Altitude distribution of aerosols over Southeast Arabian Sea coast during pre-monsoon season: Elevated layers,long-range transport and atmospheric radiative heating

Every year, during the pre-monsoon period (March–May), a pronounced increase in aerosol optical depth (AOD) is observed over the eastern Arabian Sea, which is attributed to the transport of continental aerosols. This paper presents the altitude distribution of tropospheric aerosols, characteristics of elevated aerosol layers and aerosol radiative heating of the atmosphere during the pre-monsoon season over Trivandrum (8.5°N, 77°E), a station located at the southwest coast of Indian peninsula which is covered by the eastern Arabian Sea plume. Altitude profiles of aerosol backscatter coefficient (β_a) and linear depolarization ratio (LDR) reveal two distinct aerosol layers persisting between 0–2 km and 2–4 km. The layer at 2–4 km, which contributes about 25% of the AOD during polluted conditions, contains significant amount of non-spherical aerosols. This layer is prominent only when the advection of dry airmass occurs from the northern parts of the Indian subcontinent and northern Arabian Sea. Role of long-range transport in the development of this aerosol layer is further confirmed using latitude–altitude cross-section of β_a observed by CALIPSO. Aerosol content in the layer below 2 km is large when advection of air occurs from the north and east Arabian Sea and is significantly small when it occurs from the southwest Arabian Sea or Indian Ocean. During the highly polluted conditions, aerosols tend to increase the diurnal mean atmospheric radiative heating rate by ～0.8 K day^?1 at 500 m and 0.3 K day^?1 at 3 km, which are about 80% and 30% of the respective radiative heating in the aerosol-free atmosphere.     

Influence of accidental fire on black carbon aerosol concentrations over an urban environment

Carbonaceous aerosols are emitted by combustion sources and may influence the climate by altering the radiation balance of the atmosphere. Carbonaceous particles exist mainly in the accumulation mode and thus may be transported over long distances. The present study deals with the impact of anthropogenic activity associated with accidental fires on the black carbon aerosol concentrations over an urban environment, namely Hyderabad, India. Black carbon aerosol loading in association with meteorological parameters on a normal day, an accident day and a post-accident day have been analysed. Diurnal variations of black carbon aerosols on a normal day suggest that black carbon aerosol concentrations increased by a factor of about 2 during morning and evening hours compared with afternoon hours. A drastic increase in black carbon aerosol loading was found during an accident day compared with a normal day. An immediate return to normal black carbon concentration was found during the post-accident day. Black carbon aerosol loading in relation to rainfall is also discussed in the paper.     

Effects of radiative forcing by black carbon aerosol on spring rainfall decrease over Southeast Asia

The effects of black carbon (BC) aerosol radiative forcing on spring rainfall in Southeast Asia are studied using numerical simulations with the NASA finite-volume General Circulation Model (fvGCM) forced with monthly varying three-dimensional aerosol distributions from the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART).During the boreal spring, March–April–May (MAM), BC from local emissions accumulates over Southeast Asia. The BC aerosol layer, which extends from the surface to higher elevation above planetary boundary layer (PBL), absorbs solar radiation and heats the mid-troposphere through a semi-direct effect over regions of large aerosol optical thickness (AOT) and thereby significantly perturbs large-scale and meridional circulations. Results show that anomalous precipitation patterns and associated large-scale circulations induced by radiative forcing by BC aerosol can explain observed precipitation reductions, especially over Southeast Asia. Therefore, BC aerosol forcing may be one of the important factors affecting the spring rainfall trend over Southeast Asia.     

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.     

Seasonal variation of black carbon aerosols over a tropical urban city of Pune,India

Black carbon (BC) aerosols were monitored continuously at Pune, a tropical urban location in southwest India, using aethalometer AE-42 model. Results of the data for the 1-year period (January to December 2005) have been discussed here. Seasonal and diurnal variations of BC in relation to changes in the regional meteorological conditions and local boundary layer characteristics have been studied along with the mass fraction of BC to the total suspended particulates (TSP) in different months. Also, using the Hysplit model, back-trajectories are studied to assess the sources for transported BC particles. The data collected during January to December 2005 indicated that annual average BC concentration (4.1 μg m⁻³) at Pune was comparable to that reported for other urban locations in southern Indian region. During winter season, BC concentrations were maximum (about 80% more than annual mean), mainly due to prevailing meteorological conditions like low wind speeds and low ventilation coefficients; as well as due to the transport from northeast regions. Minimum BC concentrations were observed during monsoon season (about 68% less than annual mean), which could be attributed to the wash-out effects due to precipitation as well as due to southwesterly winds coming from marine areas. Diurnal variation of BC showed two peaks, one in morning and another in the evening, which are mostly related to the daily changes in the local boundary layer. However, the intensity of local traffic emissions could have some impact on the magnitude of these peaks. BC aerosols formed about 2.3% of the total aerosol mass fraction at Pune.     

MODIS derived fire characteristics and aerosol optical depth variations during the agricultural residue burning season, north India

Agricultural residue burning is one of the major causes of greenhouse gas emissions and aerosols in the Indo-Ganges region. In this study, we characterize the fire intensity, seasonality, variability, fire radiative energy (FRE) and aerosol optical depth (AOD) variations during the agricultural residue burning season using MODIS data. Fire counts exhibited significant bi-modal activity, with peak occurrences during April-May and October-November corresponding to wheat and rice residue burning episodes. The FRE variations coincided with the amount of residues burnt. The mean AOD (2003-2008) was 0.60 with 0.87 (+1σ) and 0.32 (−1σ). The increased AOD during the winter coincided well with the fire counts during rice residue burning season. In contrast, the AOD-fire signal was weak during the summer wheat residue burning and attributed to dust and fossil fuel combustion. Our results highlight the need for ‘full accounting of GHG’s and aerosols’, for addressing the air quality in the study area.     

Local circulation and aerosol water-soluble ions--a case study in Taiwan during Mei-yu season

The Mei-yu (plum rain) season is a short but important period when the weather changes from spring to summer in Taiwan. In this study, size-segregated aerosols were collected alternately at 5 sampling sites in northwestern Taiwan from June 16 to 24, 1994. For the first time in Taiwan, this study revealed the aerosol mass spectra and water-soluble ions in the Mei-yu season. For all samples, a bi-modal aerosol mass spectra was found with modal diameters at 3.2 and 0.32 microm, respectively. The aerosol samples were able to be divided into different groups to show their mass and ion spectra according to the calculated 5-hr backward air trajectory. The utilization of enrichment factors showed that aerosol Cl-, Na+, and Mg2+ for all sizes, and super-micron SO4(2-) were related to the sea. Both the scheme of "chlorine loss" (Ohta and Okita, 1990) and a multivariate analysis (Thurston and Spengler, 1985) for categorizing water-soluble ions showed that sea-salts were major contributors in the prevalence of a sea breeze. In contrast, the secondary salts were significant for land breeze and a mix of land-sea breeze. In conclusion, the influence of local circulation on the distribution of aerosol mass and ionic species was found to be prominent.     

Elemental composition of aerosol in the Nam Co region,Tibetan Plateau,during summer monsoon season

In order to investigate the chemical characteristics of atmospheric aerosols in a remote region of the Tibetan Plateau, total suspended particles were collected continuously at the Nam Co Comprehensive Observation and Research Station from July to October 2005. The PIXE analytical results showed that Si, Ca, Fe, Al, K, and S were the major components of aerosols, ranging from 82 (K)–550 (Si) ng m⁻³. The mean elemental concentrations were comparable with those from other remote sites and significantly lower than those from megacities (e.g. Beijing). The very low presence of anthropogenic elements demonstrates that the Nam Co region is an ideal background site for atmospheric monitoring. Crustal enrichment factor (EF) calculation indicated that several anthropogenic heavy metals (Cr, Ni, Cu, Zn, As) are transported long distances atmospherically. The backward air mass trajectory analysis suggests that South Asia may be the source region of those pollutants.     

The effect of aerosol optical depth on rainfall with reference to meteorology over metro cities in India

Rainfall is a key link in the global water cycle and a proxy for changing climate; therefore, proper assessment of the urban environment’s impact on rainfall will be increasingly important in ongoing climate diagnostics and prediction. Aerosol optical depth (AOD) measurements on the monsoon seasons of the years 2008 to 2010 were made over four metro regional hotspots in India. The highest average of AOD was in the months of June and July for the four cities during 3 years and lowest was in September. Comparing the four regions, Kolkata was in the peak of aerosol contamination and Chennai was in least. Pearson correlation was made between AOD with climatic parameters. Some changes in the parameters were found during drought year. Temperature, cloud parameters, and humidity play an important role for the drought conditions. The role of aerosols, meteorological parameters, and their impacts towards the precipitation during the monsoon was studied.     

The vertical profile of atmospheric heating rate of black carbon aerosols at Kanpur in northern India

Altitude profiles of the mass concentrations of aerosol black carbon (BC) and composite aerosols were obtained from the collocated measurements of these quantities onboard an aircraft, over the urban area of Kanpur, in the Ganga basin of northern India during summer, for the first time in India. The enhancement in the mean BC concentration was observed at ∼1200 m in the summer, but the vertical gradient of BC concentration is less than the standard deviation at that altitude. The difference in the BC altitude profile and columnar concentration in the winter and summer is attributed to the enhanced turbulent mixing within the boundary layer in summer. This effect is more conspicuous with BC than the composite aerosols, resulting in an increase in the BC mass fraction (F_BC) at higher levels in summer. This high BC fraction results in an increase in the lower atmospheric heating rate in both the forenoon, FN and afternoon, AN, but with contrasting altitude profile. The FN profile shows fluctuating trend with highest value (2.1 K day⁻¹) at 300 m and a secondary peak at 1200 m altitudes, whereas the AN profile shows increasing trend with highest value (1.82 K day⁻¹) at 1200 m altitude.     

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.     

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.     

Size-resolved aerosol chemical composition over the Italian Peninsula during typical summer and winter conditions

In the frame of the MIUR-AEROCLOUDS project (Study of Direct and Indirect Aerosol Effects on Climate), night-time and daytime size-segregated aerosol samples were collected concurrently at five different sites (near-city, urban, rural, marine and mountain background sites). The paper reports on the daily evolution of the main aerosol chemical characteristics as a function of particle size in different environments over the Italian Peninsula, spanning from the Po Valley to the south Tyrrhenian coast.Two 4-day intensive observation periods (IOPs) were undertaken in July 2007 and February 2008, under meteorological conditions typical of the summer and winter climate for Italy.In the summer IOP, under stable atmospheric conditions, at the low-altitude continental sites the diurnal evolution of the planetary boundary layer (PBL), induces an atmospheric dilution effect driving the particulate matter (PM) concentrations, while, at the mountain site, it determines the upward motion of polluted air masses from the Po Valley PBL in daytime.The fine fraction was dominated by ammonium salts and carbonaceous matter (water-soluble organic matter, WSOM, and water-insoluble carbonaceous matter, WINCM). High concentrations of ammonium sulphate and WSOM due to enhanced photochemical activity constituted the background aerosol composition over the whole country, whereas, ammonium nitrate and WINCM were more associated to local emissions (e.g. urban site with concentrations peaking in the finest size range due to strong local traffic-related sources of ultrafine particles).During the winter IOP in the Po Valley, the shallow PBL depths and low wind velocity, especially at night, favoured the condensation of semi-volatile species (i.e. organic matter and ammonium nitrate), causing the high fine PM concentration observed at ground level.     

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.     

Study of aerosol transport through precipitation chemistry over Arabian Sea during winter and summer monsoons

Precipitation samples over the Arabian Sea collected during Arabian Sea Monsoon Experiment (ARMEX) in 2002–2003 were examined for major water soluble components and acidity of aerosols during the period of winter and summer monsoon seasons. The pH of rain water was alkaline during summer monsoon and acidic during winter monsoon. Summer monsoon precipitation showed dominance of sea-salt components (∼90%) and significant amounts of non-sea salt (nss) Ca²⁺ and SO₄²⁻. Winter monsoon precipitation samples showed higher concentration of NO₃⁻ and NH₄⁺ compared to that of summer monsoon, indicating more influence of anthropogenic sources. The rain water data is interpreted in terms of long-range transport and background pollution. In summer monsoon, air masses passing over the north African and Gulf continents which may be carrying nss components are advected towards the observational location. Also, prevailing strong southwesterly winds at surface level produced sea-salt aerosols which led to high sea-salt contribution in precipitation. While in winter monsoon, it was observed that, air masses coming from Asian region towards observational location carry more pollutants like NO₃⁻and nss SO₄²⁻ that acidify the precipitation.     

Evaluation of the MODIS aerosol optical depth retrieval over different ecosystems in China during EAST-AIRE

The accuracy of the Moderate Resolution Imaging Spectroradiometer's (MODIS) aerosol products is still uncertain in China, due to a lack of validation by long-term and large-scale ground-based observations. In this paper, the MODIS aerosol optical depth (AOD) product is evaluated using Chinese Sun Hazemeter Network (CSHNET) data as ground truths over different ecological regions in China during the East Asian Study of Tropospheric Aerosols—an International Regional Experiment (EAST-AIRE). The evaluation results show very large differences in the MODIS AOD retrieval between different ecosystems and geographic locations. The most agreement between the MODIS data and that of the CSHNET was in farmland sites in central-southern China, where high correlation (R>0.82) and large percentages (R2>72%) within the expected error lines issued by NASA were found. In temperate forest, coastal regions, and northeast and central farmlands, there appeared moderate agreement, with R∼0.64–0.80 and 45–73% of retrieval data falling within the expected errors. The poorest agreement existed in northern arid and semiarid regions, in remote northeast farmlands, in the Tibetan and Loess Plateau, and in southern forests, with 13–54% of retrieval data falling within the expected errors. In addition, the MODIS AOD retrievals were significantly overestimated in the northern arid and semiarid regions and underestimated in remote northeast farmlands and southern forests.     

Spatial distribution and seasonal variation of char-EC and soot-EC in the atmosphere over China

A previous study on PM_2.5 carbonaceous aerosols measured with the thermal optical reflectance (TOR) method in fourteen Chinese cities is extended by subdividing total EC into char-EC and soot-EC. Average char-EC concentrations show great differences between the fourteen cities and between winter and summer periods, with concentrations of 8.67 and 2.41 μg m^?3 in winter and summer, respectively. Meanwhile spatial and seasonal soot-EC variations are small, with average concentrations of 1.26 and 1.21 μg m^?3 in winter and summer, respectively. Spatial and temporal distributions of char-EC, similar to EC, are mainly influenced by local fuel consumption, as well as the East Asian monsoon and some meteorological factors such as the mixing height and wet precipitation. The small spatial and seasonal variation of soot-EC is consistent with its regional-to-global dispersion, which may suggest that soot carbon is not local carbon, but regional carbon. Char-EC/soot-EC ratios show summer minimum and winter maximum in all cities, which is in good agreement with the difference in source contributions between the two periods. As OC/EC ratio is affected by the formation of the secondary organic aerosol (SOA), char-EC/soot-EC ratio is a more effective indicator for source identification of carbonaceous aerosol than previously used OC/EC ratio.     

Role of black carbon in the distribution of polychlorinated dibenzo-p-dioxins/dibenzofurans in aged field-contaminated soils

Floodplain soils containing elevated levels of polychlorinated dibenzo-p-dioxins/dibenzofurans (PCDD/Fs) were collected from several locations along the Tittabawassee River (Michigan, USA). The PCDD/F profiles of these soils exhibited distinct congener patterns consistent with byproducts from either chloralkali manufacturing or chlorophenols productions. Black carbon (BC) particles were isolated for the first time from floodplain soil impacted by PCDD/Fs. Petrographic analysis showed that BC particles, including coal, oxidized coal, metallurgical coke, depositional carbon, coal tar/pitch, cenosphere, and charcoal, comprised approximately 30% by volume of the organic fraction with size range of 250 μm-2000 μm from a typical floodplain soil. The BC particles with anthropogenic origin such as pitch and coke associated with the chloralkali production process served as both the source and subsequent transporter for the highly hydrophobic PCDD/Fs. These anthropogenic BC particles were enriched with high levels of PCDFs, containing approximately 1000-fold the concentration found in the bulk soil. The strong association of PCDD/Fs with anthropogenic BC directly impacts the physicochemical and biological availability thus the risk associated with these hydrophobic organochlorines in soils and sediments.     

High carbon monoxide concentrations during the rainy season in Campo Grande, in central Brazil

This work describes an event of unusually large mixing ratios of carbon monoxide, CO, observed during a typical rainy season time period in central Brazil, when concentrations are expected to be at low levels. CO measurements were performed in Campo Grande (20.02 degrees S; 54.5 degrees W), from July 2001 to October 2002, covering entire periods of the dry and wet seasons. From January to June, average CO was 131 parts per billion by volume (ppbv). During November/December, average CO is about 180 ppbv. On November 13, 521.9 and 565.6 ppbv were observed. It is shown that for this special event, in which there was practically no fire activity at or near the site, air parcels reaching the site were enriched with fire products from regions much further north, near the equatorial region, where the fire activity is delayed in time, compared to central Brazil.