Investigation of a 1000 MW smoke plume by means of a 1.064 μm lidar—I. Lidar calibration procedure from in situ aerosol measurements and vertical lidar shots

From airborne measurements on various days, average size distributions of natural aerosol particles for different heights were obtained at our rural experimental site. Using different aerosol refractive indices and a mean particle size distribution, the backscattering and extinction coefficients β and α were computed for a 1.064 μm wavelength. Assuming the mean refractive index of the aerosol particles over a rural site as equal to 1.5−0.005 i and taking into account size and concentration distributionsof aerosol particles with height, a vertical profile of atmospheric returns from the 1.064 μm laser radiation from the ground has been computed as characteristic of the site.From numerous lidar shots on various days, an average vertical profile of lidar returns was also obtained as characteristic of both the experimental site and the whole lidar system using a laser wavelength of 1.064 μm. The relationship between the atmospheric returns and lidar signals could then be set up and used as the calibration function of the lidar. In this way, distributionsof particle concentration could be monitored from lidar shots.     

Is the size distribution of urban aerosols determined by thermodynamic equilibrium?: An application to Southern California

A size-resolved equilibrium model, SELIQUID, is presented and used to simulate the size–composition distribution of semi-volatile inorganic aerosol in an urban environment. The model uses the efflorescence branch of aerosol behavior to predict the equilibrium partitioning of the aerosol components between the gas phase and a size-resolved aerosol population over the entire RH domain. Predictions of SELIQUID are compared against size-resolved composition measurements at different locations during the Southern California Air Quality Study. Based on the modeling results, the size distribution of sub-micrometer nitrate and ammonium can be determined by thermodynamic equilibrium when the RH>60%. In cases where the RH<60%, the assumption that all aerosol particles are metastable liquid solutions may introduce unacceptable errors. On the other hand, the equilibrium assumption, in some cases at least, introduces errors in the calculation of the coarse (particles with diameter >1 μm or so) nitrate and ammonium that increase with particle size. Finally, the inclusion of crustal species is important in modeling the size distribution of coarse inorganic aerosols when the concentration of these species is high. The effect of these crustal species can be complex and counterintuitive.     

On the relation between the size and chemical composition of aerosol particles and their optical properties

The light scattering and absorption coefficients of fine atmospheric aerosol particles were recorded in Hungary under rural conditions in 1998–1999 by an integrating nephelometer and particle soot absorption photometer, respectively. In some cases optical properties in the fine size range were compared to those in the coarse particles. Results obtained indicate, as expected, that fine particles control the scattering and absorption caused by the aerosol. In 1999 the size distribution of aerosol particles was also monitored by means of an electric low pressure impactor (ELPI). This makes it possible the study of the relationship between the number, surface and mass concentration in the size range of 0.1–1.0 μm and the optical characteristics by also considering the chemical composition of the particles.     

Public Relations Handbook

A major difficulty encountered in laboratory research on the atmospheric interaction of an aerosol-gas system is the unstable nature of the aerosol phase. Previously reported aerosol stabilizing techniques often severely alter the aerosol so that laboratory results cannot be validly extrapolated to the atmospheric environment. A new technique which does not alter the nature of the aerosol is described in this paper.

Aerosol particles are deposited on an inert substrate such as Teflon beads. The deposition is carried out in a fluidized-bed to ensure discrete aerosol deposition and to achieve a uniform distribution of aerosol concentration on the supporting beads. Aerosol-gas interactions can be investigated conveniently by exposing these stabilized aerosols to the reacting gases in dynamic or static systems. Laboratory results obtained by using stabilized aerosols may be extrapolated to the atmospheric environment.

This aerosol stabilizing technique was incorporated into an investigation of the particulate-catalyzed atmospheric oxidation of sulfur dioxide. Teflon beads with deposited aerosol particles of CuCl₂, MnCl₂, and NaCI were exposed to 4–42 ppm of sulfur dioxide in a plug flow reactor. The rate of oxidation of sulfur dioxide was found to be influenced by type of catalyst, concentration of catalyst, relative humidity and concentration of sulfur dioxide. The rate of oxidation by sodium chloride particulate was measurable at low to moderate relative humidities (45–60%), but the rate was several times higher when the sodium chloride catalyst particles change from solid form into droplet form at high relative humidities (>80%).     

Dynamic Calibration of an Acid Aerosol Analyzer

A method is described for dynamic calibration of an acid aerosol analyzer based on a commercial modification of the Thomas Autometer and manufactured by the Instrument Development Company. This automated instrument removes acid aerosol from an air stream by sonic impaction, and the sulfuric acid collected is determined conductometrically. An all-glass aerosol generator based on the reaction of water vapor with sulfur trioxide vapor released from fuming sulfuric acid was built for the calibration. Air samples were withdrawn for instrument calibration before and after the concentration of the acid aerosol was determined by titration. The apparent particle size as determined by an Andersen sampler ranged from 2.0 microns to less than 0.68 micron and exhibited a sharp peak with mass median diameter at 1.3 microns in the distribution curve. The size of the aerosol, within certain limits, could be controlled by humidity. Data indicated a linear response with an aerosol collection efficiency of 80 percent in the important respirable size range.     

The Mass Distribution of Large Atmospheric Particles

This paper describes the results of a study to determine the total mass and the mass distribution of atmospheric aerosols, especially that mass associated with particles greater than 10 μm diameter. This study also determined what fraction of the total aerosol mass a standard high-volume air sampler collects and what fraction and size interval settle out on a dust fall plate. A special aerosol sampling system was designed for this study to obtain representative samples of large airborne particles. A suburban sampling site was selected because no local point sources of aerosols existed nearby. Samples were collected under various conditions of wind velocity and direction to obtain measurements on different types of aerosols.

Study measurements show that atmospheric particulate matter has a bimodal mass distribution. Mass associated with large particles mainly ranged from 5 to 100 μm in size, while mass associated with small particles ranged from an estimated 0.03 to 5 μm in size. Combined, these two distributions produced a bimodal mass distribution with a minimum around 5 μm diameter. The high-volume air sampler was found to collect most of the total aerosol mass, not just that fraction normally considered suspended particulate. Dust fall plates did not provide a good or very useful measure of total aerosol mass. The two fundamental processes of aerosol formation, condensation and dispersion appear to account for the formation of a bimodal mass distribution in both natural and anthropogenic aerosols. Particle size distribution measurements frequently are in error because representative samples of large airborne particles are not obtained. Considering this descrepancy, air pollution regulations should specify or be based upon an upper particle size limit.     

Electrical Measurement of the Mass Concentration of a Self-Preserving Aerosol Size Distribution

Recently fifty-eight measurements of urban aerosol size distributions by Clark have shown that these distributions agree quite well with the self preserving form proposed by Friedlander within the size range of 0.05 to 5 microns radius. This paper shows that for an aerosol obeying the self preserving distribution model, the volume concentration (and, hence, the mass concentration for constant density) is directly proportional to the electric current collected when the aerosol is unipolarly charged, passed through a weak electric field to remove particles smaller than 0.05 micron and then collected by a current collector. It is shown that the linear relation between the mass concentration and collected current is independent of the unipolar charging method used. A test of this theory using Clark’s electric counter data was encouraging and suggests that the electric measurement of urban aerosol mass concentrations by properly designed instruments may be feasible.     

Size resolved chemical mass balance of aerosol particles over rural Hungary

The mass size distribution of atmospheric aerosol particles was determined by means of an electric low pressure impactor (ELPI) in rural air in Hungary. The particles captured on different stages of the impactor were chemically analyzed by capillary zone electrophoresis to quantify ionic components as well as by catalytic combustion method to detect total carbon in the samples. The results show that fine aerosol consists mainly of ammonium sulfate and organic carbon. These two species have rather different size distributions since very small particles are composed almost of carbon compounds. The analysis of fine aerosol samples collected simultaneously on filters indicates that an important part of organics is soluble in water. The mass balance of fine particles as a function of their size is estimated by taking into account the liquid water adsorbed by ammonium sulfate and by converting the mass of carbon to the mass of carbon compounds. Finally, the size resolved mass balance of fine aerosol particles is presented and discussed as a function of the origin of air masses.     

Experimental analysis of particle concentration heterogeneity in a ventilated scale chamber

The mixing processes of the aerosol particles from an outdoor environment in a ventilated scale chamber were experimentally studied. The particles were classified into five groups by size: 0.3–0.5 μm, 0.5–1.0 μm, 1.0–3.0 μm, 3.0–5.0 μm and 5.0–10.0 μm. The developing process for the concentration of each particle group was measured in different kinds of flow fields.The results show that the flow field configuration can effectively influence the dispersion time rate of the particles at certain positions. The increase in particle diameter can decrease the dispersion time rate. When the gas flow velocity is high, the particle dispersion time rate is independent of particle size; but when the gas flow velocity is low, particle size can significantly affect the particle dispersion time rate because the turbulent diffusion becomes important in the air and particle transport. The uniformity of the particle concentration for certain positions in steady state tends to be controlled by the inflow velocity, flow field configuration and the particle diameters.     

Simultaneous measurement of light-scattering properties and particle size distribution for aerosols: Application to ammonium sulfate and quartz aerosol particles

An apparatus for measuring the scattering phase function and linear polarization of aerosol particles has been developed. The apparatus uses an elliptical mirror and CCD camera to image the full angular scattering range simultaneously. An in-line aerodynamic particle sizer (APS) in the particle flow stream provides for the simultaneous measurement of the aerosol particle size distribution. This apparatus allows for a comparison of measured optical properties with theoretical model calculations based on the measured aerosol size distribution. The system was calibrated and tested using monodisperse polystyrene latex (PSL) spheres and with ammonium sulfate (AS) aerosol. We have also used the apparatus for measuring the scattering phase function and linear polarization for light scattering from irregular quartz aerosol particles. Our results show that Mie theory substantially overestimates the backscattering cross-section for quartz particles in the size parameter range X∼2–4, in agreement with previous experimental work and theoretical modeling studies. We also present a normalized synthetic phase function for quartz dust aerosol in the accumulation mode size range (0.1–2.0 μm).     

Roadside aerosol study using hygroscopic,organic and volatility TDMAs: Characterization and mixing state

Traffic-related aerosol particles are ubiquitous in the urban atmosphere. As they are produced at ground level, they can also cause adverse health effects to urban dwellers. However, knowledge of the formation, transformation and chemically resolved size distribution of urban ultrafine particles is incomplete. Thus, more of these measurements are needed for better assessment of ambient air quality and its potential health effects. The particle number concentration, aerosol black carbon (BC) concentration and size distribution of traffic-related aerosols were measured near two major roads in Kuopio, Finland, from 16 June to 5 July, 2004. Furthermore, the properties of roadside aerosol particles were examined with the Tandem Differential Mobility Analyzer technique (TDMA). A suite of TDMA instruments relying on water (hygroscopic TDMA) and ethanol (organic TDMA) condensation as well as heating (volatility TDMA) were deployed to study the composition of the nucleation and Aitken mode particles (D_p = 10–50 nm) formed from vehicle exhaust. The results show that a simple three-component model was able to reproduce characteristic insoluble, organic and water-soluble volume fractions. Insoluble constituents were dominant in the Aitken mode particles, whereas organic compounds dominated the nucleation mode sizes. On average, only a small volume fraction was water-soluble, but a clear external mixing was observed particularly when enough time was allowed after the tail pipe emissions. The contribution of the insoluble material was seen to increase as a function of particle size, being typically less than 10% at 10 nm and between 20 and 50% at 50 nm, in contrast to the organic fraction, which decreased from about 80% at nucleation mode size range to 50–60% at 50 nm.     

Predominance of soot-mode ultrafine particles in Santiago de Chile: Possible sources

A monitoring campaign was performed in Santiago de Chile during a winter month of 2003 and 2006 (July) using several instruments to measure the size distribution of particulate material. For the first time, the size distribution of ultrafine particles was measured in Santiago, and an estimation of its sources was done by analyzing its temporal variation. The study was performed in three sites; one of them is located in the eastern part of Santiago, a sector with low particle concentration and about 100 m from a busy street. The other site is located in the western part, which is the sector that has the highest concentration of fine and coarse particle matter during winter, also located far from a street. The third site is located within 5 m from the busiest street in Santiago. In all stations traffic is the dominating source for fine and ultrafine particles and the size distribution is peaked towards 60–100 nm (soot mode). Only in the site near the street, it is possible to see a clear peak towards smaller sizes (10–30 nm). The size distribution measurements presented here indicate that aerosol dynamics play a more important role for the Santiago case as compared to cleaner cities in Europe. Changes in the particle size during different hours of the day reflect both variations in meteorological mixing conditions as well as effects of aerosol dynamic processes such as coagulation, condensation and dry deposition. A relative increase in the number of the larger ultrafine particles (d ≥ 70 nm), as compared to the number of smaller particles (d < 70 nm) correlated with wind speed is an indication of pollution transport with aged particles from other parts of the city.     

Design and Operating Parameters for a Large Ambient Aerosol Chamber

Recent investigations of ambient aerosol behavior over urban areas have pointed out the need for controlled experimental data to link together field investigation results and computer simulation studies. This paper describes the design considerations, construction details and operating parameters of a large (8000 ft³) outside reaction chamber constructed in rural North Carolina. The chamber is triangular in cross-section, 20 ft wide, 20 ft high and 40 ft long, and is covered with clear 5 ml Teflon film. The outdoor location of the chamber permits the reaction volume to be exposed to the natural conditions of temperature and solar radiation. A recirculating air system allows the air in the chamber to be passed through an “absolute” fiberglas filter for adjustment of condensation nuclei concentration and also through driers for humidity adjustment. Internal fans are provided for mixing of the chamber contents without use of the recirculating system so that various degrees of turbulence can be approximated. A sampling line from the chamber passes directly to an instrument room, located directly under the chamber, where direct analyses for particle composition, concentration, and size, and gas composition and concentration are carried out. Parameters which can be varied in this system include number, size, distribution, and chemical composition of pre-existing nuclei, as well as humidity, solar radiation, temperature, and trace gas concentration and composition.     

Use of two different acidic aerosol samplers to measure acidic aerosols in Hsinchu, Taiwan

Acidic aerosol concentrations measured by an annular denuder system (ADS) and a honeycomb denuder system (HDS) in Hsinchu, Taiwan, were compared. Aerosols were also sampled by a MOUDI (micro-orifice uniform deposit impactor) and analyzed by an ion chromatograph to determine the size distributions of different species. Using the measured aerosol size distribution, theoretical analysis showed that positive HNO3 artifact due to volatilization of NH4NO3 is generally negligible for both samplers. Comparing two different denuder samplers, the average concentration of HNO3 measured by the ADS was found to be lower than that measured by the HDS, while the difference between the two samplers for the average concentration of other species was found to be within +/- 15%. A possible cause of the difference in HNO3 concentrations is due to a greater loss of HNO3 in the cyclone used by the ADS than in the impactor used by the HDS. The study also showed incomplete absorption of the evaporated HCl and HNO3 from the particles on the Teflon filter by the first nylon filter in the filter pack of the ADS. Collection efficiency and capacity of HCl and HNO3 by the nylon filters need further investigation.     

Retrieval of the aerosol size distribution in the complex anomalous diffraction approximation

This contribution reports some recently achieved results in aerosol size distribution retrieval in the complex anomalous diffraction approximation (ADA) to MIE scattering theory. This approximation is valid for spherical particles that are large compared to the wavelength and have a refractive index close to 1.The ADA kernel is compared with the exact MIE kernel. Despite being a simple approximation, the ADA seems to have some practical value for the retrieval of the larger modes of tropospheric and lower stratospheric aerosols.The ADA has the advantage over MIE theory that an analytic inversion of the associated Fredholm integral equation becomes possible. In addition, spectral inversion in the ADA can be formulated as a well-posed problem. In this way, a new inverse formula was obtained, which allows the direct computation of the size distribution as an integral over the spectral extinction function. This formula is valid for particles that both scatter and absorb light and it also takes the spectral dispersion of the refractive index into account.Some details of the numerical implementation of the inverse formula are illustrated using a modified gamma test distribution. Special attention is given to the integration of spectrally truncated discrete extinction data with errors.     

Technique for Measuring Dust Collector Efficiency As a Function of Particle Size

With a specially designed generator, producing an aerosol of concentration, chemical composition, and size distribution similar to incinerator aerosols, a scrubber was tested in the laboratory by sampling before and after the collector. Using an Andersen Sampler as a 7 stage cascade impactor the efficiency for 7 different size classes was determined. This technique provides a rapid and simple method for evaluating the performance of a collector as a function of particle size. The multistage impaction classifies the particles according to their aerodynamic behavior. Gravimetric analysis of each stage eliminates the need for tedious counting and sizing.     

Size distribution of polycyclic aromatic hydrocarbons in urban and suburban sites of Beijing, China

PAHs in five-stage size segregated aerosol particles were investigated in 2003 at urban and suburban sites of Beijing. The total concentration of 17 PAHs ranged between 0.84 and 152 ng m(-3), with an average of 116 ng m(-3), in urban area were 1.1-6.6 times higher than those measured in suburban area. It suggested a serious pollution level of PAHs in Beijing. PAHs concentrations increased with decreasing the ambient temperature. Approximately 68.4-84.7% of PAHs were adsorbed on particles having aerodynamic diameter 2.0 microm. Nearly bimodal distribution was found for PAHs with two and three rings, more than four rings PAHs, however, followed unimodal distribution. The overall mass median diameter (MMD) for PAHs decreased with increasing molecular weight. Diagnostic ratios and normalized distribution of PAHs indicated that the PAHs in aerosol particles were mainly derived from fossil fuel combustion. Coal combustion for domestic heating was probably major contributor to the higher PAHs loading in winter, whereas PAHs in other seasons displayed characteristic of mixed source of gasoline and diesel vehicle exhaust. Biomass burning and road dust are minor contributors to the PAHs composition of these aerosol particles. Except for source emission, other factors, such as meteorological condition, photochemical decay, and transportation from source to the receptor site, should to be involved in the generation of the observed patterns.     

Monitoring of sources and atmospheric processes controlling air quality in an urban Mediterranean environment

Different monitoring parameters (PM mass concentrations, number–size distribution, black carbon, gaseous pollutants, and chemical composition, among others) are currently used in air quality studies. Urban aerosols are the result of several sources and atmospheric processes, which suggests that a single monitoring technique is insufficient to quantitatively evaluate all of them.This study assesses the suitability of a number of monitoring techniques (PM mass concentrations, number and size distribution of ultra-fine particles, levels of gaseous pollutants, and a complete chemical characterization of PM₁₀ and PM_2.5) by examining the response of those techniques to the different emission sources and/or atmospheric processes affecting an urban Mediterranean area (Barcelona, NE Spain).The results of this work reveal that the PM mass, the number concentration and the chemical composition give different, but complementary, information. Whereas the mineral matter, a key atmospheric aerosol component across the Mediterranean, is not properly quantitatively assessed by measuring sub-micrometric particles, the monitoring of the number concentration is indispensable to interpret the origin of specific aerosol episodes. Furthermore, the chemical composition yields very relevant information to deduce the causes of specific pollution episodes.The number concentration of ultra-fine particles in urban areas is strongly dependent upon vehicle exhaust emissions, which may cause adverse health impacts. Moreover, urban Mediterranean environments are favourable to produce nucleation-mode particles (<20 nm) with photochemical origin. In those cases, these particles are expected to be of high solubility and consequently their toxicity may differ from that of traffic-generated ultra-fine particles. Thus, the use of a single monitoring parameter to evaluate the health effects seems to be not enough.     

The size distribution of marine atmospheric aerosol with regard to primary biological aerosol particles over the South Atlantic Ocean

The marine atmosphere is characterized by particles which originate from the ocean and by those which reached the air by advection from the continent. The bubble-burst mechanism produces both sea salt as well as biological particles. The following article describes the determination of the size distribution of marine aerosol particles with special emphasis on the biological particles. Th data were obtained on three cruises with the German Research Vessel “METEOR” crossing the South Atlantic Ocean. The measurements showed that biological particles amount to 17% in number and 10% in volume concentration. Another type of particle became obvious in the marine atmosphere, the biologically contaminated particle, i.e. particles which consist partly (approximately up to one-third) of biological matter. Their concentration in the evaluated size class (r>2 μm) is higher than the concentration of the pure biological particles. The concentrations vary over about one to two orders of magnitude during all cruises.     

A Simplified Aerosol Coagulation Model

A simplified aerosol coagulation model has been developed, to determine the mutual coagulation of many discrete size classes. The model has been applied to computation of the growth of light scattering particles from a small monodisperse aerosol, and prediction of aerosol size and concentration downwind of sources. These computations are in good agreement with field observations. This model is sufficiently simplified to allow programming In contemporary desk calculators and is an extremely practical tool for application of aerosol technology to air pollution problems.