Effects of seed particle size and composition on heterogeneous nucleation of n-nonane

Heterogeneous nucleation of supersaturated n-nonane vapour on seed particles of different size and composition has been investigated using a fast expansion chamber. Monodisperse seed particle sizes were ranging from about 4 nm up to about 24 nm in diameter. By using different types of particle generators WO_x, Ag and (NH₄)₂SO₄ particles were generated. For direct comparison between different particle compositions overlapping sizes have been generated for WO_x and Ag at about 7 nm particle diameter as well as for Ag and (NH₄)₂SO₄ at about 15 nm. Nucleation temperature was kept constant at about 278 K. Experimental data were compared to Kelvin equation and Fletcher theory including the effect of line tension. It was found that heterogeneous nucleation of n-nonane seems to be independent of seed particle composition and starts well below the Kelvin curve. Good agreement was achieved with Fletcher theory including the effect of line tension.     

Condensation particle counting below 2 nm seed particle diameter and the transition from heterogeneous to homogeneous nucleation

Particle detection by condensation particle counters (CPCs) is ultimately limited by the onset of homogeneous nucleation. At vapour supersaturations around the homogeneous nucleation limit the diameter of critical clusters is typically about 2 nm. It is widely assumed that only particles larger than critical clusters can be activated by vapour condensation and the general detection limit of CPCs is therefore currently accepted to be around 2 nm particle diameter. Using an expansion type CPC with n-propanol as working fluid we investigated the transition from heterogeneous to homogeneous nucleation, clearly showing that particles are activated much before the onset of homogeneous nucleation, even at particle diameters as small as 1.4 nm. For particle diameters below 2 nm we have usually found condensation particle counting to be influenced by the simultaneous presence of ions as generated in a bipolar diffusion charger. In this paper we illustrate how the presence of ions influences particle number concentration measurement and how ions can be removed in order to obtain accurate seed particle number concentrations for particle diameters down to 1 nm.     

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.     

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.     

Mass spectrometric study of aged benzene secondary organic aerosol in the presence of dry ammonium sulfate

Inorganic seed particles have relatively large surface area, and play an important role in the formation and aging of secondary organic aerosol (SOA). The effects of dry (NH₄)₂SO₄ which is the most commonly found in urban atmosphere on the aged benzene SOA were qualitatively studied utilizing aerosol laser time-of-flight mass spectrometer (ALTOFMS) coupled with Fuzzy C-Means (FCM) clustering algorithm in this study. Experimental results indicated that nitrophenol, oxocarboxylic acid, epoxide products are the predominant components in the aged benzene SOA in the presence of low concentration (about 10 μg m^?3) of dry (NH₄)₂SO₄. These aged products are the same as the previously obtained aged benzene SOA without (NH₄)₂SO₄ seed aerosol, indicating that low concentration of dry (NH₄)₂SO₄ acts just as the nucleation or condensation center of the SOA, and do not affect the chemical composition of SOA. However, 1 H-imidazole, 1 H-imidazole-2-carbaldehyde, hydrated 1 H-imidazole-2-carbaldehyde, 2,2′-biimidazole, hydrated N-glyoxal substituted 1 H-imidazole, N-glyoxal substituted hydrated 1 H-imidazole-2- carbaldehyde, hydrated mono glyoxal substituted hydrated 1 H-imidazole-2-carboxaldehyde, mono glyoxal substituted 2,2-biimidazole and hydrated glyoxal dimer substituted imidazole which are formed from ammonium ion reaction with glyoxal are the major particulate products in the aged benzene SOA in the presence of high concentration (about 100 μg m^?3) of dry (NH₄)₂SO₄. The retention of water on the dry (NH₄)₂SO₄ particles creates ammonium ion, which can promote the formation of high-molecular-weight (HMW) products through multiphase reactions such as hydration and polymerization of aldehydes form from OH-initiated oxidation of benzene.     

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.     

Effects of inorganic seed aerosols on the growth and chemical composition of secondary organic aerosol formed from OH-initiated oxidation of toluene

(NH₄)₂SO₄, CaCl₂, Na₂SiO₃ and NaNO₃ were selected as surrogates of inorganic seed aerosols of ambient atmosphere of Chinese urban areas, respectively, to study their effects on the formation of secondary organic aerosol (SOA) in the toluene/CH₃ONO/NO_x photooxidation system. The SMPS and aerosol laser time-of-flight mass spectrometer (ALTOFMS) was used to measure the aerodynamic size and chemical composition of individual SOA particles in real-time. Experimental results indicate that either the growth or products of SOA is affected by the presence of inorganic seed aerosol. Inorganic seed aerosols would promote growth rates of SOA formation at the start of the reaction and inhibits its formation rate with prolonging the reaction time. In the case of about 100 μg m^?3 seed aerosol load, the addition of Na₂SiO₃ induced a same growth rate of SOA formation as NaNO₃. The influence of four individual seed aerosols on the generation of SOA decreased in the order of CaCl₂ > (NH₄)₂SO₄ > NaNO₃, Na₂SiO₃. The presence of Na₂SiO₃ or NaNO₃ has no obvious effect on the growth rates of SOA formation, but it does increase the yield of organic acid and nitrogen-containing organic compounds, respectively. Besides the significantly effect on the growth rate of SOA formation, the presence of CaCl₂ or (NH₄)₂SO₄ can lead to the formation of high-molecular weight species which is found to be positively correlated with the hygroscopic behavior of seed aerosols. The CaCl₂ shows the strongest hygroscopic behavior among the four individual seed aerosols, and the most significant promotion effect on the formation of the high-molecular weight species. It is proposed that the SOA generation enhancement and high-molecular weight products are achieved by particle-phase heterogeneous reactions induced and catalyzed by the acidity of CaCl₂ and (NH₄)₂SO₄ seed aerosols.     

A three-dimensional model of the global ammonia cycle

Using a three-dimensional (3-D) transport model of the troposphere, we calculated the global distributions of ammonia (NH₃) and ammonium (NH ₄ ⁺ ), taking into account removal of NH₃ on acidic aerosols, in liquid water clouds and by reaction with OH. Our estimated global 10°×10° NH₃ emission inventory of 45 Tg N-NH₃ yr^– provides a reasonable agreement between calculated wet NH ₄ ⁺ deposition and measurements and of measured and modeled NH ₄ ⁺ in aerosols, although in Africa and Asia especially discrepancies exist.NH₃ emissions from natural continental ecosystems were calculated applying a canopy compensation point and oceanic NH₃ emissions were related to those of DMS (dimethylsulfide). In many regions of the earth, the pH found in rain and cloud water can be attributed to acidity derived from NO, SO₂ and DMS emissions and alkalinity from NH₃. In the remote lower troposphere, sulfate aerosols are calculated to be almost neutralized to ammonium sulfate (NH₄)₂SO₄, whereas in the middle and upper troposphere, according to our calculations, the aerosol should be more acidic, as a result of the oxidation of DMS and SO₂ throughout the troposphere and removal of NH₃ on acidic aerosols at lower heights. Although the removal of NH₃ by reaction with the OH radical is relatively slow, the intermediate NH₂ radical can provide a substantial annual N₂O source of 0.9 _–0.4 ^+0.9 Tg, thus contributing byca. 5% to estimated global N₂O production. The oxidation by OH of NH₃ from anthropogenic sources accounts for 10% of the estimated total anthropogenic sources of N₂O. This source was not accounted for in previous studies, and is mainly located in the tropics, which have high NH₃ and OH concentrations. Biomass burning plumes, containing high NO _x and NH₃ concentrations provide favourable conditions for gas phase N₂O production. This source is probably underestimated in this model study, due to the coarse resolution of the 3-D model, and the rather low biomass burning NH₃ and NO _x emissions adopted. The estimate depends heavily on poorly known concentrations of NH₃ (and NO _x ) in the tropics, and uncertainties in the rate constants of the reactions NH₂ + NO₂ N₂O + H₂O (R4), and NH₂ + O₃ NH₂O + O₂ (R7).     

Traffic aerosols (18 nm particle size 18 μm) source apportionment during the winter period

In November 2004–January 2005, a micro orifice uniform deposit impactor (MOUDI) and a Nanometer (nanometer)-MOUDI were used in the center of Taiwan to measure particle size (18 nm particle size 18 μm) distributions of atmospheric aerosols at a traffic site during the winter period. The average Mass in Media Aerodynamic Diameter (MMAD) of suspended particles is 0.99 μm this study. As for the ultra fine and nanometer (nanometer) particle mode, the composition order for these major ions species was SO₄²⁻ NH₄⁺ NO₃⁻ Mg²⁺ Ca²⁺ Na⁺ K⁺ Cl⁻. An ion Chromatography (DIONEX-100) was used to analyze major anion species, Cl⁻, NO₃⁻, SO₄²⁻ and cation species, NH₄⁺Na⁺, K⁺, Ca²⁺Mg²⁺. Their concentrations were also extracted from various particles size modes (nanometer (nanometer), ultra fine, fine and coarse). The results obtained in this study also indicated that the average portions for the major ionic species (SO₄²⁻, NH₄⁺ and Mg²⁺) in the nanometer (nanometer), ultra fine, fine and coarse particulate modes are about 34%, 37%, 63% and 30%, respectively at this traffic sampling site during the winter period.     

A review of global stratospheric aerosol: Measurements, importance, life cycle, and local stratospheric aerosol

Stratospheric aerosol, noted after large volcanic eruptions since at least the late 1800s, were first measured in the late 1950s, with the modern continuous record beginning in the 1970s. Stratospheric aerosol, both volcanic and non-volcanic are sulfuric acid droplets with radii (concentrations) on the order of 0.1–0.5 µm (0.5–0.005 cm^− 3), increasing by factors of 2–4 (10–10³) after large volcanic eruptions. The source of the sulfur for the aerosol is either through direct injection from sulfur-rich volcanic eruptions, or from tropical injection of tropospheric air containing OCS, SO₂, and sulfate particles. The life cycle of non-volcanic stratospheric aerosol, consisting of photo-dissociation and oxidation of sulfur source gases, nucleation/condensation in the tropics, transport pole-ward and downward in the global planetary wave driven tropical pump, leads to a quasi steady state relative maximum in particle number concentration at around 20 km in the mid latitudes. Stratospheric aerosol have significant impacts on the Earth's radiation balance for several years following volcanic eruptions. Away from large eruptions, the direct radiation impact is small and well characterized; however, these particles also may play a role in the nucleation of near tropopause cirrus, and thus indirectly affect radiation. Stratospheric aerosol play a larger role in the chemical, particularly ozone, balance of the stratosphere. In the mid latitudes they interact with both nitrous oxides and chlorine reservoirs, thus indirectly affecting ozone. In the polar regions they provide condensation sites for polar stratospheric clouds which then provide the surfaces necessary to convert inactive to active chlorine leading to polar ozone loss. Until the mid 1990s the modern record has been dominated by three large sulfur-rich eruptions: Fuego (1974), El Chichón (1982) and Pinatubo (1991), thus definitive conclusions concerning the trend of non-volcanic stratospheric aerosol could only recently be made. Although anthropogenic emissions of SO₂ have changed somewhat over the past 30 years, the measurements during volcanically quiescent periods indicate no long term trend in non-volcanic stratospheric aerosol.     

Growth of monodisperse,submicron aerosol particles exposed to SO2, H2O2, and NH3

The growth of monodisperse particles (0.07 to 0.5 µm) exposed to SO₂ (0–860 ppb), H₂O₂ (0–150 ppb) and sometimes NH₃ (0–550 ppb) in purified air at 22 °C at relative humidities ranging from 25 to 75% were measured using the Tandem Differential Mobility Analyzer technique. The experiments were performed in a flow reactor with aqueous (NH₄)₂SO₄ and Na₂SO₄ droplets. For (NH₄)₂SO₄ droplets the fractional diameter growth was independent of size above 0.3 µm but decreased with decreasing size below that. When NH₃ was added the fractional growth increased with decreasing size. Measurements were compared with predictions of a model that accounts for solubility of the reactive gases, the liquid phase oxidation of SO₂ by H₂O₂, and ionic equilibria. Agreement between measured and predicted droplet growth is reasonable when the ionic strength effects are included. Theory and experiments suggest that NH₃ evaporation is responsible for the decrease in relative growth rates for small aqueous ammonium sulfate particles. The observed droplet growth rates are too slow to explain observed growth rates of secondary atmospheric sulfate particles.     

Characteristic features of air ions at Mace Head on the west coast of Ireland

Coastal nucleation events and behavior of cluster ions were characterized through the measurements of air ion mobility distributions at the Mace Head research station on the west coast of Ireland in 2006. We measured concentrations of cluster ions and charged aerosol particles in the size range of 0.34–40 nm. These measurements allow us to characterize freshly nucleated charged particles with diameters smaller than 3 nm. The analysis shows that bursts of intermediate ions (1.6–7 nm) are a frequent phenomenon in the marine coastal environment. Intermediate ion concentrations were generally close to zero, but during some nucleation episodes the concentrations increased to several hundreds per cm³. Nucleation events occurred during most of the measurement days. We classified all days into one of seven classes according to the occurrence and type of new particle formation. Nucleation events were observed during 207 days in 2006, most prominently in the spring and summer months. Rain-induced events, in turn, were observed during 132 days. Particle formation and growth events mostly coincided with the presence of low tide. Also small cluster ions (0.34–1.6 nm) were characterized. Average concentrations of small ions were 440 cm^− 3 for the negative ions and 423 cm^− 3 for the positive ions. Average mean mobilities of small ions were 1.86 cm²V^− 1s^− 1 and 1.49 cm²V^− 1s^− 1 for the negative and positive polarities, respectively. Concentrations of small ions were observed to be strongly dependent on the variations of meteorological parameters including wind speed and direction.     

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.     

Secondary aerosol formation and identification of regional source locations by PSCF analysis in the Indo-Gangetic region of India

Secondary aerosol formation was studied at Allahabad in the Indo-Gangetic region during a field campaign called Land Campaign-II in December 2004 (northern winter). Regional source locations of the ionic species in PM₁₀ were identified by using Potential Source Contribution Function (PSCF analysis). On an average, the concentration of water soluble inorganic ions (sum of anions and cations) was 63.2 μgm⁻³. Amongst the water soluble ions, average NO₃⁻ concentration was the highest (25.0 μgm⁻³) followed by SO₄²⁻ (15.8 μgm⁻³) and NH₄⁺ (13.8 μgm⁻³) concentrations. These species, contributed 87% of the total mass of water soluble species, indicating that most of the water soluble PM₁₀ was composed of NH₄NO₃ and (NH₄)₂SO₄/NH₄HSO₄ or (NH₄)₃H(SO₄)₂ particles. Further, the concentrations of SO₄²⁻, NO₃⁻, and NH4⁺ aerosols increased at high relative humidity levels up to the deliquescence point (∼63% RH) for salts of these species suggesting that high humidity levels favor the conversion and partitioning of gaseous SO₂, NO_x, and NH₃ to their aerosol phase. Additionally, lowering of ambient temperature as the winter progressed also resulted in an increase of NO₃⁻ and NH₄⁺ concentrations, probably due to the semi volatile nature of ammonium nitrate. PSCF analysis identified regions along the Indo-Gangetic Plain (IGP) including Northern and Central Uttar Pradesh, Punjab, Haryana, Northern Pakistan, and parts of Rajasthan as source regions of airborne nitrate. Similar source regions, along with Northeastern Madhya Pradesh were identified for sulfate.     

Kinetics of ammonia and ammonium ion inhibition of the atmospheric oxidation of aqueous sulfur dioxide by oxygen

This is the first study, which shows both NH₃ and NH₄⁺ to inhibit the autoxidation of aqueous SO₂ in the pH range 7.0–8.5. The rate of the autoxidation, R _aut , in both buffered and unbuffered media at a fixed pH is in conformity with the rate law:

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.     

Large aerosol particles in cirrus type clouds

Research flights in November 1990 over the central parts of the United States, Wyoming and Colorado, were aimed to the investigation of the properties and microstructure of cirrus clouds (mainly cirrocumulus lenticularis). Among the other parameters measured on board the NCAR Saberliner were the concentration and size distribution of submicron particles and, in some cases, the particle deliquescence. For coarse insoluble particles found inside and outside of cloud elements, size distributions and morphology information were obtained by evaluating inertial impactor samples with an optical microscope and scanning electron microscope. In addition, the coarse particle composition was determined by x-ray energy spectrum analysis. The following conclusions from these measurements are:The large and coarse particle size distribution can be roughly simulated by a log-normal function with the modus around r=0.5 μm. Particle concentrations are very variable between several tenths and several particles per cm³. Particle volume distribution features a distinct maximum around 0.75 μm without a broad plateau which was observed in the case of sampling at lower altitude. Aerosol composition heterogeneity at cirrus cloud level is well documented by the evaluation of the fine particle sampling taken with the UMR sampling system. This heterogeneity can be partly explained by the interaction between aerosol and cloud elements, which is documented by the measured particle size distribution curves inside and outside of cloud elements. Assuming that particle deliquescence is caused by H₂SO₄ and/or by (NH₄)₂SO₄, particle soluble mass fractions were found to be around 30% in the first case and about 40% in the second. The most frequently occurring elements in large and coarse particles at cirrus cloud level were Si, Cl, Ba, S, Ca and C.     

Characteristics of gaseous pollutants near a main traffic line in Beijing and its influencing factors

Automobile exhaust emissions are becoming increasingly serious with the drastic increase of the number of vehicles in Beijing. In order to investigate the air pollution level and characteristics in the areas near the main traffic lines in Beijing and to identify the contributions from traffic and other sources, gaseous pollutants including NOx, CO, O₃, SO₂, and meteorological parameters have been monitored at a monitoring site and a contrasting site in winter and summer in 2006. The volumes of vehicles on Beiyuan Road were recorded. The average concentrations of NO, NO₂, NOx, CO, O₃, and SO₂ at the monitoring site were 0.148 mg/m³, 0.107 mg/m³, 0.333 mg/m³, 5.110 mg/m³, 0.006 mg/m³, and 0.157 mg/m³, respectively during the sampling period in winter and 0.021 mg/m³, 0.068 mg/m³, 0.101 mg/m³, 4.170 mg/m³, 0.083 mg/m³, and 0.056 mg/m³, respectively in summer. The high concentrations of CO and O₃ reflect the influence of vehicles emission near the traffic lines evidently. The higher concentrations of CO, NO and O₃ in summer may indicate that the characteristics of traffic pollution were more pronounced in summer. Results of regression analysis showed that in winter the concentrations of SO₂ and CO were significantly positively correlated with the emission of heating boilers at night and negatively correlated with wind speed in daytime. The concentrations of NO and NOx were negatively correlated with wind speed, positively correlated with emission of heating boilers in daytime and positively correlated with traffic density at nighttime. The concentrations of NO₂ were positively correlated with the emission of heating boilers in daytime and traffic density at nighttime. In summer, the air quality at the monitoring site and the contrasting site was mainly influenced by the traffic emissions.     

Importance of sulfate emission to sulfur deposition at urban and rural sites in China

Throughfall (TF) and wet only (WO) deposition along with SO₂ and sulfate (SO₄²⁻) concentration in air at 4 urban and rural sites in southwestern China were monitored in order to understand the role of different forms of sulfur (S) emission to the S deposition and its effect in China. The sites were located in Chongqing, Hunan, and Guizhou provinces. S deposition at the most polluted site reached 15 g S m^− 2 yr^− 1. At three of the sites, located in the vicinity of several emission sources, dry S deposition is 2.1–4.2 times that of wet deposition, which is significantly higher than what is found in most other parts of the world.Main components in airborne particles (PM₁₀) are (NH₄)₂SO₄ and CaSO₄ at the highly polluted Tie Shan Ping (TSP) site. Dust particles of gypsum (CaSO₄) in the air are partly due to direct emission and partly from the reaction of calcium oxides and carbonates with sulfuric acid in the air. To illustrate the importance of sulfate emission to total S deposition we analyzed the source of S deposition based on both measurements and models. Results indicated that direct emission of SO₄²⁻ particles could account for high proportion in total S deposition at the three most polluted sites.     

Major ionic composition of precipitation in the Nam Co region, Central Tibetan Plateau

A total of 48 precipitation samples have been collected from individual precipitation events at the Nam Co Monitoring and Research Station for Multisphere Interactions (Nam Co Station, 30°47′N, 90°58′E; 4730 m a.s.l) located in the central Tibetan Plateau from August 2005 to August 2006. All samples were analyzed for major cations (NH₄⁺, Na⁺, K⁺, Ca²⁺ and Mg²⁺) and anions (Cl⁻, NO₃⁻ and SO₄²⁻), conductivity and pH. Precipitation pH values ranged from 6.03 to 7.38 with an average value of 6.59. The high pH is due to large inputs of crustal aerosols in the atmosphere, which contain a large fraction of carbonate. Ca²⁺ is the dominant cation in precipitation with an average value of 65.58 μeq L^− 1 (4.91–301.41 μeq L^− 1), accounting for 54% of the total cations in precipitation. HCO₃⁻ is the predominant anion, accounting for 62% of the total anions. When compared with data from a snow pit in the Zhadang Glacier 50 km away (5800 m a.s.l), major ion concentration in precipitation at the Nam Co Station is much higher due to local aerosol inputs. Correlation and empirical orthogonal function (EOF) analysis indicate that regional crustal aerosols and species from combustion emissions of residents are the major sources for these ions, lake salt aerosols from the Nam Co nearby and regional mineral aerosols from dry lake sediments are secondary sources, and sea salt contribution is the least due to the long distance transport.