Aerosol properties,in-canopy gradients,turbulent fluxes and VOC concentrations at a pristine forest site in Amazonia

Aerosol physical and chemical properties were measured in a forest site in central Amazonia (Cuieiras reservation, 2.61S; 60.21W) during the dry season of 2004 (Aug–Oct). Aerosol light scattering and absorption, mass concentration, elemental composition and size distributions were measured at three tower levels (Ground: 2 m; Canopy: 28 m, and Top: 40 m). For the first time, simultaneous eddy covariance fluxes of fine mode particles and volatile organic compounds (VOC) were measured above the Amazonian forest canopy. Aerosol fluxes were measured by eddy covariance using a Condensation Particle Counter (CPC) and a sonic anemometer. VOC fluxes were measured by disjunct eddy covariance using a Proton Transfer Reaction Mass Spectrometer (PTR-MS). At nighttime, a strong vertical gradient of phosphorus and potassium in the aerosol coarse mode was observed, with higher concentrations at Ground level. This suggests a source of primary biogenic particles below the canopy. Equivalent black carbon measurements indicate the presence of light-absorbing aerosols from biogenic origin. Aerosol number size distributions typically consisted of superimposed Aitken (76 nm) and accumulation modes (144 nm), without clear events of new particle formation. Isoprene and monoterpene fluxes reached respectively 7.4 and 0.82 mg m^?2 s^?1 around noon. An average fine particle flux of 0.05 ± 0.10 10⁶ m^?2 s^?1 was calculated, denoting an equilibrium between emission and deposition fluxes of fine mode particles at daytime. No significant correlations were found between VOC and fine mode aerosol concentrations or fluxes.     

Iron,manganese and copper emitted by cargo and passenger trains in Zürich (Switzerland): Size-segregated mass concentrations in ambient air

Particle emissions caused by railway traffic have hardly been investigated in the past, due to their obviously minor influence on air quality compared to automotive traffic. In this study, emissions related to particle abrasion from wheels and tracks were investigated next to a busy railway line in Zürich (Switzerland), where trains run nearly exclusively with electrical locomotives. Hourly size-segregated aerosol samples (0.1–1, 1–2.5 and 2.5–10 μm) were collected with a rotating drum impactor (RDI) and subsequently analyzed by synchrotron radiation X-ray fluorescence spectrometry (SR-XRF). In this way, hourly elemental mass concentrations were obtained for chromium, manganese, iron and copper, which are the elements most relevant for railway abrasion. Additionally, daily aerosol filters were collected at the same site as well as at a background site for subsequent analysis by gravimetry and wavelength dispersive XRF (WD-XRF). Railway related ambient air concentrations of iron and manganese were calculated for the coarse (2.5–10 μm) and fine (<2.5 μm) particle fraction by means of a Mn/Fe ratio investigation. The comparison to train type and frequency data showed that 75% and 60% of the iron and manganese mass concentrations related to cargo and passenger trains, respectively, were found in the coarse mode. The railway related iron mass concentration normalized by the train frequency ranges between 10 and 100 ng m⁻³ h iron in 10 m distance to the tracks, depending on train type. It is estimated that the personal exposure next to a busy railway line above ground is more than a magnitude lower than inside a subway station.     

Composition and mixing state of the urban background aerosol in the Rhein-Main area (Germany)

Size-resolved aerosol particle samples in the size range 0.1–10 μm aerodynamic diameter were collected in the years 2003 and 2004 at an urban background station in Mainz, Germany. Size, morphology, chemical composition and mixing state of more than 5400 individual particles of 7 selected sampling days were analyzed in detail by scanning electron microscopy and energy-dispersive X-ray microanalysis. In addition, transmission electron microscopy, aerosol mass spectrometry and atomic force microscopy were applied to obtain detailed information about the mixing state of the particles. The fine particle fraction (diameter<1 μm) is always dominated by complex secondary aerosol particles (⩾90% by number) independent from air mass origin. These particles are complex internal mixtures of ammonium and sodium sulfates, nitrates, and organic material. Between 20% and 40% of the complex secondary aerosol particles contain soot inclusions. The composition of the coarse particle fraction (>1 μm diameter) is strongly dependant on air mass history with variable abundances of complex secondary aerosol particles, aged sea salt, silicates, silicate mixtures, calcium sulfates, calcium sulfate/carbonate mixtures, calcium nitrate/carbonate mixtures, biological particles, and external soot.The dominance of complex secondary aerosol particles shows that reduction of the precursor gases is a major goal for successful reduction strategies for PM₁₀.     

What are the sources and conditions responsible for exceedences of the 24 h PM10 limit value (50 μg m−3) at a heavily trafficked London site?

The European Union has set limit values for PM₁₀ to be met in 2005. At Marylebone Road, London, where the traffic is heavy, the daily limit value of 50 μg m⁻³ is exceeded more than 35 times a year. A total of 185 days with daily PM₁₀ concentrations exceeding the limit value of 50 μg m⁻³ measured between January 2002 and December 2004 (data capture of 89.5%) are discussed in this paper. These exceedences were more frequent in early spring and in autumn. Concentrations have been disaggregated into regional, urban (background) and local (street) contributions. Most of the episodes of gravimetric PM₁₀ above the limit value were associated with a high regional background and very often the regional contribution dominated the PM₁₀ mass. The secondary aerosol (especially the particulate nitrate) made a major contribution to the PM₁₀ load. These situations were frequently observed when air masses came from the European mainland (showing that both emissions from the UK and other EU countries contributed to the exceedences), and less frequently with maritime air masses that have stagnated over the UK (showing that emissions from the UK alone less frequently contributed to the high regional background). However, the higher frequency of episodes breaching the limit value at the roadside site than at the rural site and the higher frequency of PM₁₀ concentrations above the limit value on weekdays show that the high regional contributions are additional to local and urban emissions. Local emissions mainly due to traffic were the second important contributor to the exceedences, while the contribution of the urban background of London was less important than the local emissions and the regional background. Applying the pragmatic mass closure model of Harrison et al. [2003. A pragmatic mass closure model for airborne particulate matter at urban background and roadside sites. Atmospheric Environment 37, 4927–4933], revealed that the regional aerosol is comprised very largely of ammonium nitrate and sulphate and secondary organic aerosol. Findings suggest that international abatement of secondary aerosol precursors may be the most effective measure to fulfil the requirements of the European Directive 1999/30/CE by lowering the regional background.     

Temporal trends of black carbon concentrations and regional climate forcing in the southeastern United States

The effect of black carbon (BC) on climate forcing is potentially important, but its estimates have large uncertainties due to a lack of sufficient observational data. The BC mass concentration in the southeastern US was measured at a regionally representative site, Mount Gibbes (35.78°N, 82.29°W, 2006 m MSL). The air mass origin was determined using 48-h back trajectories obtained from the hybrid single-particle Lagrangian integrated trajectory model. The highest average concentration is seen in polluted continental air masses and the lowest in marine air masses. During the winter, the overall average BC value was 74.1 ng m⁻³, whereas the overall summer mean BC value is higher by a factor of 3. The main reason for the seasonal difference may be enhanced thermal convection during summer, which increases transport of air pollutants from the planetary boundary layer of the surrounding urban area to this rural site. In the spring of 1998, abnormally high BC concentrations from the continental sector were measured. These concentrations were originating from a biomass burning plume in Mexico. This was confirmed by the observations of the Earth probe total ozone mapping spectrometer. The BC average concentrations of air masses transported from the polluted continental sector during summer are low on Sunday to Tuesday with a minimum value of 256 ng m⁻³ occurring on Monday, and high on Wednesday to Friday with a maximum value of 379 ng m⁻³ occurring on Friday. The net aerosol radiative forcing (scattering effects plus absorption effects) per unit vertical depth at 2006 m MSL is calculated to be −1.38×10⁻³ W m⁻³ for the southeastern US. The magnitude of direct radiative forcing by aerosol scattering is reduced by 15±7% due to the BC absorption.     

Aerosol size and chemical characteristics at Mumbai,India, during the INDOEX-IFP (1999)

Aerosol size and chemical characteristics govern their optical and radiative effects and their potential for cloud nucleation. This paper reports the size and chemical characteristics of surface aerosols measured at Mumbai during the Indian Ocean Experiment-Intensive Field Phase (INDOEX-IFP), January–March 1999. Carbonaceous (30%) and ionic (20%) constituents contributed significantly to aerosol mass. High black carbon concentrations and a low organic to black carbon ratio implied the predominance of primary carbonaceous aerosol, while a high nss-sulphate contribution in the fine mode, suggested a probable anthropogenic origin. Non-sea-salt potassium (nss-K⁺) and black carbon concentrations correlated during January and early February, with nss-K⁺ in the fine mode contributing 86% of total-K⁺, implying a common origin from a local biomass-burning source. Crustal sources were dominant during late-February and March, with 69% of the aerosol mass present in the coarse mode, and 60% of the variation in PM-10 measured during 12:00–16:00 h being explained by a crustal source factor. Chloride depletion was estimated throughout the study, more significantly during January and early February, from the higher RH and lower Ca²⁺/Na²⁺ ratios. A negative correlation was obtained of chloride with nitrate, indicating probable nitrate substitution. During late-February and March, nitrate correlated with calcium suggesting an association with soil. Nss-sulphate correlated with calcium but not sodium, implying a probable association with crustal aerosols.     

Simultaneous observations of boundary-layer aerosol layers with CL31 ceilometer and 1064/532 nm lidar

Aerosol backscatter measurements from a Vaisala CL31 ceilometer are compared directly with a co-located 532/1064 nm lidar in order to validate the CL31 for remote sensing of vertical aerosol structure. The cases examined include a significant aerosol event (biomass burning), which by virtue of its vertical extent, provides a robust measure of the vertical range of the ceilometer for aerosol applications. A second case is presented when the instruments were separated in order to illustrate the utility of a network of such instruments for elucidating spatial patterns in aerosol distribution and the advection of elevated pollutant layers. When co-located, the instruments show remarkable agreement and indicate that the CL31 can detect aerosol layers up to 3000 m AGL in ideal conditions (at night and with high aerosol concentrations as found in biomass burning or dust plumes). When separated, multiple instruments provide an opportunity to examine advection of pollutant layers as well as their evolution. This suggests that installation of a ceilometer network would provide a cost-effective means of examining three-dimensional aspects of regional air quality as well as distinguishing between regional and local sources of pollution     

Secondary organic aerosol formation from the oxidation of aromatic hydrocarbons in the presence of dry submicron ammonium sulfate aerosol

A laboratory study was conducted to examine formation of secondary organic aerosols. A smog chamber system was developed for studying gas–aerosol interactions in a dynamic flow reactor. These experiments were conducted to investigate the fate of gas and aerosol phase compounds generated from hydrocarbon–nitrogen oxide (HC/NO_x) mixtures irradiated in the presence of fine (<2.5 μm) particulate matter. The goal was to determine to what extent photochemical oxidation products of aromatic hydrocarbons contribute to secondary organic aerosol formation through uptake on pre-existing inorganic aerosols in the absence of liquid water films. Irradiations were conducted with toluene, p-xylene, and 1,3,5-trimethylbenzene in the presence of NO_x and ammonium sulfate aerosol, with propylene added to enhance the production of radicals in the system. The secondary organic aerosol yields were determined by dividing the mass concentration of organic fraction of the aerosol collected on quartz filters by the mass concentration of the aromatic hydrocarbon removed by reaction. The mass concentration of the organic fraction was obtained by multiplying the measured organic carbon concentration by 2.0, a correction factor that takes into account the presence of hydrogen, nitrogen, and oxygen atoms in the organic species. The mass concentrations of ammonium, nitrate, and sulfate concentrations as well as the total mass of the aerosols were measured. A reasonable mass balance was found for each of the aerosols. The largest secondary organic aerosol yield of 1.59±0.40% was found for toluene at an organic aerosol concentration of 8.2 μm⁻³, followed by 1.09±0.27% for p-xylene at 6.4 μg m⁻³, and 0.41±0.10% for 1,3,5-trimethylbenzene at 2.0 μg m⁻³. In general, these results agree with those reported by Odum et al. and appear to be consistent with the gas–aerosol partitioning theory developed by Pankow. The presence of organic in the aerosol did not affect significantly the hygroscopic properties of the aerosol.     

An examination of the physical and optical properties of aerosols collected in the IMPROVE program

The Interagency Monitoring of Protected Visual Environments (IMPROVE) protocols for reconstructing the ambient light extinction coefficient (b_ext) from measured aerosol species are the basis for evaluating compliance under the Regional Haze Rule. Aerosol mass composition and optical properties have been measured as part of the IMPROVE program since 1988, providing a long-term data set of aerosol properties at 38 sites around the US. This data set is used to evaluate assumptions made in calculating reconstructed mass and b_ext by applying statistical analysis techniques. In particular, the molecular weight to carbon weight ratio used to compute particulate organic matter is investigated. An annual average value of 1.7±0.2 for the IMPROVE sites, compared to the value of 1.4 currently assumed in the IMPROVE algorithm, is derived. Regression analysis also indicates that fine soil mass concentrations are underestimated by roughly 20% on average. Finally, aerosol mass scattering and extinction efficiencies assumed in the IMPROVE reconstructed b_ext protocol are examined. Fine mode (D_p<2.5 μm) mass scattering efficiencies have a functional dependence on mass concentrations at many sites, and use of a mass-concentration-dependent adjustment factor to refine the assumed efficiencies provides for closer agreement between measured and reconstructed b_ext.     

Transport of SO2 and aerosol over the Yellow sea

Aircraft measurements of air pollutants were made to investigate the characteristic features of long-range transport of sulfur compounds over the Yellow Sea for the periods of 26–27 April and 7–10 November in 1998, and 9–11 April and 19 June in 1999, together with aerosol measurements at the Taean background station in Korea. The overall mean concentrations of SO₂, O₃ and aerosol number in the boundary layer for the observation period ranged 0.1–7.4 ppb 32.1–64.1 ppb and 1.0–143.6 cm⁻³, respectively. It was found that the air mass over the Yellow Sea had a character of both the polluted continental air and clean background air, and the sulfur transport was mainly confined in the atmospheric boundary layer. The median of SO₂ concentration within the boundary layer was about 0.1–2.2 ppb. However, on 8 November, 1998, the mean concentrations of SO₂ and aerosol number increased up to 7.4 ppb and 109.5 cm⁻³, respectively, in the boundary layer, whereas O₃ concentration decreased remarkably. This enhanced SO₂ concentration occurred in low level westerly air stream from China to Korea. Aerosol analyses at the downstream site of Taean in Korea showed 2–3 times higher sulfate concentration than that of other sampling days, indicating a significant amount of SO₂ conversion to non sea-salt sulfate during the long-range transport.     

Mercury species measured atop the Moody Tower TRAMP site,Houston, Texas

Atmospheric mercury speciation was monitored within Houston, Texas, USA, August 6–October 14, 2006 as part of the TexAQS Radical and Aerosol Measurement Program (TRAMP). On average, all mercury levels were significantly elevated compared to a rural Gulf of Mexico coastal site. Concentrations varied from very clean to very dirty. Multi-day periods of stagnant or low-wind conditions brought elevated concentrations of all mercury species, whereas multi-day periods of strong winds, particularly southerly winds off the Gulf of Mexico, brought very low values of mercury species. Over the entire mercury measurement period, the daily averages of mercury species showed distinct and consistent relationships with the average planetary boundary layer dynamics, with gaseous elemental and particulate-bound mercury near-surface concentrations enhanced by a shallow nocturnal boundary layer, and reactive gaseous mercury concentration enhanced by midday convective boundary layer air entrainment transporting air aloft to the surface. Mercury concentrations were not significantly correlated with known products of combustion, likely indicating non-combustion mercury sources from the Houston area petrochemical complexes. On the morning of August 31, 2006 an observed emission event at a refinery complex on the Houston Ship Channel resulted in extremely high concentrations of aerosol mass and particulate-bound mercury at the TRAMP measurement site 20 km downwind.     

An analysis of seasonal surface dust aerosol concentrations in the western US (2001–2004): Observations and model predictions

Long-term surface observations indicate that soil dust represents over 30% of the annual fine (particle diameter less than 2.5 μm) particulate mass in many areas of the western US; in spring and summer, it represents an even larger fraction. There are numerous dust-producing playas in the western US, but surface dust aerosol concentrations in this region are also influenced by dust of Asian origin. This study examines the seasonality of surface soil dust concentrations at 15 western US sites using observations from the Interagency Monitoring of PROtected Visual Environments (IMPROVE) network from 2001 to 2004. Average soil concentrations in particulate matter less than 10 μm in diameter (PM₁₀) were lowest in winter and peaked during the summer months at these sites; however, episodic higher-concentration events (>10 μg m⁻³) occurred in the spring, the time of maximum Asian dust transport to the western US. Simulated surface dust concentrations from the Navy Aerosol Analysis and Prediction System (NAAPS) suggested that long-range transport from Asia dominates surface dust concentrations in the western US in the spring, and that, although some long-range transport does occur throughout the year (1–2 μg m⁻³), locally generated dust plays a larger role in the region in summer and fall. However, NAAPS simulated some anomalously high concentrations (>50 μg m⁻³) of local dust in the fall and winter months over portions of the western US. Differences between modeled and observed dust concentrations were attributed to overestimation of total observed soil dust concentrations by the assumptions used to convert IMPROVE measurements into PM₁₀ soil concentrations, lack of inhibition of model dust production in snow-covered regions, and lack of seasonal agricultural sources in the model.     

Inorganic,organic and macromolecular components of fine aerosol in different areas of Europe in relation to their water solubility

A chemical mass balance of fine aerosol (<1.5 μm AED) collected at three European sites was performed with reference to the water solubility of the different aerosol classes of components. The sampling sites are characterised by different pollution conditions and aerosol loading in the air. Aspvreten is a background site in central Sweden, K-puszta is a rural site in the Great Hungarian Plain and San Pietro Capofiume is located in the polluted Po Valley, northern Italy. The average fine aerosol mass concentration was 5.9 μg m^-3 at the background site Aspvreten, 24 μg m^-3 at the rural K-puszta and 38 μg m^-3 at the polluted site San Pietro Capofiume. However, a similarly high soluble fraction of the aerosol (65–75%) was measured at the three sites, while the percentage of water soluble organic species with respect to the total soluble mass was much higher at the background site (ca. 50%) than at the other two sites (ca. 25%). A very high fraction (over 70%) of organic compounds in the aerosol consisted of polar species. The presence of water soluble macromolecular compounds was revealed in the samples from K-puszta and San Pietro Capofiume. At both sites these species accounted for between ca. 20–50% of the water soluble organic fraction. The origin of the compounds was tentatively attributed to biomass combustion.     

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.     

Inorganic element concentrations in near surface aerosols sampled on the northwest slopes of Mount Kenya

Eight trace elements, Si, Cl, K, Ca, Ti, Mn, Fe and Zn in the near-ground atmospheric aerosols were evaluated in the northwestern part of Mount Kenya using a dichotomous sampler and an EDXRF spectrometer. The samples were taken at 2 sites situated in Nanyuki area, which is roughly on the Equator. The sampler segregated the aerosol into two aerodynamic diameter (ad) size fractions, fine (<3.5 μm ad) and coarse (>3.5 and <18 μm ad). The elemental concentrations in the two size fractions were quantified and the elements assigned to known sources. Local wind blown dust related to agricultural activities and fire burning was found to dominate the lower tropospheric aerosols. There was inconclusive evidence of long range-transported aerosols being moved by night transport from the middle to the lower parts of the troposphere. Influence of the Indian Ocean marine aerosol was suggested but conclusive evidence was lacking.     

Formation of submicron sulfate and organic aerosols in the outflow from the urban region of the Pearl River Delta in China

Size-resolved chemical compositions of non-refractory submicron aerosols were measured using a quadrupole Aerodyne aerosol mass spectrometer at a rural site near Guangzhou in the Pearl River Delta (PRD) of China in the summer of 2006. Two cases characterized as the outflows from the PRD urban region with plumes of high SO₂ concentration were investigated. The evolution of sulfate size distributions was observed on a timescale of several hours. Namely mass concentrations of sulfate in the condensation mode (with vacuum aerodynamic diameters (D_va) < 300 nm) increased at a rate of about 0.17–0.37 ppbv h^?1 during the daytime. This finding was consistent with the sulfuric acid production rates of about 0.17–0.3 ppbv h^?1, as calculated from the observed gas-phase concentrations of OH (～3.3 × 10⁶–1.7 × 10⁷ cm^?3) and SO₂ (～3–21.2 ppbv). This implies that the growth of sulfate in the condensation mode was mainly due to gas-phase oxidation of SO₂. The observed rapid increase was caused mainly by the concurrent high concentrations of OH and SO₂ in the air mass. The evolution of the mass size distributions of m/z 44, a tracer for oxygenated organic aerosol (OOA), was very similar to that of sulfate. The mass loadings of m/z 44 were strongly correlated with those of sulfate (r² = 0.99) in the condensation mode, indicating that OOA might also be formed by the gas-phase oxidation of volatile organic compound (VOC) precursors. It is likely that sulfate and OOA were internally mixed throughout the whole size range in the air mass.     

Characterization of PM2.5 aerosols dominated by local pollution and Asian dust observed at an urban site in Korea during aerosol characterization experiments (ACE)--Asia Project

Daily fine particulate matter (PM2.5) samples were collected at Gwangju, Korea, during the Aerosol Characterization Experiments (ACE)-Asia Project to determine the chemical properties of PM2.5 originating from local pollution and Asian dust (AD) storms. During the study period, two significant events occurred on April 10-13 and 24-25, 2001, and a minor event occurred on April 19, 2001. Based on air mass transport pathways identified by back-trajectory calculation, the PM2.5 dataset was classified into three types of aerosol populations: local pollution and two AD aerosol types. The two AD types were transported along different pathways. One originated from Gobi desert area in Mongolia, passing through Hunshandake desert in Northern Inner Mongolia, urban and polluted regions of China (AD1), and the other originated in sandy deserts located in the Northeast Inner Mongolia Plateau and then flowed southward through the Korean peninsula (AD2). During the AD2 event, a smoke plume that originated in North Korea was transported to our study site. Mass balance closures show that crustal materials were the most significant species during both AD events, contributing -48% to the PM2.5 mass; sulfate aerosols (19.1%) and organic matter (OM; 24.6%) were the second greatest contributors during the AD1 and AD2 periods, respectively, indicating that aerosol properties were dependent on the transport pathway. The sulfate concentration constituted only 6.4% (4.5 microg/m3) of the AD2 PM2.5 mass. OM was the major chemical species in the local pollution-dominated PM2.5 aerosols, accounting for 28.7% of the measured PM2.5 mass, followed by sulfate (21.4%), nitrate (15%), ammonium (12.8%), elemental carbon (8.9%), and crustal material (6.5%). Together with substantial enhancement of the crustal elements (Mg, Al, K, Ca, Sc, Ti, Mn, Fe, Sr, Zr, Ba, and Ce), higher concentrations of pollution elements (S, V, Ni, Zn, As, Cd, and Pb) were observed during AD1 and AD2 than during the local pollution period, indicating that, in addition to crustal material, the AD dust storms also had a significant influence on anthropogenic elements.     

Simulation of aerosol direct radiative forcing with RAMS-CMAQ in East Asia

The air quality modeling system RAMS-CMAQ is developed to assess aerosol direct radiative forcing by linking simulated meteorological parameters and aerosol mass concentration with the aerosol optical properties/radiative transfer module in this study. The module is capable of accounting for important factors that affect aerosol optical properties and radiative effect, such as incident wave length, aerosol size distribution, water uptake, and internal mixture. Subsequently, the modeling system is applied to simulate the temporal and spatial variations in mass burden, optical properties, and direct radiative forcing of diverse aerosols, including sulfate, nitrate, ammonium, black carbon, organic carbon, dust, and sea salt over East Asia throughout 2005. Model performance is fully evaluated using various observational data, including satellite monitoring of MODIS and surface measurements of EANET (Acid Deposition Monitoring Network), AERONET (Aerosol Robotic Network), and CSHNET (Chinese Sun Hazemeter Network). The correlation coefficients of the comparisons of daily average mass concentrations of sulfate, PM2.5, and PM10 between simulations and EANET measurements are 0.70, 0.61, and 0.64, respectively. It is also determined that the modeled aerosol optical depth (AOD) is in congruence with the observed results from the AERONET, the CSHNET, and the MODIS. The model results suggest that the high AOD values ranging from 0.8 to 1.2 are mainly distributed over the Sichuan Basin as well as over central and southeastern China, in East Asia. The aerosol direct radiative forcing patterns generally followed the AOD patterns. The strongest forcing effect ranging from −12 to −8 W m⁻² was mainly distributed over the Sichuan Basin and the eastern China’s coastal regions in the all-sky case at TOA, and the forcing effect ranging from −8 to −4 W m⁻² could be found over entire eastern China, Korea, Japan, East China Sea, and the sea areas of Japan     

Atmospheric phosphorus deposition at a montane site: Size distribution,effects of wildfire,and ecological implications

The dry deposition of atmospheric particulate matter can be a significant source of phosphorus (P) to oligotrophic aquatic ecosystems, including high-elevation lakes. In this study, measurements of the mass concentration and size distribution of aerosol particles and associated particulate P are reported for the southern Sierra Nevada, California, for the period July–October, 2008. Coarse and fine particle samples were collected with Stacked Filter Units and analyzed for Total P (TP) and inorganic P (IP) using a digestion-extraction procedure, with organic P (OP) calculated by difference. Particle size-resolved mass and TP distributions were determined concurrently using a MOUDI cascade impactor. Aerosol mass concentrations were significantly elevated at the study site, primarily due to transport from offsite and emissions from local and regional wildfires. Atmospheric TP concentrations ranged from 11 to 75 ng m^?3 (mean = 37 ± 16 ng m^?3), and were typically dominated by IP. Phosphorus was concentrated in the coarse (>1 μm diameter) particle fraction and was particularly enriched in the 1.0–3.2 μm size range, which accounted for 30–60% of the atmospheric TP load. Wildfire emissions varied widely in P content, and may be related to fire intensity. The estimated dry depositional flux of TP for each daily sampling period ranged between 7 and 118 μg m^?2 d^?1, with a mean value of 40 ± 27 μg m^?2 d^?1. Relative rates of dry deposition of N and P in the Sierra Nevada are consistent with increasing incidence of N limitation of phytoplankton growth and previously observed long-term eutrophication of lakes.     

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.