Chemical characteristics of free tropospheric aerosols over the Japan Sea coast: aircraft-borne measurements

Atmospheric aerosol particulate matter was directly collected in the free troposphere over the Japan Sea coast between 1992 and 1994 using an aircraft-borne nine-stage cascade impactor (particle size range: 0.1–8 μm). The water-soluble components in the aerosol particulate matter were analyzed by ion chromatography. Particulate sulfate and ammonium were detected in most of the samples and their size distributions showed noticeable peaks below the 1 μm particle size range. Water-soluble calcium (Ca²⁺) was detected in half of the samples; the size distribution showed that the maximum particle size was larger than 1 μm. Highly concentrated Ca²⁺ in larger particles was possibly due to transport of Kosa aerosols from the Asian continent in the free troposphere. The concentration of fine particulate sulfate and ammonium tended to increase whenever Ca²⁺ was detected, which suggests possible mixing of Kosa aerosols and non-Kosa aerosols during long-range transport of air masses containing Kosa particles.     

Measurements of fine and ultrafine particles formation in photocopy centers in Taiwan

This study investigates the levels of particulate matter smaller than 2.5 μm (PM_2.5) and some selected volatile organic compounds (VOCs) at 12 photocopy centers in Taiwan from November 2004 to June 2005. The results of BTEXS (benzene, toluene, ethylbenzene, xylenes and styrene) measurements indicated that toluene had the highest concentration in all photocopy centers, while the concentration of the other four compounds varied among the 12 photocopy centers. The average background-corrected eight-hour PM_2.5 in the 12 photocopy centers ranged from 10 to 83 μg m⁻³ with an average of 40 μg m⁻³. The 24-h indoor PM_2.5 at the photocopy centers was estimated and at two photocopy centers exceeded 100 μg m⁻³, the 24-h indoor PM_2.5 guideline recommended by the Taiwan EPA. The ozone level and particle size distribution at another photocopy center were monitored and indicated that the ozone level increased when the photocopying started and the average ozone level at some photocopy centers during business hour may exceed the value (50 ppb) recommended by the Taiwan EPA. The particle size distribution monitored during photocopying indicated that the emitted particles were much smaller than the original toner powders. Additionally, the number concentration of particles that were smaller than 0.5 μm was found to increase during the first hour of photocopying and it increased as the particle size decreased. The ultrafine particle (UFP, <100 nm) dominated the number concentration and the peak concentration appeared at sizes of under 50 nm. A high number concentration of UFP was found with a peak value of 1E+8 particles cm⁻³ during photocopying. The decline of UFP concentration was observed after the first hour and the decline is likely attributable to the surface deposition of charged particles, which are charged primarily by the diffusion charging of corona devices in the photocopier. This study concludes that ozone and UFP concentrations in photocopy centers should be concerned in view of indoor air quality and human health. The corona devices in photocopiers and photocopier-emitted VOCs have the potential to initiate indoor air chemistry during photocopying and result in the formation of UFP.     

Change of the ambient particle size distribution in East Germany between 1993 and 1999

Size distribution of particle number concentrations in the geometric equivalent diameter range 0.01–2.5 μm were determined in three communities, Zerbst, Bitterfeld and Hettstedt of the state of Sachsen-Anhalt in Eastern Germany, in the first half of 1993 and 1999. A Mobile Aerosol Spectrometer (MAS) consisting of a differential mobility particle spectrometer (DMPS) and a laser aerosol spectrometer (LAS-X) were used for size-selective particle number concentration measurements from which mass concentrations were derived based on an apparent mean density of the ambient aerosol of the closely situated city of Erfurt.The total number concentration was governed by ultra-fine particles (<0.1 μm) (81% in 1993 and 90% in 1999) and 0.1–0.5 μm size fraction dominates total mass concentration (approximately 80%). While the mass concentration of fine particles (PM2.5) decreased from 39 to 19 μg m⁻³, the geometric means of total number concentration showed constant concentration (13.3×10³ cm⁻³ in 1993 and 13.3×10³ cm⁻³ in 1999, p=0.975) and the geometric means of number concentration of ultra-fine particles (UP) between 10 and 30 nm increased from 5.9×10³ to 8.2×10³ cm⁻³ from 1993 to 1999 (p=0.016). The temporal changes of number and mass concentrations in the three communities are similar. The clear shift to smaller particle sizes within this six years period was caused by changes of the most prominent sources, traffic and domestic heating, since formerly dominating industries in Bitterfeld and Hettstedt had vanished grossly.     

Particulate matter in the indoor air of classrooms—exploratory results from Munich and surrounding area

Numerous epidemiological studies have demonstrated the association between particle mass (PM) concentration in outside air and the occurrence of health related problems and/or diseases. However, much less is known about indoor PM concentrations and associated health risks. In particular, data are needed on air quality in schools, since children are assumed to be more vulnerable to health hazards and spend a large part of their time in classrooms.On this background, we evaluated indoor air quality in 64 schools in the city of Munich and a neighbouring district outside the city boundary. In winter 2004–2005 in 92 classrooms, and in summer 2005 in 75 classrooms, data on indoor air climate parameters (temperature, relative humidity), carbon dioxide (CO₂) and various dust particle fractions (PM₁₀, PM_2.5) were collected; for the latter both gravimetrical and continuous measurements by laser aerosol spectrometer (LAS) were implemented. In the summer period, the particle number concentration (PNC), was determined using a scanning mobility particle sizer (SMPS). Additionally, data on room and building characteristics were collected by use of a standardized form. Only data collected during teaching hours were considered in analysis. For continuously measured parameters the daily median was used to describe the exposure level in a classroom.The median indoor CO₂ concentration in a classroom was 1603 ppm in winter and 405 ppm in summer. With LAS in winter, median PM concentrations of 19.8 μg m⁻³ (PM_2.5) and 91.5 μg m⁻³ (PM₁₀) were observed, in summer PM concentrations were significantly reduced (median PM_2.5=12.7 μg m⁻³, median PM₁₀=64.9 μg m⁻³). PM_2.5 concentrations determined by the gravimetric method were in general higher (median in winter: 36.7 μg m⁻³, median in summer: 20.2 μg m⁻³) but correlated strongly with the LAS-measured results. In explorative analysis, we identified a significant increase of LAS-measured PM_2.5 by 1.7 μg m⁻³ per increase in humidity by 10%, by 0.5 μg m⁻³ per increase in CO₂ indoor concentration by 100 ppm, and a decrease by 2.8 μg m⁻³ in 5–7th grade classes and by 7.3 μg m⁻³ in class 8–11 compared to 1–4th class. During the winter period, the associations were stronger regarding class level, reverse regarding humidity (a decrease by 6.4 μg m⁻³ per increase in 10% humidity) and absent regarding CO₂ indoor concentration. The median PNC measured in 36 classrooms ranged between 2622 and 12,145 particles cm⁻³ (median: 5660 particles cm⁻³).The results clearly show that exposure to particulate matter in school is high. The increased PM concentrations in winter and their correlation with high CO₂ concentrations indicate that inadequate ventilation plays a major role in the establishment of poor indoor air quality. Additionally, the increased PM concentration in low level classes and in rooms with high number of pupils suggest that the physical activity of pupils, which is assumed to be more pronounced in younger children, contributes to a constant process of resuspension of sedimented particles. Further investigations are necessary to increase knowledge on predictors of PM concentration, to assess the toxic potential of indoor particles and to develop and test strategies how to ensure improved indoor air quality in schools.     

Urban scale modeling of particle number concentration in Stockholm

A three-dimensional dispersion model has been implemented over the urban area of Stockholm (35×35 km) to assess the spatial distribution of number concentrations of particles in the diameter range 3–400 nm. Typical number concentrations in the urban background of Stockholm is 10 000 cm⁻³, while they are three times higher close to a major highway outside the city and seven times higher within a densely trafficked street canyon site in the city center. The model, which includes an aerosol module for calculating the particle number losses due to coagulation and dry deposition, has been run for a 10-day period. Model results compare well with measured data, both in levels and in temporal variability. Coagulation was found to be of little importance in terms of time averaged concentrations, contributing to losses of only a few percent as compared to inert particles, while dry deposition yield particle number losses of up to 25% in certain locations. Episodic losses of up to 10% due to coagulation and 50% due to deposition, are found some kilometers downwind of major roads, rising in connection with low wind speed and suppressed turbulent mixing. Removal due to coagulation and deposition will thus be more significant for the simulation of extreme particle number concentrations during peak episodes.The study shows that dispersion models with proper aerosol dynamics included may be used to assess particle number concentrations in Stockholm, where ultrafine particles principally originate from traffic emissions. Emission factors may be determined from roadside measurements, but ambient temperature must be considered, as it has a strong influence on particle number emissions from vehicles.     

The effect of humidity and state of water surfaces on deposition of aerosol particles onto a water surface

Deposition processes of particles with dry diameter larger than about 10 μm are dominated by gravitational settling, while molecular diffusion and Brownian motion predominate the deposition processes of particles smaller than 0.1 μm in dry diameter. Many air pollution derived elements exhibit characteristics common to sub-micron particles. The objective of the present study is to examine the effects of meteorological conditions within the turbulent transfer layer on the deposition velocity of particles with dry diameter between 0.1 and 1 μm. It is for these sub-micron particles that particle growth by condensation in the deposition layer, the broken water surface effect and the enhanced transfer process due to atmospheric turbulence in the turbulent transfer layer play important roles in controlling the particle deposition velocity. Results of the present study show that the `dry air’ assumption of Williams’ model is unrealistic. Effects of ambient air relative humidity and water surface temperature cannot be ignored in determining the deposition velocity over a water surface. Neglecting effects of ambient air relative humidity and water surface temperature will result in defining atmospheric stability incorrectly. It is found that the largest effect of air relative humidity on deposition velocity occurs at an air–water temperature difference corresponding to the point of `displaced neutral stability'. For a given wind speed of U=5 m s⁻¹ the additive effects of water surface temperature, T_w, changes from 5 to 25°C and ambient air relative humidity variations from 85 to 60%, respectively, lead to a maximum difference in v_d of about 20%. For a higher wind speed of 10 m s⁻¹, however, the corresponding change in v_d reduces to less than 5%. This is further confirmation that wind speed is one of the strongest variables that governs the magnitude of v_d. The present study also found that the broken surface transfer coefficient, k_bs, given as a multiple of the smooth surface transfer coefficient, k_ss, is physically more meaningful than assigning it a constant value independent of particle size. The method used in this study requires only a single level of atmospheric data coupled with the surface temperature measurement. The present method is applicable for determining deposition velocity not only at the conventional measurement height of 10 m but also at any other heights that are different from the measurement height.     

Size-resolved,real-time measurement of water-insoluble aerosols in metropolitan Atlanta during the summer of 2004

During the month of August 2004, the size-resolved number concentration of water-insoluble aerosols (WIA) from 0.25 to 2.0 μm was measured in real-time in the urban center of Atlanta, GA. Simultaneous measurements were performed for the total aerosol size distribution from 0.1 to 2.0 μm, the elemental and organic carbon mass concentration, the aerosol absorption coefficient, and the aerosol scattering coefficient at a dry (RH=30%) humidity. The mean aerosol number concentration in the size range 0.1–2.0 μm was found to be 360±175 cm⁻³, but this quantity fluctuated significantly on time scales of less than one hour and ranged from 25 to 1400 cm⁻³ during the sample period. The mean WIA concentration (0.25–2.0 μm) was 13±7 cm⁻³ and ranged from 1 to 60 cm⁻³. The average insoluble fraction in the size range 0.25–2.0 μm was found to be 4±2.5% with a range of 0.3–38%. The WIA population was found to follow a consistent diurnal pattern throughout the month with concentration maxima concurring with peaks in vehicular traffic flow. WIA concentration also responded to changes in meteorological conditions such as boundary layer depth and precipitation events. The temporal variability of the absorption coefficient followed an identical pattern to that of WIA and ranged from below the detection limit to 55 Mm⁻¹ with a mean of 8±6 Mm⁻¹. The WIA concentration was highly correlated with both the absorption coefficient and the elemental carbon mass concentration, suggesting that WIA measurements are dominated by fresh emissions of elemental carbon. For both the total aerosol and the WIA size distributions, the maximum number concentration was observed at the smallest sizes; however the WIA size distribution also exhibited a peak at 0.45 μm which was not observed in the total population. Over 60% of the particles greater than 1.0 μm were observed to be insoluble in the water sampling stream used by this instrumentation. Due to the refractive properties of black carbon, it is highly unlikely that these particles could be composed of elemental carbon, suggesting a crustal source for super-micron WIA.     

Direct measurements and parameterisation of aerosol flux,concentration and emission velocity above a city

Articles have recently been published on aerosol size distributions and number concentrations in cities, however there have been no studies on transport of these particles. Eddy covariance measurements of vertical transport of aerosol in the size range 11 nm<D_p<3 μm are presented here. The analysis shows that typical average aerosol number fluxes in this size range vary between 9000 and 90,000 cm⁻² s⁻¹. With concentrations between 3000 and 20,000 cm⁻³ this leads to estimates of particle emission velocity between 20 and 75 mm s⁻¹. The relationships between number flux and traffic activity, along with emission velocity and boundary layer stability are demonstrated and parameterised. These are used to derive an empirical parameterisation for aerosol concentration in terms of traffic activity and stability. The main processes determining urban aerosol fluxes and concentrations are discussed and quantified where possible. The difficulties in parameterising urban activity are discussed.     

Experimental study of the air pollution transport by synchronised monitoring of atmospheric aerosols

Particulate pollution transport is estimated by means of cross-correlation and regression analyses. The aerosol particle size number spectrum in the form of 12 fraction concentrations is measured in units cm⁻³ (particles per cm³) every 10 minutes during three approximately 20-day measurement campaigns simultaneously in two measurement points in Estonia. The distance between these points is approximately 100 km for two campaigns, and 7 km for the third campaign. Two electrical aerosol spectrometers designed at Tartu University, having a wide particle diameter range (10 nm–10 μm), are used. The spectrometer's record is the mean particle spectrum for the 10 min measurement time. The air pollution transport is investigated during the time intervals when the air mass moves from one measurement point towards the other. The time series of aerosol size fraction concentrations for both locations are prewhitened to eliminate auto-correlation and to achieve stationary series of the ARIMA residuals. Then the cross-correlation function of these two series of residuals is calculated. The time lag corresponding to the mode of this function is treated as the mean time of pollution transport from the windward measurement point to the leeward one. For the submicron aerosol fraction (d=60 nm–1 μm) 3–5 h time lags are found. Mostly these time lags coincide with the mean wind velocities on some of the pressure levels (ground, 850 and 700 hPa) available in the study. In cross-wind cases the fraction concentrations measured in two points separated by 100 km were uncorrelated, but for the two points separated by 7 km there was quite a high correlation with zero time lag. The part of local and distant sources in the formation of the particle concentration in the leeward location is estimated by regression analysis.     

Nanoparticle emissions on Minnesota highways

The objective of this project was to characterize on-road aerosol on highways surrounding the Minneapolis area. Data were collected under varying on-road traffic conditions and in residential areas to determine the impact of highway traffic on air quality. The study was focused on determining on-road nanoparticle concentrations, and estimating fuel-specific and particle emissions km⁻¹.On-road aerosol number concentrations ranged from 10⁴ to 10⁶ particles cm⁻³. The highest nanoparticle concentrations were associated with high-speed traffic. At high vehicular speeds engine load, exhaust temperature, and exhaust flow all increase resulting in higher emissions. Less variation was observed in particle volume, a surrogate measure of particle mass. Most of the particles added by the on-road fleet were below 50 nm in diameter. Particles in this size range may dominate particle number, but contribute little to particle volume or mass. Furthermore, particle number is strongly influenced by nucleation and coagulation, which have little or no effect on particle volume. Measurements made in heavy traffic, speeds<32 km h⁻¹, produced lower number concentrations and larger particles.Number concentrations measured in residential areas, 10–20 m from the highway, were considerably lower than on-road concentrations, but the size distributions were similar to on-road aerosol with high concentrations of very small (<20 nm) particles. Much lower number concentrations and larger particles were observed in residential areas located 500–700 m from the highway.Estimated emissions of total particle number larger than 3 nm ranged from 1.9 to 9.9×10¹⁴ particles km⁻¹ and 2.2–11×10¹⁵ particles (kg fuel)⁻¹ for a gasoline-dominated vehicle fleet.     

Seasonal characteristics of water-soluble organic carbon in atmospheric particles in the inland Kanto plain,Japan

An investigation of water-soluble organic carbon (WSOC) in atmospheric particles was conducted as an index of the formation of secondary organic aerosol (SOA) from April 2005 to March 2006 at Maebashi and Akagi located in the inland Kanto plain in Japan. Fine (<2.1 μm) and coarse (2.1–11 μm) particles were collected by using an Andersen low-volume air sampler, and WSOC, organic carbon (OC), elemental carbon (EC), and ionic components were measured. The mean mass concentrations of the fine particles were 22.2 and 10.5 μg m^?3 at Maebashi and Akagi, respectively. The WSOC in fine particles accounted for a large proportion (83%) of total WSOC. The concentration of fine WSOC ranged from 1.2 to 3.5 μg-C m^?3 at Maebashi, rising from summer to fall. At Akagi, it rose from spring to summer, associated with the southerly wind from urban areas. The WSOC/OC ratio increased in summer at both sites, but the ratio at Akagi was higher, which we attributed to differences in primary emissions and secondary formation between the sites. The fine WSOC concentration was significantly positively correlated with concentrations of SO₄^2?, EC, and K⁺, and we inferred that WSOC was produced by photochemical reaction and caused by the combustion of both fuel and biomass. We estimated that SOA accounted for 11–30% of the fine particle mass concentration in this study, suggesting that SOA is a significant year-round component in fine particles.     

Deposition velocity of PM2.5 sulfate in the summer above a deciduous forest in central Japan

In order to increase knowledge of aerosol dry deposition for the regional assessment of acid deposition and transboundary air pollution in East Asia, an experimental study on PM2.5 sulfate deposition was implemented in the early summer of 2009. The experimental field was located in a deciduous forest at the foot of Mt. Asama, central Japan. Aerosol fluxes were obtained using the aerodynamic gradient method. Three aerosol samplers were placed on an experimental tower at 21, 24 and 27 m above the ground surface, and collected PM2.5 on filters for chemical analysis. Vertical concentration differences between 21 m and 27 m of PM2.5 sulfate were detected significantly when the concentration exceeded 1 μg m^?3. Mean deposition velocity was estimated to be 0.9 ± 1.0 cm s^?1 in the daytime and 0.3 ± 0.3 cm s^?1 in the nighttime. In the case that a height-dependent correction in the roughness sub-layer was taken into account, the deposition velocities increased more, especially in daytime. Higher deposition velocities in the daytime were associated with larger friction velocities and unstable conditions. The deposition velocities observed in this study were in agreement with other experimental results found in the literature. On the other hand, they were higher than those calculated by theoretical models. Two empirical parameterizations (Wesely, M.L., Cook, D.R., Hart, R.L., 1985. Measurement and parameterization of particulate sulfur dry deposition over grass. Journal of Geophysical Research 90, 2131–2143; Ruijgrok, W., Tieben, H., Eisinga, P., 1997. The dry deposition of particles to a forest canopy: a comparison of model and experimental results. Atmospheric Environment 31, 399–415) were validated by the observations. The general trend of higher daytime and lower nighttime deposition velocities was similar among the observation and the two parameterizations. The large variability found in the measurement was not reproduced by the parameterizations, because it is attributable to random error from the differences between the samplers. The observations were in accordance with the parameterization of Ruijgrok et al. (1997) for a forest, although much larger than that of Wesely et al. (1985) for grasslands. This indicates the large difference in aerosol deposition velocities between forests and grasslands.     

The relationship between indoor and outdoor airborne particles in the residential environment

The relationship between indoor and outdoor airborne particles was investigated for 16 residential houses located in a suburban area of Brisbane, Australia. The submicrometer particle numbers were measured using the Scanning Mobility Particle Sizer, the larger particle numbers using the Aerodynamic Particle Sizer and an approximation of PM_2.5 was also measured using a DustTrak. The measurements were conducted for normal and minimum ventilation conditions using simultaneous and non-simultaneous measurement methods designed for the purpose of the study. Comparison of the ratios of indoor to outdoor particle concentrations revealed that while temporary values of the ratio vary in a broad range from 0.2 to 2.5 for both lower and higher ventilation conditions, average values of the ratios were very close to one regardless of ventilation conditions and of particle size range. The ratios were in the range from 0.78 to 1.07 for submicrometer particles, from 0.95 to 1.0 for supermicrometer particles and from 1.01 to 1.08 for PM_2.5 fraction. Comparison of the time series of indoor to outdoor particle concentrations shows a clear positive relationship existing for many houses under normal ventilation conditions (estimated to be about and above 2 h⁻¹), but not under minimum ventilation conditions (estimated to be about and below 1 h⁻¹). These results suggest that for normal ventilation conditions, outdoor particle concentrations could be used to predict instantaneous indoor particle concentrations but not for minimum ventilation, unless air exchange rate is known, thus allowing for estimation of the “delay constant”.     

Influence of the surface microlayer on atmospheric deposition of aerosols and polycyclic aromatic hydrocarbons

Atmospheric dry deposition is an important process for the introduction of aerosols and pollutants to aquatic environments. The objective of this paper is to assess, for the first time, the influence that the aquatic surface microlayer plays as a modifying factor of the magnitude of dry aerosol deposition fluxes. The occurrence of a low surface tension (ST) or a hydrophobic surface microlayer has been generated by spiking milli-Q water or pre-filtered seawater with a surfactant or octanol, respectively. The results show that fine mode (<2.7 μm) aerosol phase PAHs deposit with fluxes 2–3 fold higher when there is a low ST aquatic surface due to enhanced sequestration of colliding particles at the surface. Conversely, for PAHs bound to coarse mode aerosols (>2.7 μm), even though there is an enhanced deposition due to the surface microlayer for some sampling periods, the effect is not observed consistently. This is due to the importance of gravitational settling for large aerosols, rendering a lower influence of the aquatic surface on dry deposition fluxes. ST (mN m⁻¹) is identified as one of the key factor driving the magnitude of PAH dry deposition fluxes (ng m⁻² d⁻¹) by its influence on PAH concentrations in deposited aerosols and deposition velocities (v_d, cm s⁻¹). Indeed, v_d values are a function of ST as obtained by least square fitting and given by Ln(v_d)=−1.77 Ln(ST)+5.74 (r²=0.95) under low wind speed (average 4 m s⁻¹) conditions.     

Resuspension of coarse particles in the region of Chernobyl

Measurements of resuspension into air in the coarse particle range (>10 μm in aerodynamic diameter) were performed as part of a field measurement experiment at four sites around Chernobyl during wind-driven and anthropogenic enhanced resuspension (agricultural activities). Caesium-137 was used to quantify the magnitude of resuspension. The mean resuspension factor of coarse particles was between 1×10^-10 and 6×10^-10 m^-1 for wind-driven resuspension. During agricultural activities, the resuspension increased by up to three orders of magnitude. Coarse particles comprised about one-third of the total amount of resuspended Caesium-137. The activity size distribution of Caesium-137 was not uniform in the coarse particle range: approximately 44% of the activity was found in the range 10–20 μm aerodynamic diameter. The determination of the number concentration of particles >20 μm aerodynamic diameter showed a linear relation between particle number and activity: the mean activity per particle was 0.75±0.15 μBq at the site Novozybkov, Russia. The resuspension factor was found to decrease exponentially with increasing relative soil moisture content. At higher soil humidity, the portion of coarse particles of the total resuspended activity was larger.     

Mixing properties of individual submicrometer aerosol particles in Vienna

Individual aerosol particles were collected on 5 days with different meteorological conditions in March, April and June 1991 in the urban atmosphere of Vienna in Austria. The samples collected with an impactor were examined by electron microscopy. The mixing properties of submicrometer aerosol particles with radii between 0.1 and 1 μm were studied by using the dialysis (extraction) of water-soluble material. The averaged results showed that more than 85% of particles with radii between 0.1 and 0.7 μm were hygroscopic. However, more than 50% of particles with radii larger than 0.2 μm were mixed particles (hygroscopic particles with water-insoluble inclusions), and they were dominant (80%) in the size range 0.5–0.7 μm radius. The results also showed that the number proportion of mixed particles increased with increasing radius and the abundance increased with increasing particle loading in the atmosphere. The volume fraction of water-soluble material (ε) in mixed particles tended to decrease with increasing radius, implying the formation of mixed particles by heterogeneous processes such as condensation and/or surface reaction. Some results of elemental composition in individual particles analyzed with an energy-dispersive X-ray (EDX) analyzer equipped with an electron microscope are also presented in this paper.     

Carbonaceous aerosol in jet engine exhaust: emission characteristics and implications for heterogeneous chemical reactions

Characteristic parameters of black carbon aerosol (BC) emitted from jet engine were measured during ground tests and in-flight behind the same aircraft. Size distribution features were a primary BC mode at a modal diameter D≈0.045 μm, and a BC agglomeration mode at D<0.2 μm. The total BC number concentration at the engine exit was 2.9×10⁷ cm^-3 with good agreement between model results and in-flight measured number concentrations of non-volatile particles with D⩾0.014 μm. A comparison between total number concentration of BC particles and the non-volatile fraction of the total aerosol at the exit plane suggests that the non-volatile fraction of jet engine exhaust aerosol consists almost completely of BC. In-flight BC mass emission indices ranged from 0.11 to 0.15 g BC (kg fuel)^-1. The measured in-flight particle emission value was 1.75±0.15×10¹⁵ kg^-1 with corresponding ground test values of 1.0–8.7×10¹⁴ kg^-1. Both size distribution properties and mass emission indices can be scaled from ground test to in-flight conditions. Implications for atmospheric BC loading, BC and cirrus interaction and the potential of BC for perturbation of atmospheric chemistry are briefly outlined.     

Sources and concentrations of gaseous and particulate reduced nitrogen in the city of Münster (Germany)

Atmospheric ammonia mixing ratios and the main inorganic ions NH₄⁺, NO₃⁻ and SO₄²⁻ of size-resolved particles in the range from 0.05 to 10 μm were measured at an urban site in Münster, Germany. High mixing ratios of ammonia with a median of 5.2 ppb and a maximum of 50 ppb were detected. The mass fraction of submicron particles was much higher during the day than at night. At night, a greater particle mass and an increased presence of particulate nitrate was measured. Recurring patterns of particle distribution were distinguished and their characteristics analysed. In half of the measurements, the accumulation mode was clearly dominating, which is an indication of aged aerosol. In some measurements, higher concentrations of fine particles were found indicating particle formation. In these cases, a smaller particle mass and about four times greater ratios of ammonia versus ammonium concentrations were observed. These data show that ammonia contributes considerably to the formation of secondary particulate material.     

Dilution and aerosol dynamics within a diesel car exhaust plume—CFD simulations of on-road measurement conditions

Vehicle particle emissions are studied extensively because of their health effects, contribution to ambient PM levels and possible impact on climate. The aim of this work was to obtain a better understanding of secondary particle formation and growth in a diluting vehicle exhaust plume using 3-d information of simulations together with measurements. Detailed coupled computational fluid dynamics (CFD) and aerosol dynamics simulations have been conducted for H₂SO₄–H₂O and soot particles based on measurements within a vehicle exhaust plume under real conditions on public roads.Turbulent diffusion of soot and nucleation particles is responsible for the measured decrease of number concentrations within the diesel car exhaust plume and decreases coagulation rates. Particle size distribution measurements at 0.45 and 0.9 m distance to the tailpipe indicate a consistent soot mode (particle diameter D_p∼50 nm) at variable operating conditions. Soot mode number concentrations reached up to 10¹³ m⁻³ depending on operating conditions and mixing.For nucleation particles the simulations showed a strong sensitivity to the spatial dilution pattern, related cooling and exhaust H₂SO_4(g). The highest simulated nucleation rates were about 0.05–0.1 m from the axis of the plume. The simulated particle number concentration pattern is in approximate accordance with measured concentrations, along the jet centreline and 0.45 and 0.9 m from the tailpipe. Although the test car was run with ultralow sulphur fuel, high nucleation particle (D_p⩽15 nm) concentrations (>10¹³ m⁻³) were measured under driving conditions of strong acceleration or the combination of high vehicle speed (>140 km h⁻¹) and high engine rotational speed (>3800 revolutions per minute (rpm)).Strong mixing and cooling caused rapid nucleation immediately behind the tailpipe, so that the highest particle number concentrations were recorded at a distance, x=0.45 m behind the tailpipe. The simulated growth of H₂SO₄–H₂O nucleation particles was unrealistically low compared with measurements. The possible role of low and semi-volatile organic components on the growth processes is discussed. Simulations for simplified H₂SO₄–H₂O–octane–gasoil aerosol resulted in sufficient growth of nucleation particles.     

Effect of forest edges on deposition of radioactive aerosols

The possible enhancement of aerosol deposition at forest edges was investigated in a wind tunnel and in the field. The wind tunnel study was carried out using 0.82 μm mass median aerodynamic diameter uranium particles and a composite canopy of rye grass and spruce saplings. The field study was undertaken at a coniferous woodland near to BNFL Sellafield, Cumbria, UK. Two transects were set through the woodland to determine the influence of the forest edge on atmospheric deposition of radionuclides released under authorisation from the Sellafield site. Results from the wind tunnel study showed that the deposition flux of uranium particles decreased with distance downwind from the grass–tree edge towards the interior of the canopy. The deposition flux at the edge was maximal at about 4×10⁻⁷ μg of U cm⁻² s⁻¹. This was 3 times higher than that observed over grass where a constant flux of about 1.32×10⁻⁷ μg of U cm⁻² s⁻¹ occurred. Results from the field study showed a clear influence of the forest edge on the atmospheric deposition of ²⁴¹Am and ¹³⁷Cs. Activity depositions of around 4750 and 230 Bqm⁻² for ¹³⁷Cs and ²⁴¹Am, respectively, were measured in front of the woodland. Activity deposition inside the forest edge, however, rose to levels of between 20,200 and 50,900 Bq m⁻² and 1100 and 3200 Bq m⁻² for ¹³⁷Cs and ²⁴¹Am, respectively, depending upon the transect. Similar activity concentrations were measured in the pasture to the front and behind Lady Wood. Results from these studies corroborate those obtained from various studies on air pollutants including radionuclides. This underlines the importance of deposition at the edge of forests and its contribution to the overall canopy deposition. The edge effect is therefore an important factor that should be considered in the assessment of fallout impact, whether this is to be made by either direct sampling or by modelling.