The Danish eulerian hemispheric model — a three-dimensional air pollution model used for the arctic

A three-dimensional Eulerian hemispheric air pollution model, the Danish Eulerian Hemispheric Model (DEHM), is in development at the National Environmental Research Institute (NERI). The model has been used to study long-range transport of air pollution in the Northern Hemisphere. The present version of the model includes long-range transport of sulphur dioxide (SO₂) and particulate sulphate (SC₄²⁻. The chemistry in the model is described by a simple linear oxidation of SO₂ to SO₄²⁻, and the wet deposition of SO₂ and SO₄⁻ is estimated based on the amount of precipitation, which is calculated from the contents of liquid cloud water (see Christensen, Air Pollution Modelling and its Applicatioons, Vol. X, pp. 119–127, Vol. XI, pp. 249–256, Plenum press, New York; 1995, Ph.D. thesis, National Environmental Research Institute, Denmark). The model has been used to study the air pollution in the Arctic. Results from yr simulation with an analysis of the results is presented: the model results are verified by comparisons, to measurements not only from the Arctic region but also from Europe and Canada. Some examples of episodes in the Arctic including analysis of the meteorological conditions during the episodes are presented. Finally, the model has been used to estimate the contribution from the different source regions on the northern hemisphere to the Arctic sulphur pollution.     

A multi-component data assimilation experiment directed to sulphur dioxide and sulphate over Europe

Fine particulate matter (PM) is relevant for human health and its components are associated with climate effects. The performance of chemistry transport models for PM, its components and precursor gases is relatively poor. The use of these models to assess the state of the atmosphere can be strengthened using data assimilation. This study focuses on simultaneous assimilation of sulphate and its precursor gas sulphur dioxide into the regional chemistry transport model LOTOS–EUROS using an ensemble Kalman filter. The process of going from a single component setup for SO₂ or SO₄ to an experiment in which both components are assimilated simultaneously is illustrated. In these experiments, solely emissions, or a combination of emissions and the conversion rates between SO₂ and SO₄ were considered uncertain. In general, the use of sequential data assimilation for the estimation of the sulphur dioxide and sulphate distribution over Europe is shown to be beneficial. However, the single component experiments gave contradicting results in direction in which the emissions are adjusted by the filter showing the limitations of such applications. The estimates of the pollutant concentrations in a multi-component assimilation have found to be more realistic. We discuss the behavior of the assimilation system for this application. The model uncertainty definition is shown to be a critical parameter. The increased complexity associated with the simultaneous assimilation of strongly related species requires a very careful specification of the experiment, which will be the main challenge in the future data assimilation applications.     

Deposition of sulphur,nitrogen and acidity in precipitation over Ireland: chemistry,spatial distribution and long-term trends

The chemical composition of pollutant species in precipitation sampled daily or weekly at 10 sites in Ireland for the five-year period, 1994–1998, is presented. Sea salts accounted for 81% of the total ionic concentration. Approximately 50% of the SO₄²⁻ in precipitation was from sea-salt sources. The proportion of sea salts in precipitation decreased sharply eastwards. In contrast, the concentration of NO₃⁻ and the proportion of non-sea-salt SO₄²⁻ increased eastwards reflecting the closer proximity to major emission sources. The mean (mol_c) ratio of SO₄²⁻:NO₃⁻ was 1.6 for all sites, indicating that SO₄²⁻ was the major acid anion.The spatial correlation between SO₄²⁻, NO₃⁻ and NH₄⁺ concentrations in precipitation was statistically significant. The regional trend in NO₃⁻ concentration was best described by linear regression against easting. SO₄²⁻ concentration followed a similar pattern. However, the regression was improved by inclusion of elevation. Inclusion of northing in the regression did not significantly improve any of the relationships except for NH₄⁺, indicating a significant increase in concentrations from northwest to southeast.The spatial distribution of deposition fluxes showed similar gradients increasing from west and southwest to east and northeast. However, the pattern of deposition shows the influence of precipitation volume in determining the overall input. Mean depositions of sulphur and nitrogen in precipitation were ≈30 ktonnes S yr⁻¹ and 48 ktonnes N yr⁻¹ over the five-year period, 1994–1998, for Ireland.Least-squares linear regression analysis indicated a slight decreasing trend in precipitation concentrations for SO₄²⁻ (20%), NO₃⁻ (13%) and H⁺ (24%) and a slight increasing trend for NH₄⁺ (15%), over the period 1991–1998.     

A scheme for black carbon and sulphate aerosols tested in a hemispheric scale,Eulerian dispersion model

Production, transport and deposition of sulphate and black carbon (BC) are simulated separating aerosol modes by production mechanisms, thus facilitating calculation of aerosol physical properties. The scheme uses explicit sulphur chemistry with prescribed oxidants and aerosol transformation based on Brownian coagulation rates, and is implemented in a 3-D, hemispheric-scale transport model with off-line meteorology from ECMWF. The components are DMS, SO₂, sulphate and BC. Simulations are made for the year 1988. Predicted results for sulphate agree well with the measurements, except for considerable underestimations in the Arctic. In Europe SO₂ is slightly overestimated and sulphate is slightly underestimated in cold seasons, whilst trends are less clear in North America. Compared to many other models, we estimate a smaller effective oxidation rate for SO₂ due to reduced rates in cold clouds; a shorter turnover time for sulphate (3.7 d) due to a probably too large below-cloud scavenging ratio; and slightly smaller sulphate column burdens. Our BC results are similar to Liousse et al.’s (1996, J. Geophys. Res. 101, 19.411–19.432) except in USA, whilst the concentrations in remote areas and the turnover time (3.7 d) are considerably smaller than Cooke and Wilson’s (1996, J. Geophys. Res. 101, 190.395–19.409). Agreements with available measurements are quite close to large anthropogenic emissions (including USA), but they are considerably underestimated in Arctic winter. Transition from hydrophobic to hydrophilic BC due to coagulation is swift (6% h^-1). Sensitivity tests emphasize that sub-cloud scavenging coefficients rely on careful assumptions about size distributions, and that more research is needed on sulphate production in ice-clouds. Emphasis should also be put on production of sulphate and hydrophilic BC boundary-layer clouds; inclusion of hydrophobic accumulation mode BC and sub-grid transition to hydrophilic BC in emitting grid squares.     

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.     

Characteristics and origins of air pollutants in Wuhan,China, based on observations and hybrid receptor models

To identify the characteristics of air pollutants and factors attributing to the formation of haze in Wuhan, this study analyzed the hourly observations of air pollutants (PM_2.5, PM₁₀, NO₂, SO₂, O₃, and CO) from March 1, 2013, to February 28, 2014, and used hybrid receptor models for a case study. The results showed that the annual average concentrations for PM_2.5, PM₁₀, NO₂, SO₂, O₃, and CO during the whole period were 89.6 μg m^?3, 134.9 μg m^?3, 54.9 μg m^?3, 32.4 μg m^?3, 62.3 μg m^?3, and 1.1 mg m^?3, respectively. The monthly variations revealed that the peak values of PM_2.5, PM₁₀, NO₂, SO₂, and CO occurred in December because of increased local emissions and severe weather conditions, while the lowest values occurred in July mainly due to larger precipitation. The maximum O₃ concentrations occurred in warm seasons from May to August, which may be partly due to the high temperature and solar radiation. Diurnal analysis showed that hourly PM_2.5, PM₁₀, NO₂, and CO concentrations had two ascending stages accompanying by the two traffic peaks. However, the O₃ concentration variations were different with the highest concentration in the afternoon. A case study utilizing hybrid receptor models showed the significant impact of regional transport on the haze formation in Wuhan and revealed that the mainly potential polluted sources were located in the north and south of Wuhan, such as Baoding and Handan in Hebei province, and Changsha in Hunan province. Implications: Wuhan city requires a 5% reduction of the annual mean of PM_2.5 concentration by the end of 2017. In order to accomplish this goal, Wuhan has adopted some measures to improve its air quality. This work has determined the main pollution sources that affect the formation of haze in Wuhan by transport. We showed that apart from the local emissions, north and south of Wuhan were the potential sources contributing to the high PM_2.5 concentrations in Wuhan, such as Baoding and Handan in Hebei province, Zhumadian and Jiaozuo in Henan province, and Changsha and Zhuzhou in Hunan province.     

Modelling the atmospheric transport and deposition of sulphur and nitrogen over the United Kingdom and assessment of the influence of SO2 emissions from international shipping

A statistical Lagrangian atmospheric transport model was used to generate annual maps of deposition of sulphur and oxidised and reduced nitrogen for the UK at a 5×5 km² resolution. The model was run using emissions for the year 2002. The model was compared with measurements of gas concentrations (SO₂, NO_x, HNO₃ and NH₃) and of wet deposition and aerosol concentrations of SO₄²⁻, NO₃⁻ and NH₄⁺ from national monitoring networks. Good correlation was obtained, demonstrating that the model is capable of accurately estimating the mass balance and spatial distribution of sulphur and nitrogen compounds in the atmosphere. A future emissions scenario for the year 2020 was used to test the influence of shipping emissions on sulphur deposition in the UK. The results show that, if shipping emissions are assumed to increase at a rate of 2.5% per year, their relative contribution to sulphur deposition is expected to increase from 9% to 28% between 2002 and 2020. The model was compared to both a European scale and a global scale chemical transport model and found to give broad agreement with the magnitude and location of sulphur deposition associated with shipping emissions. Enforcement of the MARPOL convention to reduce the sulphur content in marine fuel to 1% was estimated to result in a 6% reduction in total sulphur deposition to the UK for the year 2020. The percentage area of sensitive habitats with exceedance of critical loads for acidity in the UK was predicted to decrease by 1% with the implementation of the MARPOL convention.     

Sulphate aerosol size distributions at Mumbai,India, during the INDOEX-FFP (1998)

Sulphate size distributions were measured at the coastal station of Mumbai (formerly Bombay) through 1998, during the Indian ocean experiment (INDOEX) first field phase (FFP), to fill current gaps in size-resolved aerosol chemical composition data. The paper examines meteorological, seasonal and source-contribution effects on sulphate aerosol and discusses potential effects of sulphate on regional climate. Sulphate size-distributions were largely trimodal with a condensation mode (mass median aerodynamic diameter or MMAD 0.6 μm), a droplet mode (MMAD 1.9–2.4 μm) and a coarse mode (MMAD 5 μm). Condensation mode sulphate mass-fractions were highest in winter, consistent with the high meteorological potential for gas-to-particle conversion along with low relative humidity (RH). The droplet mode concentrations and MMADs were larger in the pre-monsoon and winter than in monsoon, implying sulphate predominance in larger sized particles within this mode. In these seasons the high RH, and consequently greater aerosol water in the droplet mode, would favour aerosol-phase partitioning and reactions of SO₂. Coarse mode sulphate concentrations were lowest in the monsoon, when continental contribution to sulphate was low and washout was efficient. In winter and pre-monsoon, coarse mode sulphate concentrations were somewhat higher, likely from SO₂ gas-to-particle conversion. Low daytime sulphate concentrations with a large coarse fraction, along with largely onshore winds, indicated marine aerosol predominance. High nighttime sulphate concentrations and a coincident large fine fraction indicated contributions from anthropogenic/industrial sources or from gas-to-particle conversion. Monthly mean sulphate concentrations increased with increasing SO₂ concentrations, RH and easterly wind direction, indicating the importance of gas-to-particle conversion and industrial sources located to the east. Atmospheric chemistry effects on sulphate size distributions in Mumbai, indicated by this data, must be further examined.     

Air concentrations and wet deposition of major inorganic ions at five non-urban sites in China, 2001–2003

Air and precipitation measurements at five sites were undertaken from 2001 to 2003 in four different provinces in China, as part of the acid rain monitoring program IMPACTS. The sites were located in Tie Shan Ping (TSP) in Chongqing, Cai Jia Tang (CJT) in Hunan, Lei Gong Shan (LGS) and Liu Chong Guan (LCG) in Guizhou and Li Xi He (LXH) in Guangdong. The site characteristics are quite varied with TSP and LCG located relatively near big cites while the three others are situated in more regionally representative areas. The distances to urban centres are reflected in the air pollution concentrations, with annual average concentrations of SO₂ ranging from 0.5 to above 40 μg S m⁻³. The main components in the airborne particles are (NH₄)₂SO₄ and CaSO₄. Reduced nitrogen has a considerably higher concentration level than oxidised nitrogen, reflecting the high ammonia emissions from agriculture. The gas/particle ratio for the nitrogen compounds is about 1:1 at all the three intensive measurement sites, while for sulphur it varies from 2.5 to 0.5 depending on the distance to the emission sources. As in air, the predominant ions in precipitation are sulphate, calcium and ammonium. The volume weighted annual concentration of sulphate ranges from about 70 μeq l⁻¹ at the most rural site (LGS) to about 200 μeq l⁻¹ at TSP and LCG. The calcium concentration ranges from 25 to 250 μeq l⁻¹, while the total nitrogen concentration is between 30 and 150 μeq l⁻¹; ammonium is generally twice as high as nitrate. China's acid rain research has traditionally been focused on urban sites, but these measurements show a significant influence of long range transported air pollutants to rural areas in China. The concentration levels are significantly higher than seen in most other parts of the world.     

Variability of SO2, CO,and light hydrocarbons over a megacity in Eastern India: effects of emissions and transport

The Indo-Gangetic plain (IGP) has received extensive attention of the global scientific community due to higher levels of trace gases and aerosols over this region. Satellite retrievals and model simulations show that, in particular, the eastern part IGP is highly polluted. Despite this attention, in situ measurements of trace gases are very limited over this region. This paper presents measurements of SO₂, CO, CH₄, and C₂–C₅ NMHCs during March 2012–February 2013 over Kolkata, a megacity in the eastern IGP, with a focus on processes impacting their levels. The mean SO₂ and C₂H₆ concentrations during winter and post-monsoon periods were eight and three times higher compared to pre-monsoon and monsoon. Early morning enhancements in SO₂ and several NMHCs during winter connote boundary layer effects. Daytime elevations in SO₂ during pre-monsoon and monsoon suggest impacts of photo-oxidation. Inter-species correlations and trajectory analysis evince transport of SO₂ from regional combustion sources (e.g., coal burning in power plants, industries) along the east of the Indo-Gangetic plain impacting SO₂ levels at the site. However, C₂H₂ to CO ratio over Kolkata, which are comparable to other urban regions in India, show impacts of local biofuel combustions. Further, high levels of C₃H₈ and C₄H₁₀ evince the dominance of LPG/petrochemicals over the study location. The suite of trace gases measured during this study helps to decipher between impacts of local emissions and influence of transport on their levels.     

Shock Wave Cleaning of Air Filters

The trends in and relationships between ambient air concentrations of sulfur dioxide and sulfate aerosols at 48 urban sites and 27 nonurban sites throughout the U.S. between 1963 and 1972 have been analyzed. The substantial decreases in ambient SO₂ concentrations measured at urban sites in the eastern and midwestern U.S. are consistent with the corresponding reductions in local SO₂ emissions, but these decreases have been accompanied by only modest decreases in ambient sulfate concentrations. Large differences in the amounts of SO₂ emitted within individual air quality control regions are associated with much smaller differences in the corresponding ambient sulfate concentrations. Substantial changes in the patterns of SO₂ emissions between air quality regions result in essentially no differences between ambient sulfate concentrations in those air quality regions. Comparisons of several air quality regions in the eastern and western U.S. with similar SO₂ emission levels and patterns of emissions clearly demonstrates the higher ambient sulfate concentration levels in eastern air quality control regions. Relationships between SO₂, sulfates, and vanadium concentrations at eastern nonurban U.S. sites cannot be explained by local emission sources. These various observed results can be best explained by long distance sulfur oxide transport with chemical conversion of SO₂ to sulfates occurring over ranges of hundreds of kilometers. This conclusion has been suggested earlier and the present analysis strongly supports previous discussions. An impact of long range transport of sulfates is to emphasize the need for Consistent strategies for reduction of sulfur oxides throughout large geographical regions. Additions of large capacities involving elevated sources in mid-continental or western regions could result in significant increases in sulfate concentrations well downwind of such sources. Some of the types of research activities required to quantitate crucial experimental parameters are discussed.     

The change in O3, SO2 and NO2 concentrations in Lithuania

Due to the dynamic nature of the atmosphere, substantial amounts of gaseous and particulate pollutants are transported to the areas distant from their sources. In order to determine the regional concentration levels of atmospheric pollutants in Lithuania, concentrations of gaseous O₃, SO₂, NO₂ and other pollutants have been measured at the Preila background station (55°20′ N and 21°00′ E, 5 m a.s.l.) since 1981. The long-term concentration data set enabled us to get temporal trends, both on a seasonal and longer time scale, to identify source areas of pollutants and to relate them to the emission data. Based on the data obtained, the different tendencies in the pollutant concentration changes were revealed. Positive trends for ozone (of 2.9% per year during 1983–2000) and a distinct negative trend for both sulphur dioxide (of 3.8% per year during 1981–2000) and nitrogen dioxide (of 3.8% per year during 1983–2000) were found. The air mass back-trajectory analysis was used to assess the source region of air pollutants transported to Lithuania. The pollutant concentration levels were compared with their emission changes in Europe and Lithuania. The general trends in SO₂ as well as in NO₂ concentrations observed are consistent with changes in SO₂ and NO₂ emissions in Europe and Lithuania.     

Regional modelling of anthropogenic sulphur in Southeast Asia

A co-operative research project between the Malaysian Meteorological Service (MMS) and the Swedish Meteorological and Hydrological Institute (SMHI) focussing on the usage of an atmospheric transport and chemistry model, has just been initiated. Here, we describe the main features of the dispersion model and discuss a first set of calculations in light of available measurements of sulphuric species in Southeast Asia. According to our results, anthropogenic sulphur concentrations and depositions are particularly high near the large cities of the region, around a metal smelter in the southern Philippines, and in a region extending from northern Vietnam into southeastern China. These areas coincide with the high-emissions regions of Southeast Asia and we tentatively conclude that regional transport of acidifying species is not as far-reaching as in the mid-latitudes. From our calculations, and from supporting measurements we conclude that most of rural Southeast Asia is not yet severely affected by anthropogenic sulphur, but given the rapid rate of economical development in this region the situation may deteriorate quickly. Areas that are particularly at risk include the large cities, northern Vietnam, most of central Thailand, most of peninsular Malaysia, eastern Sumatra and parts of Java, all of which receive total-sulphur depositions in excess of 0.5 g S m⁻² yr⁻¹. Our model simulates sulphate in precipitation in accordance with measurements, but it has a tendency to overestimate atmospheric SO₂. It remains to be investigated whether this is a problem in the model formulation or a result of unrepresentative sampling. An immediate continuation of this study should be performed with higher spatial resolution than the currently used 100×100 km². Other imperfections in this model study, which should be addressed in future work, include parameterised vertical transport in deep convective clouds, the influence of natural emissions (primarily from volcanoes) on the concentration and deposition of sulphuric species, and the year-to-year variability of the driving meteorological conditions.     

Second Generation Chemical Mass Balance Source Apportionment of Sulfur Oxides and Sulfate at the Grand Canyon during the Project MOHAVE Summer Intensive

ABSTRACT

Receptor-based chemical mass balance (CMB) analysis techniques are designed to apportion species that are conserved during pollutant transport using conserved source profiles. The techniques will fail if non-conservative species (or profiles) are not properly accounted for in the CMB model. The straightforward application of the CMB model developed for Project MOHAVE using regional profiles resulted in a significant under-prediction of total sulfate oxides (SO_x, SO₂ plus fine particulate sulfate) for many samples at Meadview, AZ. In addition, for these samples the concentration of the inert tracer emitted from the MOHAVE Power Project (MPP), ocPDCH, was also under-predicted. A second-generation model has been developed which assumes that separation of particles and SO₂ can occur in the MPP plume during nighttime stable plume conditions. This second-generation CMB model accounts for all SO_x present at the various receptor sites. In addition, the concentrations of ocPDCH and the presence of other inert tracers of emission from regional sources are accurately predicted. The major source of SO_x at Meadview was the MPP, but the major source of sulfate at this site was the Las Vegas urban area. At Hopi Point in the Grand Canyon, the Baja California region (Imperial Valley and northwestern Mexico) was the major source of both SO_x and sulfate.     

Regional effects and efficiency of flue gas desulphurization in the Carpathian Basin

Although sulphur emissions (mainly as SO₂) have been continuously decreasing over the last 20 years in most western industrialized countries, localized SO₂ problems still exist in conjunction with strong local emission, meteorological, and topographical factors. In this study, the effect of supplementary installed flue gas desulphurization (FGD) units at high-capacity power plants on regional air pollution in the Carpathian Basin is investigated. The dispersion and accumulation of the SO₂ air pollutant are studied with the regional three-dimensional on-line atmosphere-chemistry model REMOTE. The changes in the SO₂ air pollution are investigated by parallel simulations in a case study, where the single modified parameter is the SO₂ emission rate. The results show that FGD units significantly reduce the horizontal and the vertical dispersion of the emitted SO₂, and its transboundary transport, too. Beside the SO₂ removal efficiency, the dispersion and accumulation also depend on the seasonal weather conditions. During winter, the dispersion and accumulation are higher than in other seasons. Due to this phenomenon, higher SO₂ removal efficiency is needed to guarantee similar air quality features like in the other seasons.     

Changes in the atmospheric deposition of acidifying compounds in the UK between 1986 and 2001

Emissions of a precursor of acidity in precipitation, sulphur dioxide (SO2), declined in the UK and the EU (15) by 71% and 72%, respectively, between 1986 and 2001, while nitrous oxide emissions declined by about 40%. Acidity in UK precipitation and the deposition of sulphate in precipitation halved during this period, but reductions were larger in the English Midlands than at the west coast and in high rainfall areas (>2000 mm). There is evidence that the smaller reductions in sulphur deposition in the west and south are due in part to shipping sources of SO2. Reductions in sulphur dry deposition (74%) are larger than in wet deposition (45%), due to changes in the canopy resistance to dry deposition. For reduced nitrogen, there has been a small (10%) reduction in emissions and deposition, while for oxidized nitrogen, a substantial reduction in emissions (40%) occurred but wet deposition of nitrate changed by less than 10%.     

A study of the total atmospheric sulfur dioxide load using ground-based measurements and the satellite derived Sulfur Dioxide Index

We present characteristics of the sulfur dioxide (SO₂) loading over Thessaloniki, Greece, and seven other selected sites around the world using SO₂ total column measurements from Brewer spectrophotometers together with satellite estimates of the Version 8 TOMS Sulfur Dioxide Index (SOI) over the same locations, retrieved from Nimbus 7 TOMS (1979–1993), Earth Probe TOMS (1996–2003) and OMI/Aura (2004–2006). Traditionally, the SOI has been used to quantify the SO₂ quantities emitted during great volcanic eruptions. Here, we investigate whether the SOI can give an indication of the total SO₂ load for areas and periods away from eruptive volcanic activity by studying its relative changes as a correlative measure to the SO₂ total column. We examined time series from Thessaloniki and another seven urban and non-urban stations, five in the European Union (Arosa, De Bilt, Hohenpeissenberg, Madrid, Rome) and two in India (Kodaikanal, New Delhi). Based on the Brewer data, Thessaloniki shows high SO₂ total columns for a European Union city but values are still low if compared to highly affected regions like those in India. For the time period 1983–2006 the SO₂ levels above Thessaloniki have generally decreased with a rate of 0.028 Dobson Units (DU) per annum, presumably due to the European Union's strict sulfur control policies. The seasonal variability of the SO₂ total column exhibits a double peak structure with two maxima, one during winter and the second during summer. The winter peak can be attributed to central heating while the summer peak is due to synoptic transport from sources west of the city and sources in the north of Greece. A moderate correlation was found between the seasonal levels of Brewer total SO₂ and SOI for Thessaloniki, Greece (R = 0.710–0.763) and Madrid, Spain (R = 0.691) which shows that under specific conditions the SOI might act as an indicator of the SO₂ total load.     

Anthropogenic sulphate aerosol from India: estimates of burden and direct radiative forcing

A one-box chemical-meteorological model had been formulated to make preliminary estimates of sulphate aerosol formation and direct radiative forcing over India. Anthropogenic SO₂ emissions from India, from industrial fuel use and biomass burning, were estimated at 2.0 Tg S yr^-1 for 1990 in the range of previous estimates of 1.54 and 2.55 Tg S yr ^-1 for 1987. Meteorological parameters for 1990 from 18 Indian Meteorological Department stations were used to estimate spatial average sulphate burdens through formation from SO₂ reactions in gas and aqueous phase and removal by dry and wet deposition. The hydrogen peroxide reaction was found dominating for undepleted oxidant-rich conditions. Monthly mean sulphate burdens ranged from 2–10 mg m^-2 with a seasonal variation of winter–spring highs and summer lows in agreement with previous GCM studies. The sulphate burdens are dominated by sulphate removal rates by wet deposition, which are high in the monsoon period from June–November. Monthly mean direct radiative forcing from sulphate aerosols is high (−3.5 and −2.3 W m^-2) in December and January, is moderate (−1.3 to −1.5 W m^-2) during February to April and November and low (−0.4 to −0.6 W m^-2) during May to October also in general agreement with previous GCM estimates. This model, in reasonable agreement with detailed GCM results, gives us a simple tool to make preliminary estimates of sulphate burdens and direct radiative forcing.     

Characterization of Several Integrative Sampling Methods for Nitric Acid,Sulphur Dioxide and Atmospheric Particles

Laboratory and field experiments were performed to evaluate integrative measurement methods for atmospheric nitrates, sulphate and sulphur dioxide. Denuder tubes and several filter media were tested under laboratory and field conditions. Effects of sampling variables such as temperature and relative humidity, flow rates, concentration, loading capacity and artifacts due to NO, NO₂ and SO₂ were also evaluated. The integrative filter sampling method and the ion chromatographic analytical procedure gave a measurement precision (relative standard deviation) of ±11.5 percent for particulate NO₃ ^? on Teflon and ±15.6 percent for gaseous HNO₃ on nylon; for both these constituents, the detection limit was about 0.1 μ m^?3.     

Ionic composition of wet precipitation over the southern slope of central Himalayas,Nepal

Severe atmospheric pollution transported to Himalayas from South Asia may affect fragile ecosystem and can be harmful for human health in the region. In order to understand the atmospheric chemistry in the southern slope of central Himalayas, where the data is limited, precipitation has been sampled at four sites: Kathmandu (1,314 m), Dhunche (2,065 m), Dimsa (3,078 m), and Gosainkunda (4,417 m) in Nepal for over a 1-year period characterized by an urban, rural, and remote sites, respectively. HCO₃ ^? is the dominant anion, while the NH₄ ⁺ is the dominant cation in precipitation at the four sites. Generally, most of ions (e.g., SO₄ ^2?, NO₃ ^?, NH₄ ⁺, HCO₃ ^?, and Ca²⁺) have higher concentrations in urban site compared to the rural sites. Neutralization factor calculation showed that precipitation in the region is highly neutralized by NH₄ ⁺ and Ca²⁺. Empirical orthogonal function and correlation analysis indicated that the precipitation chemistry was mostly influenced by crustal, anthropogenic, and marine sources in Nepal. Among different sites, urban area was mostly influenced by anthropogenic inputs and crustal dusts, whereas remote sites were mostly from marine and crustal sources. Seasonal variations show higher ionic concentrations during non-monsoon seasons mainly due to limited precipitation amount. On the other hand, lower ionic concentrations were observed during monsoon season when higher amount of precipitation washes out aerosols. Thus, precipitation chemistry from this work can provide a useful database to evaluate atmospheric environment and its impacts on ecosystem in the southern slope of central Himalayas, Nepal.