Source apportionment of surfactants in marine aerosols at different locations along the Malacca Straits

This study aims to determine the source apportionment of surfactants in marine aerosols at two selected stations along the Malacca Straits. The aerosol samples were collected using a high volume sampler equipped with an impactor to separate coarse- and fine-mode aerosols. The concentrations of surfactants, as methylene blue active substance and disulphine blue active substance, were analysed using colorimetric method. Ion chromatography was employed to determine the ionic compositions. Principal component analysis combined with multiple linear regression was used to identify and quantify the sources of atmospheric surfactants. The results showed that the surfactants in tropical coastal environments are actively generated from natural and anthropogenic origins. Sea spray (generated from sea-surface microlayers) was found to be a major contributor to surfactants in both aerosol sizes. Meanwhile, the anthropogenic sources (motor vehicles/biomass burning) were predominant contributors to atmospheric surfactants in fine-mode aerosols.     

Characteristics of aerosol types from AERONET sunphotometer measurements

By using observations from the Aerosol Robotic Network (AERONET), aerosol types are classified according to dominant size mode and radiation absorptivity as determined by fine-mode fraction (FMF) and single-scattering albedo (SSA), respectively. The aerosol type from anthropogenic sources is significantly different with regard to location and season, while dust aerosol is observed persistently over North Africa and the Arabian Peninsula. For four reference locations where different aerosol types are observed, time series and optical properties for each aerosol type are investigated. The results show that aerosol types are strongly affected by their sources and partly affected by relative humidity. The analysis and methodology of this study can be used to compare aerosol classification results from satellite and chemical transport models, as well as to analyze aerosol characteristics on a global scale over land for which satellite observations need to be improved.     

The Evolution of Visibility Deterioration and Aerosol Spectra in the St. Louis Urban Plume

Under the auspices of Project METROMEX, studies of visibility de-teoration downwind of St. Louis were conducted during July-August 1974-1975. Estimates of horizontal visual range, standard meteorological data, and aerosol characteristics within the mixing layer were acquired upwind, over, and downwind of the metropolitan area by means of airborne transects. Aerosol number, surface, and volume distributions for particles between 0.025-2.5 µm were generated from the airborne measurement of Aitken nucleus concentrations, cloud condensation nuclei, and aerosols detected in situ with optical probes. Visibility reduction amounting to 50% of prevailing regional upwind visibilities consistently occurs at a distance corresponding to 2-3 hours travel time downwind for an air parcel moving with the mean transport wind. The regions of visibility minimum do not coincide with locations of maximum Aitken nucleus concentrations, but rather correspond in space and time to increased values of cloud condensation nuclei and increased numbers of particles in the 0.1-2.5 µm diameter range. Comparisons of observed aerosol evolution with similar laboratory studies suggest that most of the light scattering aerosols are of secondary origin.     

Seasonal variability of aerosol optical properties over Beijing

The knowledge of aerosol properties at local and regional scale is important in understanding of the global climate change. In this study, the aerosol optical properties over Beijing have been presented from the Aerosol Robotic Network (AERONET) measurements during 2002–2007. The aerosol optical depth (AOD) showed a distinct seasonal variation with high values in spring (March–May) and summer (June–August). The magnitude of Ångström exponent (α) was found to be relatively high throughout the year and the highest values (1.27) occurred in summer and the lowest (1.0) in spring. The water vapor retrieved from AERONET was found to be highest (2.60 cm) in summer. The fine modes of aerosol volume size distributions showed the highest peak around radius 0.15 μm in spring, autumn (September–November) and winter (December–February), and radius 0.19 μm in summer. The coarse modes showed the maxima peak at radius 3.0 μm in all seasons. The asymmetry factor (g) has considered as 0.65 at 440, 675, 870 and 1020 nm over Beijing in climate and radiation models. The average values of the single scattering albedo (SSA) at the four wavelengths were taken as 0.89, 0.91, 0.87 and 0.86 in spring, summer, autumn and winter, respectively. Both real and imaginary parts of the refractive index showed low wavelength dependence. The highest averages of real (1.52) and imaginary parts (0.0165) were found in spring and winter respectively in the wavelength range of 440–1020 nm. The aerosol properties over Beijing were found to highly dependent on season, and changes in aerosol properties were mainly attributed to the presence of dust as the main component during the spring season and the dominance of anthropogenic pollutants during the winter season.     

Radiative effects of aerosols over Indo-Gangetic plain: environmental (urban vs. rural) and seasonal variations

Aerosol radiative effects over two environmentally distinct locations, Kanpur (urban site) and Gandhi College (rural location) in the Indo-Gangetic plain (IGP), a regional aerosol hot spot, utilizing the measured optical and physical characteristics of aerosols, an aerosol optical properties model and a radiative transfer model, are examined. Shortwave aerosol radiative forcing (ARF) at the top of the atmosphere (TOA) is 30 W m(?-?2)). Shortwave atmospheric heating due to aerosols is >0.4 K/day over IGP and peaks during premonsoon at >0.6 K/day due to lower single scattering albedo (SSA) and higher surface albedo. TOA forcing is always less negative over Kanpur when compared to Gandhi College due to lower surface albedo except in postmonsoon owing to higher SSA. This happens as TOA forcing depends on SSA and surface albedo in addition to aerosol optical depth. The magnitude of longwave forcing and atmospheric cooling in an absolute sense is significantly small and contributes only about 20% or less to the net (shortwave + longwave) forcing. Aerosol radiative effects over these two locations, despite differences in aerosol characteristics, are similar, thus confirming that aerosols and their radiative influence get transported due to circulation. ARF over Kanpur and Gandhi College is an order of magnitude higher when compared to greenhouse gas forcing. A large reduction in surface reaching solar irradiance accompanied by large atmospheric warming can have implications on precipitation and hydrological cycle, and these aerosol radiative effects should be included while performing regional-scale aerosol climate assessments.     

Optical and chemical properties of marine boundary-layer aerosol around Japan determined from shipboard measurements in 2002

Shipboard measurements of the optical and chemical properties of marine boundary-layer aerosol were made around Japan over the period from 28 August to 25 September 2002. Measurements were conducted aboard the Research Vessel (R/V) Shirase along cruise tracks beginning from Yokosuka, and proceeding on to Hakodate, Sakata, Sasebo, Naha, Kure, and Yokkaichi. This paper describes the results of optical measurements using an Optical Particle Counter (OPC), an Integrating Nephelometer (IN), and a Particle Soot/Absorption Photometer (PSAP), as well as chemical analyses of water-soluble aerosol particles collected by impactor and filter systems. Coulter Multisizer measurements were used for water-insoluble aerosol particles. The complex refractive index (CRI), scattering and absorption coefficients, and size distribution of aerosols were estimated from combined measurements made using OPC, IN, and PSAP. Contrasting aerosol characteristics were observed during different stages of the cruise. Discussion on these differences focuses mainly on two legs: Leg-1 from Yokosuka to Hakodate and Leg-4 from Sasebo to Naha. Backward trajectory analyses indicate that the air sampled during Leg-1 originated from the Pacific Ocean, whereas the air sampled during Leg-4 originated from the Chinese Continent via the Korean Peninsula. For the first half of Leg-1, the number concentration was low and larger particles were relatively predominant. The real and imaginary parts of the CRI were estimated to be 1.38–1.40 and close to zero, respectively. This estimation is consistent with the results of chemical analyses, which show that the sea salt is rich in aerosols sourced from remote ocean areas. In contrast, small particles were predominant during Leg-4, and the real and imaginary parts of the CRI were estimated to be 1.52–1.59 and approximately −0.002, respectively. These findings are also consistent with chemical analyses that reveal a mixture of mineral dust and sulfate aerosol likely transported from China and Korea. The Coulter Multisizer measurements conducted during Leg-4 reveal abundant water-insoluble particles with a mode radius of 1.35 μm.     

Effect of Roadbed Configuration on Traffic Derived Aerosols

Aerosols present upwind and downwind of freeways in the Los Angeles Basin were collected in five particle size ranges by Lundgren impactors with after filters and analyzed for elemental content by ion-excited x-ray emission. The contribution of freeway traffic to total airborne particulate load was obtained by subtracting the local background, measured by an upwind sampler, from the values obtained by downwind samplers on a size by size, element by element basis. This contribution correlated reasonably well with estimates derived from automotive and roadbed expendable rates. Traffic-derived aerosols, normalized to vehicular flow, were considerably lower in mass downwind of depressed roadbed configurations than either at grade or raised configurations. A line source model, combined with literature values for emitted lead, produced good agreement with results obtained in the at grade configuration.     

Plants Pollute Air

A recently developed photometer utilizes near-forward scattered light to count and size aerosol particles in the diameter range 0.3-17 μ. The particles are drawn through a 1-cu mm illuminated volume without entering the body of the optical chamber. Hence, purging is almost instantaneous, and number concentrations below 1,000,000/cu ft give less than 3% coincidences. The scattered light pulse from each particle is detected by a photomultiplier tube. The resultant voltage pulses are amplified, measured by a series of ten discriminator circuits, and stored in a series of ten 5-decade electronic counters. At the end of a chosen period ranging from 1/3 to 30 min, a digital printer prints the number of particles at each diameter. At the end of the printout, the procedure automatically recycles. The instrument provides ten size classifications, each successively having a width ratio of 1.5 to 1. Greater precision is seldom practical since most aerosols contain particles of different refractive index, color, and shape, all of which affect the intensity of the scattered light. Calibration is accomplished with aerosols of uniform size such as spray-dried polystyrene and other latex suspensions, supplemented by calculations based on the Mie theory of light scattering.     

Sensitivity of shortwave radiative fluxes to the vertical distribution of aerosol single scattering albedo in the presence of a desert dust layer

The aim of this work is to quantify the sensitivity of shortwave radiative fluxes to changes in the vertical distribution of aerosol absorption, taken into account through the aerosol Single Scattering Albedo (SSA). The case study represents a real atmospheric situation with a desert dust layer (DDL) in the mid troposphere over an urban Boundary Layer (BL) observed at Rome on 20 June 2007. A moderately high aerosol optical depth (AOD), 0.292 at 550 nm, and low Ångström exponent of 0.30 were measured. The observed case was reconstructed with a radiative transfer model, in which the SSA of the boundary layer aerosols was varied from that of a highly absorbing aerosol type (urban) to a highly scattering one (clear marine). The SSA of the DDL is determined keeping fixed the measured SSA of the whole atmospheric column. The simulations show notable changes in the surface and top of the atmosphere (TOA) diffuse fluxes depending on the boundary layer aerosol properties. The aerosol radiative forcing (ARF) at the surface changes by 6–19 W m^?2, depending on the solar zenith angle, when urban or clean marine particles are included in the boundary layer. The ARF differences observed at TOA are between 1 and 5 W m^?2 when urban and clean marine aerosol types in the BL are respectively used, showing a smaller dependency on the solar zenith angle than at the surface.     

Optical measurements of aerosol size distributions in Great Smoky Mountains National Park: dry aerosol characterization

Aerosol size distributions were measured during the summertime 1995 Southeastern Aerosol and Visibility Study (SEAVS) in Great Smoky Mountains National Park using an Active Scattering Aerosol Spectrometer (ASASP-X) optical particle counter. We present an overview of the experimental method, our data inversion technique, timelines of the size distribution parameters, and calculations of dry accumulation mode aerosol density and refractive index. Aerosol size distributions were recorded during daylight hours for aerosol in the size range 0.1 < Dp < 2.5 microns. The particle refractive index used for the data inversion was calculated with the partial molar refractive index approach using 12-hr measured aerosol chemical composition. Aerosol accumulation mode volume concentrations ranging from 1 to 26 micron 3 cm-3 were observed, with an average of 7 +/- 5 micron 3 cm-3. The study average dry accumulation mode geometric volume median diameter was 0.27 +/- 0.03 micron, and the mean geometric standard deviation was 1.45 +/- 0.06. Using an internally mixed aerosol model, and assuming chemical homogeneity across the measured particle distribution, an average accumulation mode dry sulfate ion mass scattering efficiency of 3.8 +/- 0.6 m2 g-1 was calculated.     

Extensive aerosol optical properties and aerosol mass related measurements during TRAMP/TexAQS 2006 – Implications for PM compliance and planning

Extensive aerosol optical properties, particle size distributions, and Aerodyne quadrupole aerosol mass spectrometer measurements collected during TRAMP/TexAQS 2006 were examined in light of collocated meteorological and chemical measurements. Much of the evident variability in the observed aerosol-related air quality is due to changing synoptic meteorological situations that direct emissions from various sources to the TRAMP site near the center of the Houston-Galveston-Brazoria (HGB) metropolitan area. In this study, five distinct long-term periods have been identified. During each of these periods, observed aerosol properties have implications that are of interest to environmental quality management agencies. During three of the periods, long range transport (LRT), both intra-continental and intercontinental, appears to have played an important role in producing the observed aerosol. During late August 2006, southerly winds brought super-micron Saharan dust and sea salt to the HGB area, adding mass to fine particulate matter (PM_2.5) measurements, but apparently not affecting secondary particle growth or gas-phase air pollution. A second type of LRT was associated with northerly winds in early September 2006 and with increased ozone and sub-micron particulate matter in the HGB area. Later in the study, LRT of emissions from wildfires appeared to increase the abundance of absorbing aerosols (and carbon monoxide and other chemical tracers) in the HGB area. However, the greatest impacts on Houston PM_2.5 air quality are caused by periods with low-wind-speed sea breeze circulation or winds that directly transport pollutants from major industrial areas, i.e., the Houston Ship Channel, into the city center.     

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.     

Estimates of Particle Hygroscopicity during the Southeastern Aerosol and Visibility Study

ABSTRACT

Aerosol water content was determined from relative humidity controlled optical particle counter (ASASP-X) size distribution measurements made during the Southeastern Aerosol and Visibility Study (SEAVS) in the Great Smoky Mountains National Park during summer 1995. Since the scattering response function of the ASASP-X is sensitive to particle refractive index, a technique for calibrating the ASASP-X for any real refractive index was developed. A new iterative process was employed to calculate water mass concentration and wet refractive index as functions of relative humidity. Experimental water mass concentrations were compared to theoretically predicted values assuming only ammonium sulfate compounds were hygroscopic. These comparisons agreed within experimental uncertainty. Estimates of particle hygroscopicity using a rural aerosol model of refractive index as a function of relative humidity demonstrated no significant differences from those made with daily varying refractive index estimates. Although aerosol size parameters were affected by the assumed chemical composition, forming ratios of these parameters nearly canceled these effects.     

Experimental Verification of Diffusion Battery Theory

The diffusion battery, an assembly of circular tubes or rectangular channels, is one of the best devices available for measuring the size and size distribution of submicron aerosols in the diameter range 0.002 to 0.2 µ m. The performance of these batteries is known from molecular diffusion theory, but until now has not been checked experimentally in this size range because of the lack of the necessary monodisperse aerosols. Experimental measurements on singly charged monodisperse aerosols from 0.01 µm to 0.1 µ m are described using a General Electric and a Pollak condensation nucleus counter to measure the aerosol penetration through the stages of a set of portable diffusion batteries in series. Particle sizes in the range tested could be selected at will by adjusting the voltage of an electric mobility classifier. The fraction of aerosol of a given size passing through each battery stage was found to agree closely with the penetration calculated from molecular diffusion theory for that size. This shows that the theory is correct and confirms that the aerosol produced by the electric mobility classifier was monodisperse. In addition, it was found that the difference in penetration between a charged versus a neutralized aerosol was insignificant except for the smallest aerosols used.     

Estimates of particle hygroscopicity during the Southeastern Aerosol and Visibility Study

Aerosol water content was determined from relative humidity controlled optical particle counter (ASASP-X) size distribution measurements made during the Southeastern Aerosol and Visibility Study (SEAVS) in the Great Smoky Mountains National Park during summer 1995. Since the scattering response function of the ASASP-X is sensitive to particle refractive index, a technique for calibrating the ASASP-X for any real refractive index was developed. A new iterative process was employed to calculate water mass concentration and wet refractive index as functions of relative humidity. Experimental water mass concentrations were compared to theoretically predicted values assuming only ammonium sulfate compounds were hygroscopic. These comparisons agreed within experimental uncertainty. Estimates of particle hygroscopicity using a rural aerosol model of refractive index as a function of relative humidity demonstrated no significant differences from those made with daily varying refractive index estimates. Although aerosol size parameters were affected by the assumed chemical composition, forming ratios of these parameters nearly canceled these effects.     

Coral reef aerosol emissions in response to irradiance stress in the Great Barrier Reef,Australia

We investigate the correlation between stress-related compounds produced by corals of the Great Barrier Reef (GBR) and local atmospheric properties—an issue that goes to the core of the coral ecosystem’s ability to survive climate change. We relate the variability in a satellite decadal time series of fine-mode aerosol optical depth (AOD) to a coral stress metric, formulated as a function of irradiance, water clarity, and tide, at Heron Island in the southern GBR. We found that AOD was correlated with the coral stress metric, and the correlation increased at low wind speeds, when horizontal advection of air masses was low and the production of non-biogenic aerosols was minimal. We posit that coral reefs may be able to protect themselves from irradiance stress during calm weather by affecting the optical properties of the atmosphere and local incident solar radiation.     

Optical Measurements of Aerosol Size Distributions in Great Smoky Mountains National Park: Dry Aerosol Characterization

ABSTRACT

Aerosol size distributions were measured during the summertime 1995 Southeastern Aerosol and Visibility Study (SEAVS) in Great Smoky Mountains National Park using an Active Scattering Aerosol Spectrometer (ASASP-X) optical particle counter. We present an overview of the experimental method, our data inversion technique, timelines of the size distribution parameters, and calculations of dry accumulation mode aerosol density and refractive index. Aerosol size distributions were recorded during daylight hours for aerosol in the size range 0.1 < Dp < 2.5 u,m. The particle refractive index used for the data inversion was calculated with the partial molar refractive index approach using 12-hr measured aerosol chemical composition. Aerosol accumulation mode volume concentrations ranging from 1 to 26 u,m³ cm^-3 were observed, with an average of 7 ± 5 u,m³ cm^-3. The study average dry accumulation mode geometric volume median diameter was 0.27 ± 0.03 u,m, and the mean geometric standard deviation was 1.45 ± 0.06. Using an internally mixed aerosol model, and assuming chemical homogeneity across the measured particle distribution, an average accumulation mode dry sulfate ion mass scattering efficiency of 3.8 ± 0.6 m² g^-1 was calculated.     

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.     

Chemical characterization of submicron organic aerosols in the tropical trade winds of the caribbean using gas chromatography/mass spectrometry

Chemical characterization of submicron (D_p<0.6 μm) organic aerosols in the tropical trade winds in the Caribbean was performed. Samples were collected with a Lundgren cascade impactor at different locations in and around the island of Puerto Rico. The majority of the samples were collected at the Lighthouse at Fajardo. The GC/MS results were compiled into a database. The compounds identified were consistently observed in most of the samples and seem to have a natural origin. The families of compounds most consistently detected were esters (fatty acid esters and phosphates), fatty acids, and normal as well as branched hydrocarbons. The modality of extracted ion from full-scan MS data did not show the presence of PAHs in any of the samples analyzed from the coastal and ocean sites. Results tend to indicate that a substantial fraction of the submicron organic aerosol found in the tropical trade winds of the Caribbean may be associated with natural oceanic emissions; therefore, any treatment of the total aerosol should consider the contribution of this natural background aerosol.     

Comparisons of aerosol properties measured by impactors and light scattering from individual particles: refractive index,number and volume concentrations,and size distributions

The southeastern aerosol and visibility study (SEAVS) was conducted in Great Smoky Mountains National Park in summer 1995 to investigate variations in ambient aerosol size distributions and their effect on visibility. In this paper, we compare dry aerosol size distribution parameters from a MOUDI impactor and two different optical particle counters (OPCs). Size distributions from the various instruments are expressed in a common measure of size, specifically, optical and aerodynamic diameters are converted to a dry, geometric diameter basis. Comparisons of the real part of particle refractive index obtained directly from light scattering measurements and inferred from aerosol composition measurements are also shown. Real refractive indices from direct measurements and those computed from measured fine aerosol chemical composition were generally within ±0.02. Maximum differences in estimated accumulation mode integrated volume concentrations from all instruments were within ∼22%. Accumulation mode integrated number concentrations and geometric standard deviations from the two OPCs agreed within ∼30% and ∼3%, respectively. Differences between MOUDI- and OPC-derived accumulation mode number concentrations and geometric standard deviations were ∼20% and ∼8%, respectively. The average geometric volume mean diameters derived from the three instruments agreed within 15% or less. The volume median diameters obtained by fitting the CSU number concentration data to a lognormal function were typically the smallest. We show that these discrepancies can be related to the differences and biases in the measurement and data analysis techniques.