Precipitation scavenging coefficient: influence of measured aerosol and raindrop size distributions

Precipitation scavenging coefficients, widely used in pollution studies, are derived from microphysical parameterisations of aerosol particles and raindrop populations and parameterisations of their interactions. The present study investigates the effects of measured aerosol and raindrop size distributions in a microphysical polydisperse framework. The interactions between aerosol and raindrops parameterised as collision efficiency are explicitly included to account for Brownian diffusion, inertial impaction and interception. Estimated values of the polydisperse scavenging coefficients exhibit variations of orders of magnitude depending on the aerosol type and almost no variation with the raindrop size distributions. For practical use, linear relationships between the scavenging coefficients and rain intensity for different aerosol types are derived.     

Size distribution and sources of aerosol in Launceston, Australia, during winter 1997

As part of a pilot study into the chemical and physical properties of Australian fine particles, a suite of aerosol samples was collected at Ti Tree Bend in Launceston, Tasmania, during June and July 1997. This period represents midwinter in the Southern Hemisphere, a period when aerosol sources in Launceston are dominated by smoke from domestic wood burning. This paper describes the results from this measurement campaign, with the aim of assessing the effect of wood smoke on the chemical and physical characteristics of ambient aerosol. A micro orifice uniform deposit impactor (MOUDI) was used to measure the size distributions of the aerosol from 0.05 to 20 microns aerodynamic diameter. Continuous measurements of fine particle mass were made using a PM2.5 tapered element oscillating microbalance (TEOM) and light scattering coefficients at 530 nm were measured with nephelometers. Mass size distributions tended to be bimodal, with the diameter of the dominant mode tending to smaller sizes with increases in total mass. Non-sea salt potassium and polycyclic aromatic hydrocarbons (PAHs) were used as chemical tracers for wood smoke. Wood smoke was found to increase absolute particle mass (enough to regularly exceed air quality standards), and to concentrate mass in a single mode below 1 micron aerodynamic diameter. The acid-base equilibrium of the aerosol was altered by the wood smoke source, with free acidity hydrogen ion, non-sea salt sulfate, and ammonium concentrations being higher and the concentration of all species, including nitrate (to differing extents), focused in the fine particle size ranges. The wood smoke source also heavily influenced the aerosol scattering efficiency, adding to a strong diurnal cycle in both mass concentration and light scattering.     

Real-time measurements of the chemical composition of size-resolved particles during a Santa Ana wind episode,California USA

Size-resolved particle composition, mass and number concentrations, aerosol scattering coefficients, and prevailing meteorological conditions were measured at the Ellen Browning Scripps Memorial Pier located in La Jolla, California on 15 December 1998. Aerosol particles were sampled using a field transportable aerosol time-of-flight mass spectrometer, allowing for the continuous detection and characterization of single particles from a polydisperse sample. An extensive and rapid change in the chemical composition of aerosol particles with aerodynamic diameters between 1.0 and 2.5 μm has been observed during the onset of a Santa Ana Winds condition. Coincident with the observed change in meteorological conditions, a substantial decrease in sea salt particles corresponds to an increase in dust and carbon-containing particles. This paper examines observations of the rapid changes occurring in the chemical composition of single aerosol particles and demonstrates the new types of information that can be obtained by measuring single particle size and composition with high temporal resolution.     

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.     

Aerosol light absorption measurement techniques: Analysis and intercomparisons

A controlled study was carried out to evaluate three measurement techniques used for the determination of aerosol light absorption coefficients from aerosol samples collected on various filter substrates. These techniques were found to agree within about 10–30% when applied to a range of filter loading obtained for a laboratory generated calibration aerosol. Microphysical properties of the calibration aerosol were used to model its optical effects using Mie theory. The measured and modeled optical properties were found to differ by less than 30%. Qualitative and quantitative agreement of these techniques indicate that they provide a reasonable indirect method for the determination of atmospheric aerosol absorption coefficients and the related concentration of elemental carbon aerosol.     

Analysis and Simulation of Wintertime Light Scattering by the Urban Aerosol in Dallas-Fort Worth

ABSTRACT

Wintertime atmospheric light scattering in Dallas, TX, was estimated through the use of aerosol models. Input data for the aerosol models were provided by measurements of aerosol chemistry, physical particle size distributions, and distributions of particulate sulfur by particle size, and by predictions by an atmospheric simulation model. Light scattering measurements provided a basis for testing the aerosol models. The SCAPE thermodynamic equilibrium model was used to estimate the amount of liquid water associated with particles and the ELSIE Mie scattering model was applied to estimate the resulting light scattering. The calculations were based on aerosol properties measured in Dallas during December 1994 and February 1995, and changes in scattering due to hypothetical changes in the aerosol were predicted. The predicted light scattering was compared to scattering measured by an Optec nephelom-eter; agreement was within 20% in every case.     

Analysis and simulation of wintertime light scattering by the urban aerosol in Dallas-Fort Worth

Wintertime atmospheric light scattering in Dallas, TX, was estimated through the use of aerosol models. Input data for the aerosol models were provided by measurements of aerosol chemistry, physical particle size distributions, and distributions of particulate sulfur by particle size, and by predictions by an atmospheric simulation model. Light scattering measurements provided a basis for testing the aerosol models. The SCAPE thermodynamic equilibrium model was used to estimate the amount of liquid water associated with particles and the ELSIE Mie scattering model was applied to estimate the resulting light scattering. The calculations were based on aerosol properties measured in Dallas during December 1994 and February 1995, and changes in scattering due to hypothetical changes in the aerosol were predicted. The predicted light scattering was compared to scattering measured by an Optec nephelometer; agreement was within 20% in every case.     

Light scattering characteristics of aerosols as a function of relative humidity: Part I--A comparison of measured scattering and aerosol concentrations using the theoretical models

The Southeastern Aerosol and Visibility Study (SEAVS) was undertaken to characterize the size-dependent composition, thermodynamic properties, and optical characteristics of the ambient atmospheric particles in the southeastern United States. The field portion of the study was carried out from July 15 to August 25, 1995. As part of the study a relative humidity controlled inlet was built to raise or lower the relative humidity to predetermined levels before the aerosol was passed into an integrating nephelometer or particle-sizing device. Five other integrating nephelometers were operated in various configurations, two of which were fitted with a 2.5 microns inlet. Fine particle (< 2.5 microns) samplers were operated to measure concentrations of sulfate, nitrate, and ammonium ions, organic and elemental carbon, and fine soil. Mass size distributions were measured with an eight-stage, single orifice cascade impactor. Four different strategies for estimating scattering were used. First, an externally mixed model with constant specific scattering coefficients, sulfate ion mass interpreted as ammonium bisulfate, and ammonium bisulfate growth as a function of relative humidity, is assumed. Second, an externally mixed aerosol model, assuming constant dry specific scattering but with sulfate ammoniation and associated composition-dependent hygroscopicity explicitly accounted for, is used. Third, an externally mixed aerosol model, but with sulfate ammoniation, associated growth as a function of relative humidity, and sulfate size distributions, is applied. Fourth, an internally mixed aerosol model with measured sulfur size distributions and estimated size distributions for other species is used with the growth characteristics of the mixture being estimated using the Zdanovskii-Stokes-Robinson (ZSR) assumptions. Only ionic species were considered to be hygroscopic. The second, third, and fourth approaches yield similar results with reconstructed scattering comparing quite favorably with measured scattering. Accounting for sulfate ammoniation and associated water uptake was the most important detail in achieving closure between measurements and modeled scattering. In general, differences between estimated scattering, assuming internally or externally mixed models, was small. These same models were used to estimate wet to dry scattering ratios. The R2 for an ordinary least-squares regression between measured and predicted ratios was high (0.71-0.92), and in most cases the scattering ratio was insensitive to modeling assumptions. However, during some sample periods differences between predicted scattering ratios for the different modeling assumptions were as high as 30%.     

Size Distribution and Sources of Aerosol in Launceston,Australia, during Winter 1997

ABSTRACT

As part of a pilot study into the chemical and physical properties of Australian fine particles, a suite of aerosol samples was collected at Ti Tree Bend in Launceston, Tasmania, during June and July 1997. This period represents midwinter in the Southern Hemisphere, a period when aerosol sources in Launceston are dominated by smoke from domestic wood burning. This paper describes the results from this measurement campaign, with the aim of assessing the effect of wood smoke on the chemical and physical characteristics of ambient aerosol. A micro orifice uniform deposit impactor (MOUDI) was used to measure the size distributions of the aerosol from 0.05 to 20 n m aerodynamic diameter. Continuous measurements of fine particle mass were made using a PM_2.5 tapered element oscillating microbalance (TEOM) and light scattering coefficients at 530 nm were measured with nephelometers.

Mass size distributions tended to be bimodal, with the diameter of the dominant mode tending to smaller sizes with increases in total mass. Non-sea salt potassium and polycyclic aromatic hydrocarbons (PAHs) were used as chemical tracers for wood smoke. Wood smoke was found to increase absolute particle mass (enough to regularly exceed air quality standards), and to concentrate mass in a single mode below 1 μm aerodynamic diameter. The acid-base equilibrium of the aerosol was altered by the wood smoke source, with free acidity hydrogen ion, non-sea salt sulfate, and ammonium concentrations being higher and the concentration of all species, including nitrate (to differing extents), focused in the fine particle size ranges. The wood smoke source also heavily influenced the aerosol scattering efficiency, adding to a strong diurnal cycle in both mass concentration and light scattering.     

Aerosol physical,chemical and optical properties during the Rocky Mountain Airborne Nitrogen and Sulfur study

During the Rocky Mountain Airborne Nitrogen and Sulfur (RoMANS) study, conducted during the spring and summer of 2006, a suite of instruments located near the eastern boundary of Rocky Mountain National Park (RMNP) measured aerosol physical, chemical and optical properties. Three instruments, a differential mobility particle sizer (DMPS), an optical particle counter (OPC), and an aerodynamic particle sizer (APS), measured aerosol size distributions. Aerosols were sampled by an Interagency Monitoring of Protected Visual Environments (IMPROVE) sampler and a URG denuder/filter-pack system for compositional analysis. An Optec integrating nephelometer measured aerosol light scattering. The spring time period had lower aerosol concentrations, with an average volume concentration of 2.2 ± 2.6 μm³ cm^?3 compared to 6.5 ± 3.9 μm³ cm^?3 in the summer. During the spring, soil was the single largest constituent of PM_2.5 mass, accounting for 32%. During the summer, organic carbon accounted for 60% of the PM_2.5 mass. Sulfates and nitrates had higher fractional contributions in the spring than the summer. Variability in aerosol number and volume concentrations and in composition was greater in the spring than in the summer, reflecting differing meteorological conditions. Aerosol scattering coefficients (b_sp) measured by the nephelometer compared well with those calculated from Mie theory using size distributions, composition data and modeled RH dependent water contents.     

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).     

Air mass characteristics in the vicinity oF Barrow,Alaska, 9–19 March 1983

The synoptic conditions over the Alaskan Arctic during the Arctic Gas and Aerosol Sampling Program (AGASP) of March 1983 are described. Air mass characteristics are pictured in terms of meteorological parameters, condensation nuclei, ozone and CO₂ concentrations, aerosol size and number distributions, and aerosol scattering coefficients, as measured at the Barrow Geophysical Monitoring for Climatic Change (GMCC) baseline station and by aircraft Latitude-altitude cross sections of meteorological and aerosol parameters indicated both strong vertical and horizontal variability within the Arctic air mass. Aerosol concentrations aloft were usually higher than those measured at the ground and peak-to-peak variations are greater aloft than at the surface, showing that the stable Arctic boundary layer reduces mixing from aloft to the surface. Thus, surface measurements cannot be extrapolated to higher levels in a straightforward manner. Horizontal variability in the haze, as determined by the aircraft, was found to be abrupt and was not generally due to the presence of strong meteorological fronts. During 9–19 March 1983, at least four different air mass types were present in the Barrow region, each of which was characterized by distinct meteorological, aerosol and trace gas characteristics.     

Approximate determination of particulate mass loading by using junge-type extinction models for continental and rural aerosol particles

Sets of mass extinction coefficients at visible and near infrared wavelengths were calculated for four aerosol particle polydispersions of continental and rural origins, which are characterized by Junge-type size distribution curves with different radius intervals. The calculations were made by using a very accurate computer programme for Mie extinction. The results show that the mass extinction coefficients are closely related to the upper limit of the radius range as well as to the right wing features of the particle size distribution curves. A procedure is suggested for determining the vertical particulate mass loading from multispectral sun photometer measurements taken in very clear atmospheres. The examination of atmospheric particle extinction measurements in terms of the various extinction models shows that our model CR (based on continental and rural aerosol particle size distributions characterized by different values of Junge parameter in six contiguous radius subintervals from 0.003 to 20 μm) should give realistic estimates of the particulate mass loading in cases in which Angström's exponent α is nearly equal to or higher than 1.4. However, for the majority of real cases giving values of α smaller than 1.4, the model CR gives a good estimate of the lower limit for the particulate mass loading.     

Impacts of meteorological situations and chemical reactions on daily dry deposition of nitrogen into the southern North Sea

The impact of the meteorological situation and chemistry on dry deposition to the southern North Sea is investigated. The studies are performed using a high-resolution meteorology/chemistry model system of different complexity for a five-day period in June 1998. The simulations consider passive tracer transport (Case I), gas phase chemistry (Case II), gas phase plus simple aerosol chemistry (Case III), gas phase plus size dependent aerosol chemistry (Case IV). The results show a very good agreement of meteorology model results with measured data and a reasonable agreement for the concentrations. The dry deposition to the southern North Sea differs a factor of three to seven within the investigated five-day period. Differences are larger for a more complex chemistry. The average dry deposition increases by a factor of three when including gas phase reactions or adding a simple aerosol model and up to a factor of eleven when considering a sectional aerosol model. The input composition depends on the chemistry considered.     

Number size distribution of atmospheric aerosols during ACE-Asia dust and precipitation events

Measurements of size-resolved particle number concentrations during the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia) field campaign were made at the Gosan super-site, South Korea. In East Asia, dust and precipitation phenomena play a crucial role in atmospheric environment and climate studies because they are major sources and sinks of atmospheric aerosols, especially in the springtime. Total Ozone Mapping Spectrometer (TOMS) Aerosol Index and backward trajectories are analyzed to investigate the spatial and temporal evolution of dust storms. The size distributions between dust and non-dust periods and times with and without precipitation are compared. In order to understand the temporal evolution of the aerosol size distribution during dust and precipitation events, a simple aerosol dynamics model is employed. The model predicted and observed size distributions are compared with the measured data. The results show that the coarse mode particle number concentrations increase by a factor of 10–16 during dust events. During precipitation, however, particles in the coarse mode are scavenged by impaction mechanism. It is found that the larger particles are more efficiently scavenged. The degree of scavenged particle varies depending on the rainfall rate, raindrop size distribution and aerosol size distribution.     

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.     

Aerosol ion characteristics during the Big Bend Regional Aerosol and Visibility Observational study

The ionic compositions of particulate matter with aerodynamic diameter < or = 2.5 microm (PM2.5) and size-resolved aerosol particles were measured in Big Bend National Park, Texas, during the 1999 Big Bend Regional Aerosol and Visibility Observational study. The ionic composition of PM2.5 aerosol was dominated by sulfate (SO4(2-)) and ammonium (NH4+). Daily average SO4(2-) and NH4+ concentrations were strongly correlated (R2 = 0.94). The molar ratio of NH4+ to SO4(2-) averaged 1.54, consistent with concurrent measurements of aerosol acidity. The aerosol was observed to be comprised of a submicron fine mode consisting primarily of ammoniated SO4(2-) and a coarse particle mode containing nitrate (NO3-). The NO3- appears to be primarily associated with sea salt particles where chloride has been replaced by NO3-, although formation of calcium nitrate (Ca(NO3)2) is important, too, on several days. Size-resolved aerosol composition results reveal that a size cut in particulate matter with aerodynamic diameter < or = 1 microm would have provided a much better separation of fine and coarse aerosol modes than the standard PM2.5 size cut utilized for the study. Although considerable nitric acid exists in the gas phase at Big Bend, the aerosol is sufficiently acidic and temperatures sufficiently high that even significant future reductions in PM2.5 SO4(2-) are unlikely to be offset by formation of particulate ammonium nitrate in summer or fall.     

The effect of temperature on the gas–particle partitioning of reactive mercury in atmospheric aerosols

Measurements of gas–particle-partitioning coefficients for reactive mercury in dry urban and laboratory aerosol were found to strongly depend on ambient temperature. Samples of atmospheric and laboratory aerosols (defined as both the gas and particle phases) were collected using filter and absorbent methods and analyzed for reactive mercury using thermal desorption combined with cold vapor atomic fluorescence spectroscopy. Synthetic ambient aerosols were generated in the laboratory from ammonium sulfate and adipic acid mixed with mercuric chloride in a purpose-built aerosol reactor. The aerosol reactor was operated in a temperature-controlled laboratory. Linear relationships between the logarithm of inverse gas–particle partitioning and inverse temperature were observed and parameterized for use in the atmospheric modeling of reactive mercury. Reactive mercury was observed to partition from the particle to the gas phase as ambient temperature increased. Good agreement between measurements made using urban and laboratory aerosols was seen after gas–particle-partitioning coefficients were normalized for surface area instead of mass. Thermodynamic analyses of the urban and laboratory gas–particle-partitioning measurements revealed that the strength of interaction between reactive mercury and particle surfaces was suggestive of chemisorption. Gas–particle-partitioning coefficients made with the Tekran ambient mercury analyzer (AMA) also showed a dependence on temperature. However, the Tekran AMA partitioning coefficients did not agree well with partitioning coefficients measured using the filter-based methods. The disagreement is consistent with the 50 °C operational temperature of the Tekran AMA.     

基本单分散气溶胶透过率测试中真实值的计算

通过对高效、超高效滤料透过率测试台工作原理的分析得到:利用基本单分散粒子作为气溶胶测得的透过率关系与滤料真正的透过率-粒径曲线有区别,实际上是所使用实验气溶胶的综合透过率。详细研究了真正透过率与实验透过率的关系、误差和偏离产生原因,最终提出了一种独特的计算方法,实现了根据实验得到的表观透过率-粒径关系,就可以计算出真实透过率-粒径曲线,并得到了采用较为理想的实验气溶胶测试出的真实透过率的实际验证,这将大大提高高效、超高效滤料性能测试台的精度,拓展了其应用范围,为高效滤料的过滤理论和应用研究提供了比较理想的测试手段。     

Total scatter-to-backscatter ratio of aerosol derived from aerosol size distribution measurement

Based on in-situ aerosol size-distribution measurements and Mie scattering theory, total scattering coefficients and backscattering coefficients were calculated to derived wavelength dependent lidar ratio S for 355 nm and 532 nm. Effective radius and C/F ratio of aerosol are also calculated to study the relationships between lidar ratio and particle size dependences. The results show backscatter-related scattering properties are more sensitive to coarse mode particle than total scattering. The mean values of lidar ratio for 355 nm and 532 nm are 31.9 ± 6.2 sr and 40.5 ± 6.1 sr respectively, and S₃₅₅ and S₅₃₂ are linear correlated for S₃₅₅ < 50 sr. S₃₅₅ is highly correlated with effective radius of aerosol, and S₅₃₂ is highly correlated with volume C/F ratio.