On the prediction of concentration variations in a dispersing heavy-duty truck exhaust plume using k–ε turbulent closure

This work presents the computational fluid dynamic modeling of an exhaust plume dispersed from the exhaust pipe of a class-8 tractor truck powered by 330 hp Cummins M11 electronically controlled diesel engine. This effort utilizes an advanced CFD technique to accurately predict the variation of carbon dioxide concentration inside a turbulent plume using a k–ε eddy dissipation model. The simulation includes the “real-world” operation of a truck and its exhaust plume in a NASA, Langley aircraft testing wind tunnel, that had an effective volume of 226, 535 m³ (8,000,000 ft³). The predicted results show an excellent agreement with the experimentally measured values of CO₂ concentrations, dilution ratios, and the temperature variations inside the plume. A specific goal of this effort was to study the effect of recirculation region near the truck walls on dispersion of the plume. For this purpose, growth of the plume from the center of the exhaust pipe is also presented and discussed. This work also shows the benefits of CFD modeling in applications where dispersion correlations are not required a priori, instead the dispersion coefficients are calculated precisely by solving the turbulent kinetic energy and dissipation equations.     

Modelling plume rise and dispersion from pool fires

This paper describes an investigation into the behaviour of smoke plumes from pool fires, and the subsequent generation of empirical models to predict plume rise and dispersion from such a combustion source. Synchronous video records of plumes were taken from a series of small-scale (0.06–0.25m²) outdoor methanol/toluene pool fire experiments, and used to produce sets of images from which plume dimensions could be derived. Three models were used as a basis for the multiple regression analysis of the data set, in order to produce new equations for improved prediction. Actual plume observations from a large (20.7 m×14.2 m) aviation fuel pool fire were also used to test the predictions. The two theoretically based models were found to give a better representation of plume rise and dispersion than the empirical model based on measurements of small-scale fires. It is concluded that theoretical models tested on small-scale fires (heat output ≈70 kW) can be used to predict plume behaviour from much larger combustion sources (heat output ≈70 MW) under near neutral atmospheric conditions.     

Comparison of concentration/flux ratios measured with a backscatter Lidar and with a chemical tracer

A series of backscatter Lidar measurements were made around a bio-waste power station at Eye in Suffolk over a period of 10 days in May 1999. These measurements were supplemented with bag samples of SF₆ tracer, analysed on site using gas chromatography with an electron capture detector. Despite problems with contamination, a detection limit of 20 ppt was eventually achieved and this permitted useful plume measurements from a release rate of 1–2 l min⁻¹. Concentration/flux ratios were estimated from the Lidar measurements using an integral technique. Of the Lidar runs obtained, 24 were coincident with a tracer release. After allowing for the background of both aerosol and tracer, it was apparent that the independent calibrations of concentration/flux ratio from Lidar or tracer agreed with each other to within 20–60%. This permits the Lidar scans to be used to estimate peak near-ground concentrations, though because of various technical difficulties (poor alignment, background sources of aerosol, or an inconvenient wind direction) this cannot always be achieved. Besides giving confidence in the Lidar calibration, the tracer measurements were valuable in permitting aerosol from the stack to be distinguished from aerosol from fugitive sources. Meteorological parameters were logged simultaneously with the dispersion measurements. These parameters included conventional means of wind speed and direction, temperature, humidity and insolation, and also micrometeorological measurements of turbulence and of turbulent fluxes. The Lidar was used to estimate wind speed and direction at plume height and the boundary layer depth and cloud-base where possible. Source emission characteristics were also logged.     

The characteristics of Asian-dust storms during 2000–2002: From the source to the sea

About 42 Asian-dust storms influenced the mainland and China during 2000–2002. Based on the Micaps meteorology data provided by China Meteorological Administration, the basic characteristics, including the source, movement route and influenced areas were studied for each case. It was shown that about 70% Asian-dust storms that influence China came from Mongolia, and were strengthened during the way from west to east. In 2000–2002, there was about 63.9% Asian-dust weather that might have affected China seas through three different routes. The probability is affecting the Bohai Sea was 27.4%, the Yellow Sea 30.9%, the East China Sea 12.3%, the Korea Channel 20.2% and the Japan Sea 9.2%. Annual dry deposition flux to the Yellow Sea was about 0.13 g m⁻² d⁻¹, and in spring was ∼0.20 g m⁻² d⁻¹. The total amount of dry deposition to the Yellow Sea was ∼17.9 Tg yr⁻¹.     

Sources and concentration of nanoparticles (<10 nm diameter) in the urban atmosphere

Whilst limited information on particle size distributions and number concentrations in cities is available, very few data on the very smallest of particles, nanoparticles, have been recorded. Measurements in this study show that road traffic and stationary combustion sources generate a significant number of nanoparticles of diameter <10 nm. Measurements at the roadside (4 m from the kerb) and downwind from the traffic (more than 25 m from the kerb) show that nanoparticles (<10 nm diameter) accounted for more than 36–44% of the total particle number concentrations. Measurements designed to sample the plume of individual vehicles showed that both a diesel- and a petrol-fuelled vehicle generated nanoparticles (<10 nm diameter). The fraction of nanoparticles was even greater in a plume 350 m downwind of a stationary combustion source. On a few occasions, a temporal association between nanoparticles in the size range 3–7 nm and solar radiation was observed in urban background air at times when no other local sources were influential, which suggests that homogeneous nucleation can also be an important source of particles in the urban atmosphere.     

Natural emissions of methane from geological seepage in Europe

Recent studies have shown that geological emissions of methane are an important greenhouse-gas source. Remarkable amounts of methane, estimated in the order of 40–60 Tg yr^?1, are naturally released into the atmosphere from the Earth's crust through faults and fractured rocks. The main source is natural gas, both microbial and thermogenic, produced in hydrocarbon-prone sedimentary basins and injected into the atmosphere through macro-seeps (onshore and offshore mud volcanoes and other seeps) and microseepage, an invisible but pervasive flux from the soil. This source is now evaluated for Europe on the basis of a literature survey, new field measurements and derived emission factors. The up-scaling criteria recommended by the EMEP/CORINAIR guidelines are applied to the local point and area source data.In Europe, 25 countries host oil and/or natural gas reservoirs and potentially, or actually, emit geological methane. Flux data, however, are available only from 10 countries: the onshore or offshore petroliferous sectors of Denmark, Italy, Greece, Romania, Spain, Switzerland, United Kingdom and Black Sea countries (Bulgaria, Ukraine, Georgia). Azerbaijan, whose emissions due to mud volcanism are known to be relevant, is included in the estimate.The sum of emissions, regional estimates and local measurements, related to macro-seeps leads to a conservative total value of about 2.2 Tg yr^?1. Together with the potential microseepage fluxes from the petroliferous basins, estimated on the basis of the Total Petroleum System concept (around 0.8 Tg yr^?1), the total European seepage is projected to 3 Tg yr^?1. This preliminary figure would represent, in terms of magnitude, the second natural methane source for Europe after wetlands. The estimate will have to be refined by increasing the number of seepage measurements both on lands, where there is high potential for microseepage (e.g., Germany, Hungary, Romania, Ukraine, Belarus, Russia, Georgia) and in coastal marine areas (the North Sea, the Black Sea, offshore Greece and Italy) where emission factors and the extent of the underwater seeping area are not completely known.     

Evaluation of the reactive and optics model of emissions (ROME)

The reactive and optics model of emissions (ROME) is a reactive plume visibility model that simulates the potential atmospheric impacts of stack emissions. We present here an evaluation of the ability of ROME to simulate several plume physical and chemical variables, using an experimental data base that consists of a total of 40 case studies from four field programs. The evaluation variables include plume height, horizontal width, NO_x and SO₂ maximum concentrations, NO₂/NO_x concentration ratio at the plume centerline, and plume-to-sky radiance ratios. Three algorithms used to simulate plume dispersion in ROME were compared: (1) the empirical Pasquill–Gifford–Turner (PGT) scheme, (2) a first-order closure (FOC) algorithm and (3) a second-order closure (SOC) algorithm that simulates the instantaneous plume dimensions.The plume height results show a correlation of 0.82 between simulated and measured values and a gross error that is 13% of the mean measured value. For plume horizontal dispersion, the second-order closure algorithm produces a moderate correlation (0.54) and a small bias (5% of the mean measured value) in comparison with the field data. Although the PGT scheme also demonstrates moderate correlation with the measurements, it produces a negative bias by significantly underestimating plume horizontal dispersion. The first-order closure algorithm overestimates plume width and shows the least correlation (with the measurements) of the three dispersion algorithms.For the NYSEG data set where coordinated measurements of stack emissions, meteorology at plume height and plume characteristics were available, the SOC algorithm provides better correlations for NO_x concentrations, NO₂/NO_x ratios and plume visibility than the FOC and PGT algorithms. For plume visibility, the SOC algorithm shows a correlation of 0.96 at 405 nm, the wavelength where the plume was visible, and it simulates no visible plume at the other wavelengths (550 and 700 nm).A comparison of ROME simulations with those of the plume visibility model PLUVUE II shows that ROME, with the SOC algorithm, performs better for all variables.     

Synoptic weather patterns and their relationship to high ozone concentrations in the Taichung Basin

Frequent high ozone days (defined as daily maximum ozone concentration ⩾80 ppb) during recent years in the Taichung Basin have caused much concern. High ozone days occur mainly during autumn and spring. Statistically, there is no clear linear relationship between a single meteorological variable and ozone concentration. In this study, data from 1996–2000 has shown that high ozone concentrations occur during two types of synoptic weather patterns. The first type is a continental cyclone emanating from mainland China, the southern part of it swept towards Taiwan by easterly winds. The second pattern is a tropical depression moving northwards toward the region, the northern part of it affecting Taiwan via easterly winds. Both types cover Taiwan with easterly winds, which are blocked by the Central Mountain Ranges (altitude of 2000–3000 m). The ranges create lee cyclogenesis to the west, which is unfavorable for pollutant dispersion and leads to serious air pollution episodes.The statistical results of the synoptic weather patterns in relation to ozone concentrations are based on the 5 yr data (1996–2000). This was obtained from a network of air-pollution monitoring sites in the study area, while the vertical data come from two 3-day tethersonde experimental campaigns conducted during March and October 2000, measuring air pressure, air temperature, relative humidity, wind speed and direction, non-methane hydrocarbons, NO_x and O₃.     

Physical features of the atmospheric aerosol determined with an aureolemeter and a FSSP probe in the Mediterranean Lampedusa island

In order to investigate the influence of the atmospheric aerosol on the ultraviolet radiation on earth, the measurement campaign Photochemical Activity and Ultraviolet Radiation (PAUR II) Modulation was carried out in the central Mediterranean Sea during the period May–June 1999. Two sites were chosen for measurements: the island of Crete (Greece), and the island of Lampedusa (Italy). The aerosol features over the Lampedusa island, as well as the dust coming from Sahara desert, were investigated by measurements of direct and diffuse solar irradiance carried out with an aureolemeter. The columnar volume size distributions of the aerosol showed a four-modal shape in a less turbid atmosphere when the aerosol optical depth was less than 0.2 at λ=500 nm, and a tri-modal shape in a turbid atmosphere when the aerosol optical depth at the same wavelength was greater than 0.5; the background aerosol turned out to be mainly composed of sea salt. The increase of the aerosol optical depth and of the particles density with radius about 1 μm has been found to be strictly related to the passage of Saharan dust in the time periods 14–22 May and 1–3 June, 1999. The columnar volume of particles obtained by the aureolemeter has been compared with the columnar volume of particles retrieved by in situ measurements carried out with a forward scattering spectrometer probe (FSSP) aboard a light aircraft flying over the island. Although the above two techniques refer to aerosol columns of different height and operate with different resolutions, their relevant results are in good agreement, especially during days with lower aerosol content. The two volume radius distributions have been also compared and their behaviours show a satisfactory agreement, mainly for particles with radius greater than 1 μm.     

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.     

Ions in motor vehicle exhaust and their dispersion near busy roads

Measurements in the exhaust plume of a petrol-driven motor car showed that molecular cluster ions of both signs were present in approximately equal amounts. The emission rate increased sharply with engine speed while the charge symmetry remained unchanged. Measurements at the kerbside of nine motorways and five city roads showed that the mean total cluster ion concentration near city roads (603 cm^?3) was about one-half of that near motorways (1211 cm^?3) and about twice as high as that in the urban background (269 cm^?3). Both positive and negative ion concentrations near a motorway showed a significant linear increase with traffic density (R² = 0.3 at p < 0.05) and correlated well with each other in real time (R² = 0.87 at p < 0.01). Heavy duty diesel vehicles comprised the main source of ions near busy roads. Measurements were conducted as a function of downwind distance from two motorways carrying around 120–150 vehicles per minute. Total traffic-related cluster ion concentrations decreased rapidly with distance, falling by one-half from the closest approach of 2 m to 5 m of the kerb. Measured concentrations decreased to background at about 15 m from the kerb when the wind speed was 1.3 m s^?1, this distance being greater at higher wind speed. The number and net charge concentrations of aerosol particles were also measured. Unlike particles that were carried downwind to distances of a few hundred metres, cluster ions emitted by motor vehicles were not present at more than a few tens of metres from the road.     

An episode of photooxidant plume pollution over the Paris region

An ozone pollution episode typically at the mesoscale is studied for the period 17–20 July 1996 in the northern half of France. This episode has been documented through extra stations supplementing the regular French network in the southwest of the Paris region at large: the ozone threshold value of 90 ppb has been observed to be exceeded only at downwind rural stations at distances ranging between 25 and 110 km from downtown Paris. This episode has been simulated with the mesoscale model Meso-NH-C in which the meteorological model Meso-NH is coupled on-line with a chemistry module. Various assumptions are presented which must be made in order to run Meso-NH-C:  e.g. reduction of the chemical scheme to reduce the computational costs or definition of procedures to fill in the lack of emission inventory data. Meso-NH appears to realistically simulate the position, extent, average and peak ozone values within the pollution plume. Sensitivity analyses emphasize, in particular, the need for accurate simulation of the wind field to capture correct characteristics of this plume.     

Mineralogical and chemical characterization of suspended atmospheric particles over the east Mediterranean based on synoptic-scale circulation patterns

Suspended atmospheric particles were collected in Israel in order to identify their nature and relationships with the major synoptic-scale circulation patterns. The particles were analyzed for their major and trace element concentrations and mineralogical composition. Samples were collected during three synoptic systems associated with desert dust storms: Red Sea trough, Sharav cyclone and cold depression, and during deep and shallow modes of Persian Gulf trough, which prevails in the summer months and is not associated with dust storms.All samples mostly contain particles smaller than 2 μm. The suspended desert dust is composed primarily of illite–smectite and calcite. Some indicative secondary minerals were found for each of the dust transporting synoptic systems (e.g., palygorskite for Red Sea trough). The bulk chemistry data support the mineralogical observations and reveal additional chemical signatures of each dust transporting system. For instance, Red Sea trough samples have significantly higher Ca/Al and Ca/Mg in the carbonate and Mg/Al in Al-silicate fraction than cold depression samples. Nevertheless, Sharav cyclone samples have intermediate values in spite of the fact that the source of the dust during these conditions is similar to cold depression (i.e., North Africa). Even though differences in the chemical and the mineralogical composition of desert dust do exist, this study reveals their overall chemical and mineralogical similarities.In contrast to the synoptic systems that carry desert dust, the inorganic fraction of the Persian Gulf trough samples contains significant amount (up to 50%) of non-mineral material that has a pronounced chemical signature in terms of major element concentrations (e.g., Al, Ca, Mg, Na, S) implying their anthropogenic nature, probably from countries around the Black Sea. This striking finding is indicative for atmospheric pollution in the Eastern Mediterranean region during the summer.     

Flow patterns influencing the seasonal behavior of surface ozone and carbon monoxide at a coastal site near Hong Kong

Surface O₃ and CO were measured at Cape D’Aguilar, Hong Kong during the period of January 1994 to December1996 in order to understand the temporal variations of surface O₃ and CO in East Asia–West Pacific region. The isentropic backward trajectories were used to isolate different air masses reaching the site and to analyze the long-range transport and photochemical buildup of O₃ on a regional scale. The results show that the diurnal variation of surface O₃ was significant in all seasons with daily O₃ production being about 20 ppbv in fall and 10 ppbv in winter, indicating more active photochemical processes in the subtropical region. The distinct seasonal cycles of O₃ and CO were found with a summer minimum (16 ppbv)–fall maximum (41 ppbv) for O₃ and a summer minimum (116 ppbv)–winter maximum (489 ppbv) for CO. The isentropic backward trajectory cluster analyses suggest that the air masses (associated with regional characteristics) to the site can be categorized into five groups, which are governed by the movement of synoptic weather systems under the influence of the Asian monsoon. For marine-originated air masses (M-SW, M-SE and M-E, standing for marine-southwest, marine-southeast and marine-east, respectively) which always appear in summer and spring, the surface O₃ and CO have relatively lower mixing ratios (18, 16 and 30 ppbv for O₃, 127, 134 and 213 ppbv for CO), while the continental air masses (C-E and C-N, standing for continent-east and continent-north, respectively) usually arrive at the site in winter and fall seasons with higher O₃ (43 and 48 ppbv) and CO (286 and 329 ppbv). The 43 ppbv O₃ and 286 ppbv CO are representative of the regionally polluted continental outflow air mass due to the anthropogenic activity in East Asia, while 17 ppbv O₃ and 131 ppbv CO can be considered as the signature of the approximately clean marine background of South China Sea. The very high CO values (461–508 ppbv) during winter indicate that the long-range transport of air pollutants from China continent is important at the monitoring site. The fall maximum (35–46 ppbv) of surface O₃ was believed to be caused by the effects of the weak slowly moving high-pressure systems which underlie favorable photochemical production conditions and the long-range transport of aged air masses with higher O₃ and its precursors.     

Speciated particle dry deposition to the sea surface: results from ASEPS ’97

It has been postulated that atmospheric pathways may comprise a significant source of nitrogen for aquatic ecosystems and excess atmospheric deposition to coastal areas may be a major cause of eutrophication. Dry deposition of nitrogen containing particles is a potential, but poorly quantified pathway, for atmospheric nitrogen flux. This pathway is not well quantified because deposition velocities for particles are difficult to calculate and incorporate substantial uncertainties. Herein we employ an amended version of the Hummelshøj et al. (1992, Proceedings of the 5th International Conference on Precipitation Scavenging and Atmosphere–Surface Exchange Processes. AMS, Richland, Washington, USA, 12pp.) model to calculate size-segregated dry deposition of particle inorganic nitrogen compounds to the western Baltic during the late Spring of 1997 based on data collected as part of the Air–Sea Exchange Process Study (ASEPS). The results show that over a 15 d period in April and May dry deposition fluxes varied between 30 and 400 μg m^-2 d^-1 for nitrate and 1 and 120 μg m^-2 d^-1 for ammonium. Sensitivity analyses run to assess the potential bounds on actual dry deposition indicate that, for reasonable variation of model parameters and formulation, particle nitrogen dry deposition may be varied by up to an order of magnitude. The primary sources of uncertainty are identified and are discussed in the context of alternative model formulations.     

The evolution of photochemical smog in a power plant plume

The evolution of photochemical smog in a plant plume was investigated with the aid of an instrumented helicopter. Air samples were taken in the plume of the Cumberland Power Plant, located in central Tennessee, during the afternoon of 16 July 1995 as part of the Southern Oxidants Study – Nashville Middle Tennessee Ozone Study. Twelve cross-wind air sampling traverses were made at six distance groups from 35 to 116 km from the source. During the sampling period the winds were from the west–northwest and the plume drifted towards the city of Nashville TN. Ten of the traverses were made upwind of the city, where the power plant plume was isolated, and two traverses downwind of the city when the plumes were possibly mixed. The results revealed that even six hours after the release, excess ozone production was limited to the edges of the plume. Only when the plume was sufficiently dispersed, but still upwind of Nashville, was excess ozone (up to 109 ppbv, 50–60 ppbv above background levels) produced in the center of the plume. The concentrations image of the plume and a Lagrangian particle model suggests that portions of the power plant plume mixed with the urban plume. The mixed urban power plant plume began to regenerate O₃ that peaked at 120 ppbv at a short distance (15–25 km) downwind of Nashville. Ozone productivity (the ratio of excess O₃ to NO_y and NO_z) in the isolated plume was significantly lower compared with that found in the city plume. The production of nitrate, a chain termination product, was significantly higher in the power plant plume compared to the mixed plume, indicating shorter chain length of the photochemical smog chain reaction mechanism.     

Sulphate aerosol size distributions at Mumbai,India, during the INDOEX-FFP (1998)

Sulphate size distributions were measured at the coastal station of Mumbai (formerly Bombay) through 1998, during the Indian ocean experiment (INDOEX) first field phase (FFP), to fill current gaps in size-resolved aerosol chemical composition data. The paper examines meteorological, seasonal and source-contribution effects on sulphate aerosol and discusses potential effects of sulphate on regional climate. Sulphate size-distributions were largely trimodal with a condensation mode (mass median aerodynamic diameter or MMAD 0.6 μm), a droplet mode (MMAD 1.9–2.4 μm) and a coarse mode (MMAD 5 μm). Condensation mode sulphate mass-fractions were highest in winter, consistent with the high meteorological potential for gas-to-particle conversion along with low relative humidity (RH). The droplet mode concentrations and MMADs were larger in the pre-monsoon and winter than in monsoon, implying sulphate predominance in larger sized particles within this mode. In these seasons the high RH, and consequently greater aerosol water in the droplet mode, would favour aerosol-phase partitioning and reactions of SO₂. Coarse mode sulphate concentrations were lowest in the monsoon, when continental contribution to sulphate was low and washout was efficient. In winter and pre-monsoon, coarse mode sulphate concentrations were somewhat higher, likely from SO₂ gas-to-particle conversion. Low daytime sulphate concentrations with a large coarse fraction, along with largely onshore winds, indicated marine aerosol predominance. High nighttime sulphate concentrations and a coincident large fine fraction indicated contributions from anthropogenic/industrial sources or from gas-to-particle conversion. Monthly mean sulphate concentrations increased with increasing SO₂ concentrations, RH and easterly wind direction, indicating the importance of gas-to-particle conversion and industrial sources located to the east. Atmospheric chemistry effects on sulphate size distributions in Mumbai, indicated by this data, must be further examined.     

Trace gas variations at Cape Point,South Africa,during May 1997 following a regional biomass burning episode

During the continuous monitoring of atmospheric parameters at the station Cape Point (34°S, 18°E), a smoke plume originating from a controlled fire of 30-yr-old fynbos was observed on 6 May 1997. For this episode, which was associated with a nocturnal inversion and offshore airflow, atmospheric parameters (solar radiation and meteorological data) were considered and the levels of various trace gases compared with those measured at Cape Point in maritime air. Concentration maxima in the morning of 6 May for CO₂, CO, CH₄ and O₃ amounted to 370.3 ppm, 491 ppb, 1730 ppb and 47 ppb, respectively, whilst the mixing ratios of several halocarbons (F-11, F-12, F-113, CCl₄ and CH₃CCl₃) remained at background levels. In the case of CO, the maritime background level for this period was exceeded by a factor of 9.8. Differences in ozone levels of up to 5 ppb between air intakes at 4 and 30 m above the station (located at 230 m above sea level) indicated stratification of the air advected to Cape Point during the plume event. Aerosols within the smoke plume caused the signal of global solar radiation and UV–A to be attenuated from 52.4 to 13.0 mW cm⁻² and from 2.3 to 1.3 mW cm⁻², respectively, 5 h after the trace gases had reached their maxima. Emission ratios (ERs) calculated for CO and CH₄ relative to CO₂ mixing ratios amounted to 0.042 and 0.0040, respectively, representing one of the first results for fires involving fynbos. The CO ER is somewhat lower than those given in the literature for African savanna fires (average ER=0.048), whilst for CH₄ the ER falls within the range of ERs reported for the flaming (0.0030) and smouldering phases (0.0055) of savanna fires. Non-methane hydrocarbon (NMHC) data obtained from a grab sample collected during the plume event were compared to background levels. The highest ERs (ΔNMHC/ΔCH₄) have been obtained for the C₂–C₃ hydrocarbons (e.g. ethene at 229.3 ppt ppb⁻¹), whilst the C₄–C₇ hydrocarbons were characterised by the lowest ERs (e.g. n-hexane at 1.0 and n-pentane at 0.8 ppt ppb⁻¹).     

Aerosol mass-size distributions at a tropical coastal environment: response to mesoscale and synoptic processes

Regular measurements of total mass concentration and mass-size distribution of near-surface aerosols, made using a ten-channel Quartz Crystal Microbalance (qcm) Impactor for the period October 1998–December 1999 at the tropical coastal station Trivandrum (8.5°N, 77°E), are used to study the response of aerosol characteristics to regional mesoscale and synoptic processes. Results reveal that aerosol mass concentrations are generally higher under land breeze conditions. The sea breeze generally has a cleansing effect, depleting the aerosol loading. The continental air (LB regime) is richer in accumulation mode (submicron) aerosols than the marine air. On a synoptic scale, aerosol mass concentration in the submicron mode decreased from an average high value of ∼86 μg m⁻³ during the dry months (January–March) to ∼11 μg m⁻³ during the monsoon season (June–September). On the contrary mass concentration in the supermicron mode increased from a low value of ∼15 μg m⁻³ during the dry months to reach a comparatively high value of ∼35 μg m⁻³ during April, May. Correspondingly, the effective radius (R_eff) increased from a low value of 0.15–0.17 μm to ∼0.3 μm indicating a seasonal change in the size distribution. The mass-size distribution shows mainly three modes, a fine mode (∼0.1 μm); a large mode (∼0.5 μm) and a coarse mode (∼3 μm). The fine mode dominates in winter. In summer the large mode becomes more conspicuous and the coarse mode builds up. The fine mode is highly reduced in monsoon and the large and coarse modes continue to remain high (replenished) so that their relative dominance increases. The size distribution tends to revert to the winter pattern in the post-monsoon season. Accumulation (submicron) aerosols account for ∼98% of the total surface area and ∼70% of the total volume of aerosols during winter. During monsoon, even though they still account for ∼90% of the area, their contribution to the volume is reduced to ∼50%; the coarse aerosols account for the rest.     

Vertical profiles of ultrafine to supermicron particles measured by aircraft over Osaka metropolitan area in Japan

Intensive aircraft- and ground-based measurements of ultrafine to supermicron particles in the Osaka metropolitan area, Japan, were carried out on 17–19 March 2003, in order to investigate vertical profiles of size-resolved particles in the urban atmosphere. Differently sized particles were observed at different altitudes on 19 March. Relatively higher concentrations of ultrafine particles (31 nm) and submicron particles (0.3–0.5 μm) were measured (100–200 cm⁻³) at altitudes of 300 and 600 m, whereas supermicron particles (2–5 μm) were present (300–600 cm⁻³) at higher altitudes (1300 m in the morning and 2200 m in the afternoon). The chemical composition analysis showed that supermicron particles evidently comprised mainly soil particles mixed internally with anthropogenic species such as carbonaceous components and sulfate. Numerical simulation using the Chemical weather FORecasting System (CFORS) suggested the long-range transport of soil dust and black carbon from the Asian continent. Total number concentrations of particles sized 10–875 nm ranged from 4.8×10³ to 3.0×10⁴ cm⁻³ at an altitude of 300 m and from 7.3×10² to 4.8×10³ cm⁻³ at an altitude of 1300 m. Total number concentrations of particles sized 10–875 nm correlated very well with NO_X concentrations, and, therefore, ultrafine and submicron particles were likely emitted from urban activities such as car traffic and vertically transported. Number size distributions at lower altitudes obtained by aircraft measurements were similar to those obtained by ground measurements, with modal diameters of 20–30 nm on 18 March and about 50 nm on 19 March.