerosols (RA) with a diameter of 3–1000 nm was found to be 0.05–0.1 molecules per 1 eV of absorbed radiation, while the physical upper limit is 0.25–0.4 molecules/eV. In an interval of exposition time from 6 to 800 s (adsorbed energy is 3 · 10¹²–10¹⁴ eV/cm³) the RA mass concentration at different sites was increased from 1–10 to 50–500 μg/m³. According to the liquid chromatography data the major RA material is the H₂O/HNO₃ solution with acid concentration  25%. The used physical model presents new aerosols as a product from small and intermediate ion association through formation of neutral clusters and describes adequately some of the peculiarities in field experiment data. Introducing SO₂, NH₃, and also hydrochloric, nitric and sulphuric acid vapours with concentration 0.1–1 mg/m³ in the irradiated air stimulated an increase of mass aerosol concentration by a factor of 8–30. The mean size also decreased by a factor of 3–5. These facts allowed us to expect that the chemical composition of radiolytic aerosols generated in outdoor air would noticeably differ after addition of the gas-precursors.     

Wet deposition of precipitation chemistry during 2005–2009 at a remote site (Nam Co Station) in central Tibetan Plateau

Chemical compositions of precipitation samples collected from a remote and high elevation site (Nam Co Station, 30°46.44??N, 90°59.31??E, 4730?m?a.s.l.) in central Tibetan Plateau (TP, hereafter) from August 2005 to August 2009 are investigated. During the study period, Ca²⁺ and HCO ₃ ^- have the highest concentrations among ions and are the dominant cation and anion in precipitation, taking 27.46?% and 30.84?% to the total ions respectively. Empirical Orthogonal Functions (EOFs) analyses reveal that crustal aerosol inputs significantly contributed to the loading of Ca²⁺, Mg²⁺, SO ₄ ^2- and HCO ₃ ^- in precipitation, while lake salt plays a major source of K⁺ and Cl^-. Seasonal variations of ionic wet deposition fluxes show high values during monsoon seasons due to large precipitation amount. Among the cations, annual Ca²⁺ flux is the largest (86.26?eq hm^?2), Na⁺ and NH ₄ ⁺ fluxes are following. Among anions, HCO ₃ ^- has the highest flux (98.66?eq hm^?2) while that of NO ₃ ^- is the lowest. Annual wet deposition of nitrogen has varied considerably with the average value of 0.70?kg?ha^?1 a^?1 at Nam Co Station. About 80?% of total nitrogen flux occurs during the monsoon seasons when precipitation is concentrated, in which NH ₄ ⁺ and NO ₃ ^- contributed to 61?% and 39?% of the total nitrogen deposition. Thus, our ionic concentrations and wet deposition fluxes in precipitation can provide a useful dataset to assess atmospheric environment and its impacts on ecosystem in the inland TP.     

One year measurements of aerosol optical properties over an urban coastal site: Effect on local direct radiative forcing

We present results of direct aerosol radiative forcing over a French Mediterranean coastal zone based on one year of continuous observations of aerosol optical properties during 2005–2006. Monthly-mean aerosol optical depth at 440 nm ranged between 0.1 and 0.34, with high Angstrom coefficient (α > 1.2). The single scattering albedo (at 525 nm) estimated at the surface ranged between 0.7 and 0.8, indicating significant absorption. The presence of aerosols over the Mediterranean zone during summer decreases the shortwave radiation reaching the surface by as much as 26 ± 3.9 W m^− 2, and increases the top of the atmosphere reflected radiation by as much as 5.2 ± 1.0 W m^− 2. The shortwave atmospheric absorption translates to an atmospheric heating of 2.5 to 4.6 K day^− 1. Concerted efforts are needed for investigating the possible impact of the increase in heating rate on the maintenance of heat-waves frequently occurring over this coastal region during summer time.     

Geochemistry of regional background aerosols in the Western Mediterranean

The chemical composition of regional background aerosols, and the time variability and sources in the Western Mediterranean are interpreted in this study. To this end 2002–2007 PM speciation data from an European Supersite for Atmospheric Aerosol Research (Montseny, MSY, located 40 km NNE of Barcelona in NE Spain) were evaluated, with these data being considered representative of regional background aerosols in the Western Mediterranean Basin. The mean PM₁₀, PM_2.5 and PM₁ levels at MSY during 2002–2007 were 16, 14 and 11 µg/m³, respectively. After compiling data on regional background PM speciation from Europe to compare our data, it is evidenced that the Western Mediterranean aerosol is characterised by higher concentrations of crustal material but lower levels of OM + EC and ammonium nitrate than at central European sites. Relatively high PM_2.5 concentrations due to the transport of anthropogenic aerosols (mostly carbonaceous and sulphate) from populated coastal areas were recorded, especially during winter anticyclonic episodes and summer midday PM highs (the latter associated with the transport of the breeze and the expansion of the mixing layer). Source apportionment analyses indicated that the major contributors to PM_2.5 and PM₁₀ were secondary sulphate, secondary nitrate and crustal material, whereas the higher load of the anthropogenic component in PM_2.5 reflects the influence of regional (traffic and industrial) emissions. Levels of mineral, sulphate, sea spray and carbonaceous aerosols were higher in summer, whereas nitrate levels and Cl/Na were higher in winter. A considerably high OC/EC ratio (14 in summer, 10 in winter) was detected, which could be due to a combination of high biogenic emissions of secondary organic aerosol, SOA precursors, ozone levels and insolation, and intensive recirculation of aged air masses. Compared with more locally derived crustal geological dusts, African dust intrusions introduce relatively quartz-poor but clay mineral-rich silicate PM, with more kaolinitic clays from central North Africa in summer, and more smectitic clays from NW Africa in spring.     

Numerical simulation of the relationship between electrification and microphysics in the prelightning stage of thunderstorms

To further investigate the influence of cloud base temperature, updraft velocity and precipitation particle constitution on cloud electrification, five thunderstorms in various regions of China were simulated by using the three-dimensional compressible hailstorm numerical model including inductive and non-inductive charging mechanisms. The results indicate that changes of cloud base temperature have an influence on the initial electrification. Comparison of the above cases shows that in the case of warm cloud base and moderate updraft velocity (< 20 m s^{−  1}), active electrification occurred below the − 10 °C level before moving upward to the − 20 °C level. In contrast, when cloud base is cold and updraft velocity is intensive, the main charging region is at the − 20 °C or even higher level. In that case, the vertical extent of the main negative charge region becomes larger with the increase of cloud base temperature. Apart from the main dipolar or tripolar charge structure, some smaller charge regions with relatively high values of charge density may also appear. Frozen drops, originating mainly from supercooled raindrops, mainly get electrified through charging interactions with snow at or below the − 20 °C level. They are responsible for the negative charge region near the melting level at the initial stage of precipitation if there is a large supercooled raindrop content. Non-inductive charging during hail-snow collisions is rather weak, resulting in the charge density on hail of no more than − 0.01 nC m^− 3.     

Trends in chemical composition of precipitation in Nanjing, China, during 1992–2003

In this study, variations of the chemical composition of precipitation in Nanjing, China, over a 12-year period (1992–2003) are presented. The average annual concentration of pH value was 5.15, ranging from 4.93 to 5.36, and there was no significant trend in the acidity of precipitation. SO₄²⁻, Cl⁻ and NO₃⁻ were the main anions, while Ca²⁺, NH₄⁺ and Mg²⁺ were the main cations. The concentrations of these main ions were very high compared to those reported in many other areas around the world. Most of the ions came from anthropogenic and crustal sources. High correlations were found among dust-derived cations Ca²⁺, Mg²⁺and K⁺, between Cl⁻ and SO₄²⁻, between Cl⁻ and NH₄⁺ and between acidic anions and dust-derived cations, such as SO₄²⁻ and Ca²⁺, SO₄²⁻ and K⁺, Cl⁻ and Ca²⁺, Cl⁻ and K⁺, F⁻ and Mg²⁺ and F⁻ and K⁺. A significant decreasing trend was observed in concentration of SO₄²⁻ because of the abatement strategies for SO₂ emissions and energy policy change, while a significant increasing trend was found in the contribution of NO₃⁻ to acidification due to the rapidly growing number of motor vehicles. A significant decreasing trend was found in dust-derived cation Ca²⁺ due to more stringent controls of industrial dust emissions and rapid urbanization reducing the amount of open land, while the contribution of NH₄⁺ to neutralization increased relatively.     

Size-resolved aerosol chemical concentrations at rural and urban sites in Central California, USA

Aerosol size distributions were measured with Micro Orifice Uniform Deposit Impactor (MOUDI) cascade impactors at the rural Angiola and urban Fresno Supersites in California's San Joaquin Valley during the California Regional PM₁₀/PM_2.5 Air Quality Study (CRPAQS) winter campaign from December 15, 2000 to February 3, 2001. PM_2.5 filter samples were collected concurrently at both sites with Sequential Filter Samplers (SFS). MOUDI nitrate (NO₃⁻) concentrations reached 66 μg/m³ on January 6, 2001 during the 1000–1600 PST (GMT-8) period. Pair-wise comparisons between PM_2.5 MOUDI and SFS concentrations revealed high correlations at the Angiola site (r > 0.93) but more variability (r < 0.85) at the Fresno site for NO₃⁻, sulfate (SO₄⁼), and ammonium (NH₄⁺). Correlations were higher at Fresno (r > 0.87) than at Angiola (r < 0.7) for organic carbon (OC), elemental carbon (EC), and total carbon (TC). NO₃⁻ and SO₄⁼ size distributions in Fresno were multi-modal and wider than the uni-modal distributions observed at Angiola. Geometric mean diameters (GMD) were smaller for OC and EC than for NO₃⁻ and SO₄⁼ at both sites. OC and EC were more concentrated on the lowest MOUDI stage (0.056 µm) at Angiola than at Fresno. The NO₃⁻ GMD increased from 0.97 to 1.02 µm as the NO₃⁻ concentration at Angiola increased from 43 to 66 µg m^− 3 during a PM_2.5 episode from January 4–7, 2001. There was a direct relationship between GMD and NO₃⁻ and SO₄⁼ concentrations at Angiola but no such relationships for OC or EC. This demonstrates that secondary aerosol formation increases both concentration and particle size for the rural California environment.     

Ship measurements of submicron aerosol size distributions over the Yellow Sea and the East China Sea

During the spring of 2005, the total particle concentrations and the submicron aerosol size distributions were measured on board the research vessel over the south sea of Korea and the Korean sector of the Yellow Sea. Similar measurements were made over the East China Sea in autumn 2005. The aerosol properties varied dynamically according to the meteorological conditions, the proximity to the land masses and the air mass back trajectories. The average total particle concentration was the lowest over the East China Sea, 4335 ± 2736 cm^− 3, but the instantaneous minimum, 837 cm^− 3, for the entire ship measurement was recorded during the Yellow Sea cruise. There was also a long (more than 6 h) stretch of low total particle concentrations that fell as low as 1025 cm^− 3 during the East China Sea cruise when the ship was the farthest from the shores and the air mass back trajectories resided long hours over the sea. These observations lead to the suggestion of ~ 1000 cm^− 3 as the background total particle concentration over the marine boundary layer in the studied region of the Yellow Sea and the East China Sea, implying significant anthropogenic influence even for the background value. In the mean time, average aerosol size distributions were unimodal and the mode diameter ranged between 52 and 86 nm, excluding the fog periods, which suggests that the aerosols measured in this study experienced relatively less aging processes within the marine boundary layer.     

Polycyclic aromatic hydrocarbons, polychlorinated biphenyls and organochlorine pesticides in urban air of Konya, Turkey

Polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) were determined in urban air samples of Konya, Turkey between August 2006 and May 2007. The concentrations of pollutants in both the gas and particulate phase were separately analysed. The average total (gas + particulate) concentrations of PAHs, PCBs and OCPs were determined as 206 ng m^− 3, 0.106 ng m^− 3, 4.78 ng m^− 3 respectively. All of the investigated target compounds were dominantly found in the gas phase except OCPs. Higher air concentrations of PAHs were found at winter season while the highest concentrations of PCBs were determined in September. The highest OCPs were detected in October and in March. In urban air of Konya, PCB 28 and PCB 52 congeners represent 46% and 35% of total PCBs while Phenanthrene, Fluoranthene, Pyrene accounted for 29%, 13%, 10% of total PAHs. HCH compounds (α + β + γ + δ-HCH), total DDTs (p,p′-DDE, p,p′-DDD, p,p′-DDT), Endosulfan compounds (Endosulfan I, Endosulfan II, Endosulfan sulfate) were dominantly determined as 30%, 21%, 20% of total OCPs respectively. Considering the relation between these compounds with temperature, there was no significant correlation observed. Despite banned/restricted use in Turkey, some OCPs were determined in urban air. These results demonstrated that they are either illegally being used in the course of agricultural activity and gardens in Konya or they are residues of past use in environment. According to these results, it can be suggested that Konya is an actively contributing region to persistent organic pollutants in Turkey.     

Black carbon relationships with emissions and meteorology in Xi'an, China

Aerosol black carbon (BC) was measured every 5 min at Xi'an, China from September 2003 to August 2005. Daily BC concentrations ranged from 2 to 65 μg m^− 3, averaging 14.7 ± 9.5 μg m^− 3 and displayed clear summer minima and winter maxima. BC typically peaked between 0800 and 1000 LST and again between 2000 and 2200 LST, corresponding with morning and evening traffic combined with nighttime residential cooking and heating. The nocturnal peak was especially evident in winter, when more domestic heating is used and pollutant-trapping surface-inversions form earlier than in summer. BC frequency distributions the most commonly occurring concentrations occurred between 5 and 10 μg m^− 3 in all four seasons. BC ranged from 1.6% and 15.6%, and averaged 8.3% of PM_2.5. A clear inverse relationship between BC and wind speed (WS) was found when WS was below 2.5 to 3.0 m s^− 1, implying a local origin for BC. Mixed layer depths (MLDs) were shallower during BC episodes compared to cleaner conditions.     

Statistical analysis of microphysical properties and the parameterization of effective radius of warm clouds in Beijing area

In this paper warm cloud microphysical parameters including cloud droplet number concentration (N_c), liquid water content (q_l) and effective radius (r_e) from 75 flights around the Beijing area during 2005 and 2006 are summarized. Average N_c (cm^− 3) for Cu, Sc, Ac, As and Ns are 376 ± 290, 257 ± 226, 147 ± 112, 60 ± 35 and 60 ± 84, respectively. Many records of high N_c above 1000 cm^− 3 are observed. The large standard deviations indicate a large variation of N_c and q_l in this region. The maxima of q_l reach 1.4 g m^− 3 in Cu and 1.0 g m^− 3 in Sc, respectively. Different parameterizations of effective radius are examined with the in-situ data in this area. There are different ways to obtain the prefactor representing the relationship between effective radius and mean volume radius. Significant systematic errors are found to be at the large sizes when the prefactor is expressed with relative dispersion under the Gamma Distribution. Fixed prefactor of 1, which was widely used, even produces much larger error. A prefactor of 1.22 is found to be better than the former two methods by fitting with the observed data. The effective radius is further parameterized as functions of mean volume radius, liquid water content and cloud droplet number concentration. We suggest that the effective radius can be parameterized as r_e,p ≈ 1.20r_v + 0.22–1.28/r_v², which is a practical and more accurate scheme without too much computation complexity.     

Asian Dust effects on Total Suspended Particulate (TSP) compositions at Gosan in Jeju Island, Korea

The compositions of TSP between AD and NAD storm periods were compared to study their long-term variations and chemical characteristics. TSP samples were collected at Gosan site in Jeju Island of Korea from February to May of 1992–2004. The major ionic and elemental species of TSP aerosols were analyzed. During AD periods, the concentrations of crust components (nss-Ca²⁺, Al, Fe, Ca, Mg, Ba, Sr, Ti) increased remarkably, and the concentrations of anthropogenic components (nss-SO₄²⁻, NO₃⁻, S, Zn, Pb, Cr, Ni, Cd), with the exception of NH₄⁺, increased weakly. The concentration ratios of all major components between AD and NAD periods showed ranges from 1.2 to 8.5, except for NH₄⁺. The slope of the linear regression indicated that the contribution of CO₃²⁻ may have comprised up to 17% of the total anions. Our results suggested that the AD storm greatly influenced TSP compositions. Linear regression analyses indicated that NH₄⁺ was not correlated with NO₃⁻, but highly correlated with nss-SO₄²⁻ during both periods. The nss-SO₄²⁻ was also correlated with NH₄⁺, K⁺, nss-Mg²⁺, and nss-Ca²⁺ during both periods. Interestingly, NO₃⁻ was associated with nss-Ca²⁺ and nss-Mg²⁺ during AD periods. Of the metal elements, Fe, Ca, Mg, Ti, Mn, Ba, Sr, V, and Co were highly correlated with Al during both periods, signifying that these metals were mostly originated from soils.     

An Investigation into the Ionic Chemical Composition and Mixing State of Biomass Burning Particles Recorded During TRACE-P P3B Flight#10

In this study bulk airborne aerosol composition measured by the PILS-IC (integration time of 3 min 24 s) during TRACE-P P3B Flight 10 are used to investigate the ionic chemical composition and mixing state of biomass burning particles. A biomass burning plume, roughly 3–4 days old, moderately influenced by urban pollution aerosols recorded in the Philippine Sea is investigated. Focusing on the fine particle NO₃⁻, SO₄²⁻, K⁺, NH₄⁺, and water-soluble organics, the observed correlations and nearly 1-to-1 molar ratios between K⁺ and NO₃⁻ and between NH₄⁺ and (SO₄²⁻+ inferred Organics) suggest the presence of fine-mode KNO₃, (NH₄)₂SO₄, and NH₄(Organics) aerosols. Under the assumption that these ion pairs existed, and because KNO₃ is thermodynamically less favored than K₂SO₄ in a mixture of NO₃⁻, SO₄²⁻, K⁺, NH₄⁺, and Organic anions, the measurements suggest that aerosols could be composed of biomass burning particles (KNO₃) mixed to a large degree externally with the (NH₄)₂SO₄ aerosols. A “closed-mode” thermodynamic aerosol simulation predicts that a degree of external mixing (by SO₄²⁻ mass) of 60 to 100% is necessary to achieve the observed ionic associations in terms of the existence of KNO₃. However, the degree of external mixing is most likely larger than 90%, based on both the presence of KNO₃ and the amounts of NH₄NO₃. Calculations are also shown that the aerosol mixing state significantly impacts particle growth by water condensation/evaporation. In the case of P3B Flight #10, the internal mixture is generally more hygroscopic than the external mixture. This method for estimating particle mixing state from bulk aerosol data is less definitive than single particle analysis, but because the data are quantitative, it may provide a complementary method to single particle chemical analysis.     

Deposition of atmospheric particulate PCBs in suburban site of Turkey

Dry deposition and air concentration samples were collected from July 2004 to May 2005 at a suburban site in Turkey. A water surface sampler (WSS) was used to measure directly the dry deposition flux of particulate polychlorinated biphenyls (PCBs) while a high volume air sampler (HVAS) was employed to collect air samples. Particulate PCB concentrations accounted for 15% of total PCBs (gas + particle phase) at the site. The overall particulate phase PCB flux ranged from 2 to 160 ng m^− 2 d^− 1 with an average of 46.3 ± 40.6 ng m^− 2 d^− 1. Forty one PCB congeners were targeted in the samples while twenty one congeners were found to be higher than detection limits in deposition samples. Fluxes for homolog groups ranged between 0.9 (7-CBs) and 21.0 (3-CBs) ng m^− 2 d^− 1. Measured dry deposition fluxes were lower than the ones usually reported for urban sites. Average PCB dry deposition velocity, calculated using flux values and concurrently measured atmospheric concentrations, was 1.26 ± 1.86 cm s^− 1 depended on size distribution of particles, atmospheric PCB concentrations and meteorological conditions.     

Sulfate-coated dust particles in the free troposphere over Japan

Airborne aerosol collections were performed over Wakasa bay (36°00′N, 135°30′E) in March and Kumano open sea (34°00′N, 136°50′E) and Seto (35°10′N, 137°10′E) in July 2001 at altitudes between 1.0 and 5.8 km. The particles were individually analyzed using transmission electron microscopy (TEM). Relatively large mineral-dust (mostly clay) particles were abundant in the March samples. They also dominated in July in the mid-troposphere higher than 4 km altitude, whereas sea salt and ammonium sulfate were more abundant at lower altitudes. Ca-coated grid samples show many traces of aqueous sulfate droplets. The proportions of former sulfate droplets to the total collected particles apparently increased with increasing relative humidity at the time of sampling. TEM analysis revealed that a significant fraction of these former droplets enclose mineral-dust particles as well as sea salt, soot, and fly ash. Some enclose mixtures of mineral-dust, sea-salt, soot, and fly ash particles. The results provide evidence that mineral dust from the Asian continent could acquire coatings of sulfate while being transported in the free troposphere. The mineral-dust particles probably acquired the sulfate coatings either through heterogeneous uptake of gaseous SO₂ and subsequent oxidation or through coagulation with cloud or fog droplets. The presence of the mixed particles in sulfate droplets also indicates that aggregation of particles of different origins occurred through cloud processing. Such sulfate-coated dust particles would affect cloud formation, precipitation, and chemistry of the free troposphere.     

Condensed water in tropical cyclone “Oliver”, 8 February 1993

On February 8, 1993, the NASA DC-8 aircraft profiled from 10,000 to 37,000 feet (3.1–11.3 km) pressure altitude in a stratified section of tropical cyclone “Oliver” over the Coral Sea northeast of Australia. Size, shape and phase of cloud and precipitation particles were measured with a 2-D Greyscale probe. Cloud/ precipitation particles changed from liquid to ice as soon as the freezing level was reached near 17,000 feet (5.2 km) pressure altitude. The cloud was completely glaciated at −5°C. There was no correlation between ice particle habit and ambient temperature. In the liquid phase, the precipitation-cloud drop concentration was 4.0 × 10³ m⁻³, the geometric mean diameter D_g=0.5−0.7 mm, and the liquid water content 0.7−1.9 g m⁻³. The largest particles anywhere in the cloud, dominated by fused dendrites at concentrations similar to that of raindrops (2.5 × 10³ m⁻³) but a higher condensed water content (5.4 g m⁻³ estimated) were found in the mixed phase; condensed water is removed very effectively from the mixed layer due to high settling velocities of the large mixed particles. The highest number concentration (4.9 × 10⁴ m⁻³), smallest size (D_g=0.3−0.4 mm), largest surface area (up to 2.6 × 10² cm² m⁻³ at 0.4−1.0 g m⁻³ of condensate) existed in the ice phase at the coldest temperature (−40°C) at 35,000 feet (10.7 km). Each cloud contained aerosol (haze particles) in addition to cloud particles. The aerosol total surface area exceeded that of the cirrus particles at the coldest temperature. Thus, aerosols must play a significant role in the upscattering of solar radiation. Light extinction (6.2 km⁻¹) and backscatter (0.8 sr⁻¹ km⁻¹) was highest in the coldest portion of the cirrus cloud at the highest altitude.