Simulation of aerosol radiative properties with the ORISAM-RAD model during a pollution event (ESCOMPTE 2001)

The aim of this study is to present the organic and inorganic spectral aerosol module-radiative (ORISAM-RAD) module, allowing the 3D distribution of aerosol radiative properties (aerosol optical depth, single scattering albedo and asymmetry parameter) from the ORISAM module. In this work, we test ORISAM-RAD for one selected day (24th June) during the ESCOMPTE (expérience sur site pour contraindre les modèles de pollution atmosphérique et de transport d’emissions) experiment for an urban/industrial aerosol type. The particle radiative properties obtained from in situ and AERONET observations are used to validate our simulations. In a first time, simulations obtained from ORISAM-RAD indicate high aerosol optical depth (AOD)0.50–0.70±0.02 (at 440 nm) in the aerosol pollution plume, slightly lower (10–20%) than AERONET retrievals. In a second time, simulations of the single scattering albedo (ω_o) have been found to well reproduce the high spatial heterogeneities observed over this domain. Concerning the asymmetry parameter (g), ORISAM-RAD simulations reveal quite uniform values over the whole ESCOMPTE domain, comprised between 0.61±0.01 and 0.65±0.01 (at 440 nm), in excellent agreement with ground based in situ measurements and AERONET retrievals. Finally, the outputs of ORISAM-RAD have been used in a radiative transfer model in order to simulate the diurnal direct radiative forcing at different locations (urban, industrial and rural). We show that anthropogenic aerosols strongly decrease surface solar radiation, with diurnal mean surface forcings comprised between −29.0±2.9 and −38.6±3.9 W m⁻², depending on the sites. This decrease is due to the reflection of solar radiations back to space (−7.3±0.8<ΔF_TOA<−12.3±1.2 W m⁻²) and to its absorption into the aerosol layer (21.1±2.1<ΔF_ATM<26.3±2.6 W m⁻²). These values are found to be consistent with those measured at local scale.     

Aerosol optical,chemical and physical properties at Gosan,Korea during Asian dust and pollution episodes in 2001

In order to understand the influence of dust and anthropogenic pollution aerosols on regional climate in East Asia, we analyzed the aerosol optical, chemical and physical properties for two cases with high aerosol loading and assessed the radiative forcing of these cases. The 1st case study is a heavy dust episode (DE) in April (during ACE-Asia) 2001 and the 2nd case is a regional-scale pollution event in November 2001. The Ångström exponent (Å) for DE was 0.38 from sunphotometer measurements. The mean single scattering albedo (550 nm) at the surface reported during the pollution episode (PE, 0.88) was lower than that of DE (0.91). The concentrations of organic (OC) and elemental carbon (EC) measured during the PE were about 90% and 30% higher than DE. The aerosol mass scattering efficiency (α_s) of PE is a factor of about 2 higher than that of the DE. The difference in the mass absorption efficiency (α_a) of EC during DE and PE is small and within the measurement uncertainty. The diurnally averaged aerosol radiative forcing efficiency (ΔDFE, W m⁻² τ⁻¹) during DE is similar to results of other studies at Gosan.     

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.     

Exposure of acid aerosol for schoolchildren in metropolitan Taipei

Metropolitan Taipei, which is located in the subtropical area, is characterized by high population and automobile densities. For convenience, most primary schools are located near major roads. This study explores the exposure of acid aerosols for schoolchildren in areas in Taipei with different traffic densities. Acid aerosols were collected by using a honeycomb denuder filter pack sampling system (HDS). Experimental results indicated that the air pollutants were significantly correlated with traffic densities. The ambient air NO₂, SO₂, HNO₃, NO₃⁻, SO₄²⁻, and aerosol acidity concentrations were 31.3 ppb, 4.7 ppb, 1.3 ppb, 1.9 μg m⁻³, 18.5 μg m⁻³, and 49.5 nmol m⁻³ in high traffic density areas, and 6.1 ppb, 1.8 ppb, 0.9 ppb, 0.7 μg m⁻³, 8.8 μg m⁻³ and 14.7 nmol m⁻³ in low traffic density areas. The exposure levels of acid aerosols for schoolchildren would be higher than the measurements because the sampling height was 5 m above the ground. The SO₂ levels were low (0.13–8.03 ppb) in the metropolitan Taipei. However, the SO₄²⁻ concentrations were relatively high, and might be attributed to natural emissions of sulfur-rich geothermal sources. The seasonal variations of acid aerosol concentrations were also observed. The high levels of acidic particles in spring time may be attributed to the Asian dust storm and low height of the mixture layer. We conclude that automobile contributed not only the primary pollutants but also the secondary acid aerosols through the photochemical reaction. Schoolchildren were exposed to twice the acid aerosol concentrations in high traffic density areas compared to those in low traffic density areas. The incidence of allergic rhinitis of schoolchildren in the high traffic density areas was the highest in spring time. Accompanied by high temperature variation and high levels of air pollution in spring, the health risk of schoolchildren had been observed.     

Characterization of aerosol over the Northern South China Sea during two cruises in 2003

Atmospheric transport of trace elements has been found to be an important pathway for their input to the ocean. TSP, PM10, and PM2.5 aerosol samples were collected over the Northern South China Sea in two cruises in 2003 to estimate the input of aerosol from continent to the ocean. About 23 elements and 14 soluble ions in aerosol samples were measured. The average mass concentration of TSP in Cruise I in January (78 μg m⁻³) was ∼twice of that in Cruise II in April (37 μg m⁻³). Together with the crustal component, heavy metals from pollution sources over the land (especially from the industry and automobiles in Guangzhou) were transported to and deposited into the ocean. The atmospheric MSA concentrations in PM2.5 (0.048 μg m⁻³ in Cruise I and 0.043 μg m⁻³ in Cruise II) over Northern South China Sea were comparable to those over other coastal regions. The ratio of non-sea-salt (NSS)-sulfate to MSA is 103-655 for Cruise I and 15-440 for Cruise II in PM2.5 samples, which were much higher than those over remote oceans. The estimated anthropogenic sulfate accounts for 83–98% in Cruise I and 63–95% in Cruise II of the total NSS-sulfate. Fe (II) concentration in the aerosols collected over the ocean ranged from 0.1 to 0.9 μg m⁻³, accounting for 16–82% of the total iron in the aerosol, which could affect the marine biogeochemical cycle greatly.     

Sulfate aerosols forcing: An estimate using a three-dimensional interactive chemistry scheme

The tropospheric sulfate radiative forcing has been calculated using an interactive chemistry scheme in LMD-GCM. To estimate the radiative forcing of sulfate aerosol on climate, a consistent interaction between atmospheric circulation and radiation computation has been allowed in LMD-GCM. The model results indicate that the change in the sulfate aerosols number concentration is negatively correlated to the indirect radiative forcing. The model simulated annual mean direct radiative forcing ranges from −0.1 to −1.2 W m⁻², and indirect forcing ranges from −0.4 to −1.6 W m⁻². The global annual mean direct effect estimated by the model is −0.48 W m⁻², and that of indirect is −0.68 W m⁻².     

Estimating bulk optical properties of aerosols over the western North Pacific by using MODIS and CERES measurements

Over the western North Pacific, a large amount of land aerosols from Asian-Pacific countries is transported by the prevailing westerlies. This transport makes the radiative characteristics of these aerosols diverse, particularly when one compares those characteristics over the coastal sea with those over the open sea. In this paper we discuss a method that uses satellite data to obtain the single-scattering albedo (ω) and asymmetry factor (g) of atmospheric aerosols for two large-scale subdivisions—the coastal sea (within 250 km from the coast) and the open sea (the remaining area)—over the western North Pacific (110°E–180°, 20°N–50°N). Our estimation method uses satellite measurements, obtained over a six-year period (2000–2005), of aerosol optical depth (AOD) and shortwave fluxes at both the surface and the top of the atmosphere (TOA); the measurements are obtained using the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Clouds and the Earth's Radiant Energy System (CERES). For the two subdivisions, the estimated annual means of (ω,g) at 630 nm are significantly different: (0.94, 0.65) over the coastal sea and (0.97, 0.70) over the open sea. From a quantitative viewpoint, this result indicates that in comparison with aerosols over the open sea, those over the coastal sea show greater absorption and lesser forward scattering of solar radiation. The estimated optical properties are responsible for the aerosol surface cooling observed by MODIS and CERES, which is approximately 138 and 108 W m⁻² per AOD over the coastal sea and open sea, respectively.     

Visibility impairment during Yellow Sand periods in the urban atmosphere of Kwangju,Korea

For continuous monitoring of atmospheric visibility in the city of Kwangju, Korea, a transmissometer system consisting of a transmitter and a receiver was installed at a distance of 1.91 km across the downtown Kwangju, Korea. At the transmitter site a nephelometer and an aethalometer were also installed to measure the scattering and absorption coefficients of the atmosphere, respectively. Unusually high number of Yellow Sand events had occurred in the Northeast Asia during the spring of 2000. Visibility in Kwangju under such conditions was greatly impaired over large area for a few days. In order to investigate the effects of Yellow Sand on visibility impairment, chemical and elemental analyses of aerosol samples were performed along with the optical measurement of visibility. Hourly averaged visual range decreased from 61.7 to 1.9 km when hourly averaged concentration of PM10 varied from 32.9 to 601.8 μg/m³ during Yellow Sand periods. Fine particulate (<2.5 μm) concentrations were relatively lower than coarse particulate matters. Results of the data analyses show that mineral dusts originated from continental sources were simultaneously transported along with anthropogenic sulfate aerosols and marine aerosols. Total light extinction coefficient, b_ext, proposed by the IMPROVE network showed poor correlation with b_ext measured by transmissometer. Coarse mass scattering efficiency was classified into three categories; E_NHSOc, E_mineral, and E_sea-salt, which were determined as ammonium sulfate combined with nss-sulfate of 1.0, sea-salt of 0.4, and mineral of 0.77 m²/g, respectively. Mass fraction of NHSOc, sea-salt, and mineral dust was 0.20, 0.14, and 0.66, respectively.     

Aerosol scattering properties in northern China

The aerosol scattering properties were investigated at two continental sites in northern China in 2004. Aerosol light scattering coefficient (σ_sp) at 525 nm, PM₁₀, and aerosol mass scattering efficiencies (α) at Dunhuang had a mean value of 165.1±148.8 M m⁻¹, 157.6±270.0 μg m⁻³, and 2.30±3.41 m² g⁻¹, respectively, while these values at Dongsheng were, respectively, 180.2±151.9 M m⁻¹, 119.0±112.9 μg m⁻³, and 1.87±1.41 m² g⁻¹. There existed a seasonal variability of aerosol scattering properties. In spring, at Dunhuang PM₁₀, σ_sp, and α were 184.1±211.548 μg m⁻³, 126.3±89.6 M m⁻¹, and 1.05±0.97 m² g⁻¹, respectively, and these values at Dongsheng were 146.4±142.1 μg m⁻³, 183.4±81.7 M m⁻¹, and 1.98±1.52 m² g⁻¹, respectively. However, in winter at Dunhuang PM₁₀, σ_sp, and α were 158.1±261.4 μg m⁻³, 303.3±165.2 M m⁻¹, and 3.17±1.93 m² g⁻¹, respectively, and these values at Dongsheng were 155.7±170.1 μg m⁻³, 304.4±158.1 M m⁻¹, and 2.90±1.72 m² g⁻¹, respectively. σ_sp and α in winter were higher than that in spring at both the sites, which coincides with the characteristics of dust aerosol and pollution aerosol. Overall, the dominant aerosol types in spring and winter at both sites in northern China are dust aerosol and pollution aerosol, respectively.     

Organochlorine pesticides and polybrominated diphenyl ethers in irrigated soils of Beijing, China: Levels, inventory and fate

Limited information on the levels, inventory and fate of Organochlorine pesticides (OCPs) and Polybrominated diphenyl ethers (PBDEs) in the soils irrigated by sewage or wastewater is available. In this study, variation in concentrations, profiles and fate of OCPs and PBDEs were investigated using soil samples collected from a region irrigated by sewage, mixed water and clean water in the east of Beijing, China. No significant variation was observed among groups, except for penta-BDEs. The measured ΣOCPs and ΣPBDEs residues ranged from 6.4 to 171.2 ng g⁻¹ (dw) and 501.9 to 3310.7 pg g⁻¹ (dw), respectively. ΣDDTs and BDE-209 were the most abundant congeners accounting for about 76% of ΣOCPs and 93% of ΣPBDEs. Concentrations of hexachlorocyclohexanes (HCHs), dichlorodiphenyltrichloroethane (DDTs) and its major degradation products, and hexachlorobenzene (HCB) ranged from 1.2 to 11.4 ng g⁻¹ (dw), 4.0 to 155.6 ng g⁻¹ (dw) and 0.3 to 3.4 ng g⁻¹ (dw), respectively. The major DDT degradation products were p,p′-DDT and p,p′-DDE. The major hexachlorocyclohexane (HCH) isomer in irrigated soils is β-HCH, reflecting its higher affinity to solids and resistance to degradation than other isomers. Both α-HCH/β-HCH and p,p′-DDT/p,p′-DDE ratios were log-normally distributed and negatively correlated to log(ΣHCHs) and log(ΣDDTs), respectively, suggesting no significant recent application of OCPs. Individual BDE congeners, ΣPBDEs and ΣOCPs were significantly correlated with total organic carbon (TOC). Moreover, a good correlationship between ΣPBDEs and black carbon (BC) was obtained but not between ΣOCPs and BC. Sewage irrigation did not have obvious effect on their contaminant levels and inventory of OCPs and PBDEs.     

Physicochemical variations in atmospheric aerosols recorded at sea onboard the Atlantic–Mediterranean 2008 Scholar Ship cruise (Part I): Particle mass concentrations,size ratios,and main chemical components

We report on ambient atmospheric aerosols present at sea during the Atlantic–Mediterranean voyage of Oceanic II (The Scholar Ship) in spring 2008. A record was obtained of hourly PM₁₀, PM_2.5, and PM₁ particle size fraction concentrations and 24-h filter samples for chemical analysis which allowed for comparison between levels of crustal particles, sea spray, total carbon, and secondary inorganic aerosols. On-board monitoring was continuous from the equatorial Atlantic to the Straits of Gibraltar, across the Mediterranean to Istanbul, and back via Lisbon to the English Channel. Initially clean air in the open Atlantic registered PM₁₀ levels <10 μg m^?3 but became progressively polluted by increasingly coarse PM as the ship approached land. Away from major port cities, the main sources of atmospheric contamination identified were dust intrusions from North Africa (NAF), smoke plumes from biomass burning in sub-Saharan Africa and Russia, industrial sulphate clouds and other regional pollution sources transported from Europe, sea spray during rough seas, and plumes emanating from islands. Under dry NAF intrusions PM₁₀ daily mean levels averaged 40–60 μg m^?3 (30–40 μg m^?3 PM_2.5; c. 20 μg m^?3 PM₁), peaking briefly to >120 μg m^?3 (hourly mean) when the ship passed through curtains of higher dust concentrations amassed at the frontal edge of the dust cloud. PM₁/PM₁₀ ratios ranged from very low during desert dust intrusions (0.3–0.4) to very high during anthropogenic pollution plume events (0.8–1).     

Quantitative chemical composition and characteristics of aerosols over western India: One-year record of temporal variability

One-year quantitative chemical data set consisting of water-soluble constituents (NH₄⁺, Na⁺, K⁺, Mg²⁺, Ca²⁺, Cl^?, NO₃^?, SO₄^2? and HCO₃^?), crustal and trace elements (Al, Fe, Ca, Mg, K, Mn, Zn, Pb) and carbonaceous species (OC, EC) in ambient aerosols, collected over an urban site located in a high-dust semi-arid region of western India, reveals excellent linear relationship (r² = 0.92; slope = 0.96 ± 0.05) between gravimetrically assessed TSP (total suspended particulates) and chemically analyzed aerosol mass. The TSP abundance ranging from 60 to 250 μg m^?3, over a period of 12 months (January–December), is dominated by mineral dust (～70%); whereas contribution from sea-salts, anthropogenic and carbonaceous species exhibits significant temporal variability depending upon the wind regimes. The mineral dust is enriched in Ca, Mg and Fe with respect to upper continental crust (UCC); whereas Zn and Pb exhibit a characteristic anthropogenic source and high enrichment factors. The carbonaceous species show significant seasonality; with dominance of OC (range: 4.6–28 μg m^?3; average: 12.8 μg m^?3; SD: 6.8) and minor contribution from EC (range: 0.3–4.4 μg m^?3; average: 2.4 μg m^?3; SD: 1.4). The observed concentrations are significantly lower than those reported for the metro cities in South Asia but the OC/EC ratios (range: 4.3–35; average: 8.3; SD: 5.7) are significantly higher than the characteristic ratio (～2–4) reported for the urban atmosphere. Such quantitative chemical characterization of aerosols is essential in assessing their role in atmospheric chemistry and climate change. This study could also be useful in understanding the physical and optical aerosol properties documented from the same site and thus, in validating regional climate models.     

Volcanic sulphate and arctic dust plumes over the North Atlantic Ocean

High time resolution aerosol mass spectrometry measurements were conducted during a field campaign at Mace Head Research Station, Ireland, in June 2007. Observations on one particular day of the campaign clearly indicated advection of aerosol from volcanoes and desert plains in Iceland which could be traced with NOAA Hysplit air mass back trajectories and satellite images. In conjunction with this event, elevated levels of sulphate and light absorbing particles were encountered at Mace Head. While sulphate concentration was continuously increasing, nitrate levels remained low indicating no significant contribution from anthropogenic pollutants. Sulphate concentration increased about 3.8 μg m⁻³ in comparison with the background conditions. Corresponding sulphur flux from volcanic emissions was estimated to about 0.3 TgS yr⁻¹, suggesting that a large amount of sulphur released from Icelandic volcanoes may be distributed over distances larger than 1000 km. Overall, our results corroborate that transport of volcanogenic sulphate and dust particles can significantly change the chemical composition, size distribution, and optical properties of aerosol over the North Atlantic Ocean and should be considered accordingly by regional climate models.     

Spatial character of polychlorinated biphenyls from soil and respirable particulate matter in Taiyuan, China

As one of China’s great metropolises, Taiyuan is affected by heavy chemical industry and manufacture of chemical products, and faces pollution from polychlorinated biphenyls (PCBs). Therefore, this study was conducted to determine the PCB concentrations in various environmental media in Taiyuan. We collected 15 soil samples, 34 respirable particulate matter (PM) samples (17 of PM_2.5 and 17 of PM₁₀) from urban areas of Taiyuan, and measured a total of 144 PCB congeners (including some coeluting PCB congeners). The total PCB concentrations were 51–4.7 × 10³ pg g⁻¹ in soil, 27–1.4 × 10² pg m⁻³ in PM_2.5 and 16–1.9 × 10² pg m⁻³ in PM₁₀. Of the PCB homologues, the dominant PCBs detected in the various media were all tri-CBs. Soil was relatively the most polluted media. Furthermore, principal-component analysis revealed that the major PCB source in Taiyuan may be associated with the main commercial PCB through long-range transmission. Toxic equivalency (TEQ) concentrations (based on ten dioxin-like PCBs) ranged from N.D. to 5.9 × 10⁻³ pg-WHO TEQ g⁻¹ in soil, 2.0 × 10⁻⁴–3.4 × 10⁻³ pg-WHO TEQ m⁻³ and 1.0 × 10⁻⁴–1.2 × 10⁻³ pg-WHO TEQ m⁻³ in PM_2.5 and PM₁₀, respectively. In previous studies, PCBs were not a severe component of contaminant in Taiyuan; however, this study suggested there is a potential threat of human exposure to PCBs for residents of Taiyuan.     

On the contribution of black carbon to the composite aerosol radiative forcing over an urban environment

This paper discusses the extent of Black Carbon (BC) radiative forcing in the total aerosol atmospheric radiative forcing over Pune, an urban site in India. Collocated measurements of aerosol optical properties, chemical composition and BC were carried out for a period of six months (during October 2004 to May 2005) over the site. Observed aerosol chemical composition in terms of water soluble, insoluble and BC components were used in Optical Properties of Aerosols and Clouds (OPAC) to derive aerosol optical properties of composite aerosols. The BC fraction alone was used in OPAC to derive optical properties of BC aerosols. The aerosol optical properties for composite and BC aerosols were separately used in SBDART model to derive direct aerosol radiative forcing due to composite and BC aerosols. The atmospheric radiative forcing for composite aerosols were found to be +35.5, +32.9 and +47.6 Wm^?2 during post-monsoon, winter and pre-monsoon seasons, respectively. The average BC mass fraction found to be 4.83, 6.33 and 4 μg m^?3 during the above seasons contributing around 2.2 to 5.8% to the total aerosol load. The atmospheric radiative forcing estimated due to BC aerosols was +18.8, +23.4 and +17.2 Wm^?2, respectively during the above seasons. The study suggests that even though BC contributes only 2.2–6% to the total aerosol load; it is contributing an average of around 55% to the total lower atmospheric aerosol forcing due to strong radiative absorption, and thus enhancing greenhouse warming.     

Long-term variation of PM2.5 levels and composition at rural, urban, and roadside sites in Hong Kong: Increasing impact of regional air pollution

Long-term study of air pollution plays a decisive role in formulating and refining pollution control strategies. In this study, two 12-month measurements of PM_2.5 mass and speciation were conducted in 00/01 and 04/05 to determine long-term trend and spatial variations of PM_2.5 mass and chemical composition in Hong Kong. This study covered three sites with different land-use characteristics, namely roadside, urban, and rural environments. The highest annual average PM_2.5 concentration was observed at the roadside site (58.0±2.0 μg m⁻³ (average±2σ) in 00/01 and 53.0±2.7 μg m⁻³ in 04/05), followed by the urban site (33.9±2.5 μg m⁻³ in 00/01 and 39.0±2.0 μg m⁻³ in 04/05), and the rural site (23.7±1.9 μg m⁻³ in 00/01 and 28.4±2.4 μg m⁻³ in 04/05). The lowest PM_2.5 level measured at the rural site was still higher than the United States’ annual average National Ambient Air Quality Standard of 15 μg m⁻³. As expected, seasonal variations of PM_2.5 mass concentration at the three sites were similar: higher in autumn/winter and lower in summer. Comparing PM_2.5 data in 04/05 with those collected in 00/01, a reduction in PM_2.5 mass concentration at the roadside (8.7%) but an increase at the urban (15%) and rural (20%) sites were observed. The reduction of PM_2.5 at the roadside was attributed to the decrease of carbonaceous aerosols (organic carbon and elemental carbon) (>30%), indicating the effective control of motor vehicle emissions over the period. On the other hand, the sulfate concentration at the three sites was consistent regardless of different land-use characteristics in both studies. The lack of spatial variation of sulfate concentrations in PM_2.5 implied its origin of regional contribution. Moreover, over 36% growth in sulfate concentration was found from 00/01 to 04/05, suggesting a significant increase in regional sulfate pollution over the years. More quantitative techniques such as receptor models and chemical transport models are required to assess the temporal variations of source contributions to ambient PM_2.5 mass and chemical speciation in Hong Kong.     

Modeling the spectral optical properties of ammonium sulfate and biomass burning aerosols: parameterization of relative humidity effects and model results

The importance of including the global and regional radiative effects of aerosols in climate models has increasingly been realized. Accurate modeling of solar radiative forcing due to aerosols from anthropogenic sulfate and biomass burning emissions requires adequate spectral resolution and treatment of spatial and temporal variability. The variation of aerosol spectral optical properties with local relative humidity and dry aerosol composition must be considered. Because the cost of directly including Mie calculations within a climate model is prohibitive, parameterizations from off-line calculations must be used. Starting from a log-normal size distribution of dry ammonium sulfate, we developed optical properties for tropospheric sulfate aerosol at 15 relative humidities up to 99%. The resulting aerosol size distributions were then used to calculate bulk optical properties at wavelengths between 0.175 and 4 μm. Finally, functional fits of optical properties were made for each of 12 wavelength bands as a function of relative humidity. Significant variations in optical properties occurred across the total solar spectrum. Relative increases in specific extinction and asymmetry factor with increasing relative humidity became larger at longer wavelengths. Significant variation in single-scattering albedo was found only in the longest near-IR band. This is also the band with the lowest single scattering albedo. A similar treatment was done for aerosols from biomass burning. In this case, two size distributions were considered. One was based on a distribution measured for Northern Hemisphere temperate forest fires while the second was based on a measured size distribution for tropical fires. Equilibrium size distributions and compositions were calculated for 15 relative humidities and five black carbon fractions. Mie calculations and band averages of optical properties were done for each of the resulting 75 cases. Finally, fits were made for each of 12 spectral bands as functions of relative humidity and black carbon fraction. These optical properties result in global average forcing from anthropogenic sulfate aerosols of −0.81 Wm^-2. The global average forcing for biomass aerosols ranged from −0.23 to −0.25 Wm^-2 depending on the assumed size distribution, while fossil fuel organic and black carbon are estimated to heat the atmosphere by about 0.16 Wm^-2.     

Impact of the Saharan dust outbreaks on the ambient levels of total suspended particles (TSP) in the marine boundary layer (MBL) of the Subtropical Eastern North Atlantic Ocean

Six years (1998–2003) of measurements of ambient air concentrations of total suspended particulate (TSP) measured at a rural background monitoring station in Tenerife (Canary Islands), the El Río station (ER, 28°08′35″N, 16°39′20″W, 500 m a.s.l.) were studied. African dust outbreaks were objectively identified using a new quantitative tool, called the African Index. This index indicates the percentage of time that an air mass remained over an African region at one of three possible height intervals of the lower troposphere. After identifying these episodes, a study of the background TSP levels at the ER station and of direct and indirect (those which cause vertical deposition of dust) African air mass intrusion impacts was performed. Taking into account both direct and indirect episodes, a total of 322 days of African dust intrusion were objectively identified (a mean of 54 episodes per year) in the period 1998–2003, some of them caused by “transition episodes” or “return African air masses”. A subjective method confirmed that 256 of these days were caused by direct impacts of African dust on the ER station. A mean TSP value of 21.6 μg m⁻³ was found at the station during this period. All the episodes occurred when the TSP concentration was >28.5 μg m⁻³. The TSP background (14 μg m⁻³) can be assumed to be representative of the MBL of the Eastern North Atlantic subtropical region. The highest number of dust gravitational settlement (or indirect) episodes occurs in summer, but the highest contribution of these episodes to the TSP levels is in March with a monthly mean TSP contribution of up to 30.5 μg m⁻³.     

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

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

A global assessment of chromium pollution using sperm whales (Physeter macrocephalus) as an indicator species

Chromium (Cr) is a well-known human carcinogen and a potential reproductive toxicant, but its contribution to ocean pollution is poorly understood. The aim of this study was to provide a global baseline for Cr as a marine pollutant using the sperm whale (Physeter macrocephalus) as an indicator species. Biopsies were collected from free-ranging whales around the globe during the voyage of the research vessel The Odyssey. Total Cr levels were measured in 361 sperm whales collected from 16 regions around the globe detectable levels ranged from 0.9 to 122.6 μg Cr g tissue⁻¹ with a global mean of 8.8 ± 0.9 μg g⁻¹. Two whales had undetectable levels. The highest levels were found in sperm whales sampled in the waters near the Islands of Kiribati in the Pacific (mean = 44.3 ± 14.4) and the Seychelles in the Indian Ocean (mean = 19.5 ± 5.4 μg g⁻¹). The lowest mean levels were found in whales near the Canary Islands (mean = 3.7 ± 0.8 μg g⁻¹) and off of the coast of Sri Lanka (mean = 3.3 ± 0.4 μg g⁻¹). The global mean Cr level in whale skin was 28-times higher than mean Cr skin levels in humans without occupational exposure. The whale levels were more similar to levels only observed previously in human lung tissue from workers who died of Cr-induced lung cancer. We conclude that Cr pollution in the marine environment is significant and that further study is urgently needed.