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1.
In this study, we used and compared three different statistical clustering methods: an hierarchical, a non-hierarchical (K-means) and an artificial neural network technique (self-organizing maps (SOM)). These classification methods were applied to a 4-year dataset of 5 days kinematic back trajectories of air masses arriving in Athens, Greece at 12.00 UTC, in three different heights, above the ground. The atmospheric back trajectories were simulated with the HYSPLIT Vesion 4.7 model of National Oceanic and Atmospheric Administration (NOAA). The meteorological data used for the computation of trajectories were obtained from NOAA reanalysis database. A comparison of the three statistical clustering methods through statistical indices was attempted. It was found that all three statistical methods seem to depend to the arrival height of the trajectories, but the degree of dependence differs substantially. Hierarchical clustering showed the highest level of dependence for fast-moving trajectories to the arrival height, followed by SOM. K-means was found to be the least depended clustering technique on the arrival height. The air quality management applications of these results in relation to PM10 concentrations recorded in Athens, Greece, were also discussed. Differences of PM10 concentrations, during certain clusters, were found statistically different (at 95% confidence level) indicating that these clusters appear to be associated with long-range transportation of particulates. This study can improve the interpretation of modelled atmospheric trajectories, leading to a more reliable analysis of synoptic weather circulation patterns and their impacts on urban air quality.  相似文献   

2.
Dimethylsulfide (DMS), sulfur dioxide (SO2), methanesulfonate (MSA), nonsea-salt sulfate (nss-SO4 2–), sodium (Na+), ammonium (NH4 +), and nitrate (NO3 –) were determined in samples collected by aircraft over the open ocean in postfrontal maritime air masses off the northwest coast of the United States (3–12 May 1985). Measurements of radon daughter concentrations and isentropic trajectory calculations suggested that these air masses had been over the Pacific for 4–8 days since leaving the Asian continent. The DMS and MSA profiles showed very similar structures, with typical concentrations of 0.3–1.2 and 0.25–0.31 nmol m–3 (STP) respectively in the mixed layer, decreasing to 0.01–0.12 and 0.03–0.13 nmol m–3 (STP) at 3.6 km. These low atmospheric DMS concentrations are consistent with low levels of DMS measured in the surface waters of the northeastern Pacific during the study period.The atmospheric SO2 concentrations always increased with altitude from <0.16–0.25 to 0.44–1.31 nmol m–3 (STP). The nonsea-salt sulfate (ns-SO4 2–) concentrations decreased with altitude in the boundary layer and increased again in the free troposphere. These data suggest that, at least under the conditions prevailing during our flights, the production of SO2 and nss-SO4 2– from DMS oxidation was significant only within the boundary layer and that transport from Asia dominated the sulfur cycle in the free troposphere. The existence of a sea-salt inversion layer was reflected in the profiles of those aerosol components, e.g., Na+ and NO3 –, which were predominantly present as coarse particles. Our results show that long-range transport at mid-tropospheric levels plays an important role in determining the chemical composition of the atmosphere even in apparently remote northern hemispheric regions.  相似文献   

3.
Ambient air quality in respect of SO2, NO2 and total suspended particulate matter (TSPM) was monitored at Pantnagar, India from May, 2008 to April, 2009 and statistically analyzed with meteorological variables such as relative humidity (RH), wind speed (WS), precipitation (P) and mean air temperature (T). TSPM was found to be the major air pollutant causing significant deterioration of air quality with annual mean concentrations of 280 μg/m3. Further, weekly mean air pollutant concentrations were statistically analyzed through stepwise multiple linear regression analysis in respect of independent meteorological variables to develop suitable statistical models. Both NO2 and TSPM concentrations were found to have been influenced by meteorological variables with coefficient of determination (R2) of 82.21 and 92.84%, respectively. However, atmospheric SO2 revealed only 22.87% of dependencies on meteorological variables. Partial correlation coefficients revealed that wind speed has the maximum influence (77.80 and 31.50%) on proposed equations for NO2 and SO2, closely followed by weekly mean temperature (73.60 and 24.30%). However, in case of TSPM, individual contribution of ambient temperature (94.40%) was found maximum, followed by relative humidity (86.50%). Model performances were evaluated through both quantitative data analysis techniques and statistical methods. Nearly 98 and 95% of potential error has been explained by the model developed for TSPM and NO2, while in case of SO2, it is found as only 61%. Therefore, performances of models (for TSPM and NO2) to predict ambient weekly mean concentrations based on forecasted weather parameters were found to be excellent, however, performance of model developed for SO2 was found only satisfactory.  相似文献   

4.
We present a 16-month record of ozone (O3), carbon monoxide (CO), total reactive nitrogen (NOy), sulphur dioxide (SO2), methane (CH4), C2 – C8 non-methane hydrocarbons (NMHCs), C1 – C2 halocarbons, and dimethyl sulfide (DMS) measured at a southern China coastal site. The study aimed to establish/update seasonal profiles of chemically active trace gases and pollution tracers in subtropical Asia and to characterize the composition of the `background' atmosphere over the South China Sea (SCS) and of pollution outflow from the industrialized Pearl River Delta (PRD) region and southern China. Most of the measured trace gases of anthropogenic origin exhibited a winter maximum and a summer minimum, while O3 showed a maximum in autumn which is in contrast to the seasonal behavior of O3 in rural eastern China and in many mid-latitude remote locations in the western Pacific. The data were segregated into two groups representing the SCS background air and the outflow of regional continental pollution (PRD plus southern China), based on CO mixing ratios and meteorological conditions. NMHCs and halocarbon data were further analyzed to examine the relationships between their variability and atmospheric lifetime and to elucidate the extent of atmospheric processing in the sampled air parcels. The trace gas variability (S) versus lifetime (τ) relationship, defined by the power law, Slnx = Aτ− b, (where X is the trace gas mixing ratio) gives a fit parameter A of 1.39 and exponent b of 0.42 for SCS air, and A of 2.86 and b of 0.31 for the regional continental air masses. An examination of ln[n-butane]/ln[ethane] versus ln[propane]/ln[ethane] indicates that their relative abundance was dominated by mixing as opposed to photochemistry in both SCS and regional outflow air masses. The very low ratios of ethyne/CO, propane/ethane and toluene/benzene suggest that the SCS air mass has undergone intense atmospheric processing since these gases were released into the atmosphere. Compared to the results from other polluted rural sites and from urban areas, the large values of these species in the outflow of PRD/southern China suggest source(s) emitting higher levels of ethyne, benzene, and toluene, relative to light alkanes. These chemical characteristics could be unique indicators of anthropogenic emissions from southern China.  相似文献   

5.
Six years of observations (1980 to 1986) of the composition of lower tropospheric aerosols at Alert on northern Ellesmere Island in the Canadian high Arctic yield insight into the seasonal variation of Arctic air pollutants as well as of substances of natural origin. A principal component analysis of 138 observations of 21 aerosol constituents (major ions, metals, nonmetallic trace elements) for the most polluted period of December to April identified not only a soil, sea salt and anthropogenic aerosol component, but also one associated with photochemical reactions in the atmosphere that occur at polar sunrise. Depending on the source of their gaseous precursors, elements in the photochemical component can be natural or anthropogenic in origin. For instance, SO4 2-, existing mostly as H2SO4, originates probably from both anthropogenic and natural sources while Br– is likely of marine origin. In contrast, SO4 2- in the anthropogenic component has the stoichiometry of NH4HSO4. In the winter months, over 90% of Arctic SO4 2- is in the anthropogenic and photochemical components.In winter, a substantial portion (11 to 35%) of Na+ is associated with the anthropogenic aerosol component suggesting either that marine aerosols have been physically or chemically modified by interactions with air pollution or that there are anthropogenic sources of Na+.The aerosol soil component is controlled by both local and distant dust sources. During a year, it has two peaks at Alert, one in April/May coinciding with the Asian dust storm season and one in September.There is a marked difference in the seasonal variation of particulate Br– and iodine concentrations in the air. Both have a peak in April/May associated with polar sunrise and, hence, photochemical reactions in the atmosphere. However, iodine also peaks in early fall. This may be a product of biogenic iodine emissions to the atmosphere during secondary blooms in northern oceans in late summer.Presented at the Second Conference on Baseline Observations in Atmospheric Chemistry (SABOAC II) in Melbourne, Australia, November 1988  相似文献   

6.
Carbon dioxide (CO2) has been measured at Alert by grab flask sampling since 1975 as part of the World Meteorological Organization's Background Air Pollution Monitoring Program. Deviations of CO2 concentration from the mean annual cycle have previously been attributed to air masses arriving at Alert from the source regions of the industrialized parts of Europe and the Soviet Union. In situ measurements of ambient CO2 and methane (CH4) were made at Alert using an automated gas chromatograph, as part of the Arctic Haze Study during April 1986. The temporal behaviour of CO2 and CH4 during this period was found to be highly correlated with measurements of particulate sulphate and other atmospheric trace species of anthropogenic origin. Examination of calculated air mass back-trajectories provided further evidence that the observed short-term increases in CO2 and CH4 mixing ratios were due to long-range transport from anthropogenic source regions.  相似文献   

7.
Described is a system for analyzing and forecasting the air quality in the central regions of Russia, During the operation of the system, the detailed meteorological information provided by the WRF-ARW model is used by the CHIMERE chemistry transport model for simulating the processes of transport, chemical transformation, and deposition of atmospheric minor constituents. Considered is the quality of retrieved and forecasted (with the lead time up to three days) concentrations of O3, NO2, NO, CO, and PM10. The presented verification scores of pollutant concentrations demonstrate a relative success of the system. Demonstrated is a need in improving the data on the emissions of the air pollutants used for simulations. A procedure for the statistical correction of computed concentrations is described and verification scores of its results are given.  相似文献   

8.
Middle tropospheric CO2 air concentrations, measured during a four year observation period at an Alpine Station (Plateau Rosa, Italian North-West Alps, 3480 m a.s.l.), have been correlated with the relevant synoptic air trajectories crossing the observation site. Meaningful relationships have been found among average curvature, altitude and potential temperature of clusters of homogeneous trajectories and their related CO2 concentrations measured at Plateau Rosà, allowing an objective identification of weather conditions giving rise to fully mixed air masses corresponding to background atmospheric CO2 levels. Air trajectories were calculated by using the wind speed fields provided by the ECMWF objective analysis. As during the analysis period a change of the ECMWF model resolution occurred (from T106 to T213), the study was also carried out in the sub-periods respectively preceding and following this change (in September 1991). Even if some features of the wind field turned out to be statistically different in the two sub-periods, nevertheless the differences on the trajectory patterns were small enough to keep almost unchanged all conclusions drawn for the whole four-year period.  相似文献   

9.
Abstract

Arctic haze has been attributed to industrial pollution released at mid‐latitudes. Our current understanding has been pieced together from routine meteorological data, ground‐based air chemistry observations and limited aircraft measurements. This study investigates the relationship between synoptic boundary‐layer meteorology and the composition of the near‐surface atmosphere during the polar sunrise at Alert, N.W.T. A secondary objective is to characterize the influence of local activity on the atmospheric composition at a site for a new baseline monitoring station and at a location where aerosol chemistry and grab‐flask samples for CO2 have been made for many years. Detailed measurements of the vertical distribution of aerosols were obtained from an upward‐looking lidar to complement the ground‐based measurements. Meteorological profiles of the near‐surface boundary layer were obtained from both free‐flying and tethered balloons. Near‐surface measurements were made of aerosol physical and chemical properties, O3, NO2, NO/NOx, Peroxyacetylnitrate (PAN) and hydrocarbons.

The study period was characterized by prolonged periods with strong surface inversions, which were broken up occasionally by intrusions of cold air into the warmer air aloft. Lidar observations showed that ice crystals often accompanied aerosols and were responsible for reducing visibility below 30–40 km. There was a strong correlation between aerosol mass in the diameter size range 0.15 to 1.5 μm and total SO4 = . PAN found at concentrations of about 200 ppt(v) was the main carrier of atmospheric nitrogen. Aerosol trace elements were divisible into anthropogenic soil, mixed soil/anthropogenic sea salt and halogens. Vertical transport in the surface boundary layer, as regulated by the strength of the surface radiation inversion, may play an important role in influencing the chemical composition of the air at the ground. The location of the new baseline monitoring laboratory was found to be generally windier and warmer than the lower altitude weather station, and the influence of local activity was found to be minimal.  相似文献   

10.
This study investigates atmospheric conditions’ influence on the mean and extreme characteristics of PM10 concentrations in Poznań during the period 2006–2013. A correlation analysis was carried out to identify the most important meteorological variables influencing the seasonal dynamics of PM10 concentrations. The highest absolute correlation values were obtained for planetary boundary layer height (r = ?0.57), thermal (daily minimum air temperature: r = ?0.51), anemological (average daily wind speed: r = ?0.37), and pluvial (precipitation occurrence: r = ?0.36) conditions, however the highest correlations were observed for temporal autocorrelations (1 day lag: r = 0.70). As regulated by law, extreme events were identified on the basis of daily threshold value i.e. 50 μg m?3. On average, annually there are approximately 71.3 days anywhere in the city when the threshold value is exceeded, 46.6 % of those occur in winter. Additionally, 83.7 % of these cases have been found to be continuous episodes of a few days, with the longest one persisting for 22 days. The analysis of the macro-scale circulation patterns led to the identification of an easy-to-perceive seasonal relations between atmospheric fields that favour the occurrence of high PM10 concentration, as well as synoptic situations contributing to the rapid air quality improvement. The highest PM10 concentrations are a clear reaction to a decrease in air temperature by over 3 °C, with simultaneous lowering of PBL height, mean wind speed (by around 1 m s?1) and changing dominant wind directions from western to eastern sectors. In most cases, such a situation is related to the expansion of a high pressure system over eastern Europe and weakening of the Icelandic Low. Usually, air quality conditions improve along with an intensification of westerlies associated with the occurrence of low pressure systems over western and central Europe. Opposite relations are distinguishable in summer, when air quality deterioration is related to the inflow of tropical air masses originating over the Sahara desert.  相似文献   

11.
Continuous measurements of ozone and its precursors including NO, NO2, and CO at an urban site (32°03′N, 118°44′E) in Nanjing, China during the period from January 2000 to February 2003 are presented. The effects of local meteorological conditions and distant transports associated with seasonal changed Asian monsoons on the temporal variations of O3 and its precursors are studied by statistical, backward trajectory, and episode analyses. The diurnal variation in O3 shows high concentrations during daytime and low concentrations during late night and early morning, while the precursors show high concentrations during night and early morning and low concentrations during daytime. The diurnal variations in air pollutants are closely related to those in local meteorological conditions. Both temperature and wind speed have significant positive correlations with O3 and significant negative correlations with the precursors. Relative humidity has a significant negative correlation with O3 and significant positive correlations with the precursors. The seasonal variation in O3 shows low concentrations in late autumn and winter and high concentrations in late spring and early summer, while the precursors show high concentrations in late autumn and winter and low concentrations in summer. Local mobile and stationary sources make a great contribution to the precursors, but distant transports also play a very important role in the seasonal variations of the air pollutants. The distant transport associated with the southeastern maritime monsoon contributes substantially to the O3 because the originally clean maritime air mass is polluted when passing over the highly industrialized and urbanized areas in the Yangtze River Delta. The high frequency of this type of air mass in summer causes the fact that a common seasonal characteristic of surface O3 in East Asia, summer minimum, is not observed at this site. The distant transports associated with the northern continental monsoons that dominate in autumn and winter are related to the high concentrations of the precursors in these two seasons. This study can contribute to a better understanding of the O3 pollution in vast inland of China affected by meteorological conditions and the rapid urbanization and industrialization.  相似文献   

12.
Measurements of atmospheric dimethylsulfide (DMS) and its oxidation products, sulfur dioxide (SO2), methanesulfonic acid (MSA) and non-sea-salt sulfate (nss-SO4 2-) were monitored during the period June 9–26, 1989 at a coastal site in Brittany. As indicated by the radon (Rn-222) activities and the high concentrations of NOx the air masses, for most of the experiment, were continental in origin. The observed concentrations range from 1.9 to 65 nmol/m3 for DMS (n=157), 0.6 to 94.2 nmol/m3 for SO2 (n=50), 0.6 to 11.6 nmol/m3 for MSA (n=44) and 42 to 350 nmol/m3 for nss-SO4 2- (n=44). Aitken nuclei reached values as high as 4.5 × 105 particles/m3. When continental conditions predominated, the measured SO2 concentrations were lower than those expected from a consideration of the observed DMS concentrations and the existence of SO2 background of the continental air masses. Similarly, compared to the MSA/DMS ratio in the marine atmosphere, higher concentrations of MSA were observed than those expected from the measured levels of DMS. The presence of enhanced levels of MSA was also endorsed by the observation that the measured mean MSA/nss-SO4 2- ratio of 6±3% was similar to the mean value of 6.9% observed in the marine atmosphere. These above observations are in line with recent laboratory findings by Barnes et al. (1988), which show an increase of the MSA/DMS yield with a simultaneous decrease of the SO2/DMS yield in the presence of NOx.  相似文献   

13.
Radon has been measured continuously at Cape Grim, Tasmania with a detection limit of about 0.05 Bq m-3 (1.4 pCi m-3). The annual average level from a close continental source is 3.8 Bq m-3, whereas the level in maritime air streams is typically 0.5 Bq m-3. The contribution of the ocean is about 0.04 Bq m-3, which indicates that more than 90% of radon in maritime air is from a continent. Thus radon can provide much less equivocal evidence of the degree of continental influence on an air stream than can other atmospheric constituents, whose sources and loss mechanisms are more complex. A knowledge of the past history of an air stream is important in the interpretation of atmospheric measurements.There is a close correlation between low radon and low Aitken particle concentrations, which suggests a continental origin for these particles. On the basis of present data it is difficult to reconcile this with evidence that the particles are generated photochemically over the ocean. An extension of the radon program to other latitudes would help to resolve this discrepancy.  相似文献   

14.
As part of the second Arctic Gas and Aerosol Sampling Program (AGASP II) continuous measurements of atmospheric aerosol black carbon (BC) were made at the NOAA/GMCC observatory at Barrow, Alaska (71°19N, 156°36W) during the period March 21–April 22, 1986. Black carbon is produced only by incomplete combustion of carbonaceous materials and so is a particularly useful atmospheric indicator of anthropogenic activities. The BC data have been analyzed together with the concurrent measurements of carbon dioxide (CO2), methane (CH4), and condensation nuclei (CN) that are routinely made at the observatory. All four species showed elevated and highly variable concentrations due to local human activities, principally in the township of Barrow, 7 km to the southwest, and at the DEW Line radar installation 1 km to the northwest. We distinguish between those periods of the record that are affected by local activities and those that are not, on the basis of the short-term (periods of up to 1 hour) variability of the continuous CO2 and CN records, with large short-term variabilities indicating local sources. We identified seven periods of time (events) with durations ranging from 13 to 37 hours when the BC, CO2, and CH4 concentrations changed smoothly over time, were highly correlated with each other, and were not influenced by local activities. These events had BC/CO2 ratios in the range (50–103)×10–6. These ratios are dimensionless since we convert the CO2 concentrations to units of ng m–3 of carbon. Such values of BC/CO2 are characteristic of the combustion effluent from large installations burning heavy fuel oil or coal, automobiles, and domestic-scale natural gas usage. We conclude that these events are indicative of air masses that have been polluted with combustion emissions in a distant location and then transported to the Arctic. In the absence of species-selective loss mechanisms, these air masses will maintain their combustion effluent signatures during the transport. The BC/CO2 ratios found for the local combustion activities are consistent with those expected from known combustion processes.  相似文献   

15.
This two-year study investigates the relative influence of meteorological variables (precipitation amount and temperature), atmospheric circulation, air mass history, and moisture source region on Irish precipitation oxygen isotopes (δ18Op) on event and monthly timescales. Single predictor correlations reveal that on the event scale, 20% of δ18Op variability is attributable to the amount effect and 7% to the temperature effect while on the monthly timescale the North Atlantic Oscillation accounts for up to 20% of δ18Op variability and the amount and temperature effects are not significant. In comparison, multivariate linear regression reveals that the interaction of temperature and precipitation amount explains up to 40% of δ18Op variance at event and monthly timescales. Five-day kinematic back trajectories suggest that the amount-weighted mean δ18Op value of southerly- and northerly-derived events are lower by 2‰ relative to events derived from the west. Because air mass history and atmospheric circulation appear to influence δ18Op in Ireland, Irish paleo-δ18Op proxy records are best interpreted as reflecting a combination of parameters, not just paleotemperature or paleorainfall.  相似文献   

16.
The occurrence of a severe storm in the Argentine littoral has been analyzed. Although general atmospheric conditions were not favorable to the development of deep convection, this storm produced strong winds and hail of considerable intensity. Its occurrence was associated with the entrance of a pulse of humid air at low levels and could be related to the development of two vorticity centers in the region. Atmospheric conditions existing above a low-level inversion are used to simulate two possible clouds, with base altitudes at 2200 and 3000 m and updraft speeds reaching maximum values of 27 and 29 m s−1 respectively. It is noted that the base temperature of about 13°C, found for the first cloud, can be correlated with the prevalence of frozen drop embryos, observed in an analyzed hailstone sample. Hailstone vertical trajectories are simulated in both modeled clouds, assuming spheroidal and spherical particles and assigning different values to the drag coefficient Cd.  相似文献   

17.
Inhalable particles (PM10), with aerodynamic equivalent diameters that are generally 10 micrometers or smaller, are basic pollutants in many areas, especially in northern China, and thus the pollution from PM10 inhalable particulate matter is a growing concern for public health. Independent long-term observations are necessary to evaluate the efficacy of PM10 reduction actions. Variations in the PM10 concentration from 2006 to 2017 at an observation station (NJ) in Beijing were recorded and analyzed. The average value ±1 standard deviation of daily mean PM10 concentrations was 138.8 ±96.1 μg m-3 for 1307 days (accounting for 34.7% of the total days), showing PM10 concentration exceeding the National Ambient Air Quality Standard (NAAQS) 24-h average of 150 μg m-3. Particulate concentration depended upon various meteorological conditions as also observed in this work: at low wind speed (<4 m s-1), the concentrations of PM10 revealed a downward trend with -19 μg m-3 per unit of wind speed, but when wind speed rose (>4 m s-1), the values increased by 49 μg m-3 per unit of wind speed. In Beijing, air masses from northwest China, especially from the Gobi Desert and other desert areas, had net contributions to long-range transport of natural dust, enhancing the PM10 concentrations by up to 29%. Overall, PM10 mass concentration showed a significant downward trend with -8.0 μg/m3/yr from 2006 to 2017. Although with higher fluctuations in recorded data, similar downward trends derived from the ) in 2017 still exceeded the NAAQS standard. The results showed that there is still a long way to go to reduce PM10 in Beijing.  相似文献   

18.
Gas and particle phase concentrations of atmospheric polychlorinated biphenyls (PCBs) were measured at an urban/industrial site in the city of Bursa, Turkey. PCB concentration levels were presented between July 2004 and May 2005. Average particle and gas phase concentrations of individual PCB congeners ranged from 0.08 (PCB-183) to 6.86 (PCB-49) pg m− 3 and from 0.01 (PCB-209) to 47.2 (PCB-33) pg m− 3, respectively. The mean concentration of total (gas + particle) PCBs varied between 24.27 and 666.21 pg m− 3 with an average of 287.27 ± 174.80 pg m− 3. PCB concentrations at the sampling site were higher than the concentrations reported at non-urban sites. PCBs partitioned between gas and particle phases and the partitioning was examined according to different approaches such as logKp–logPLo, logKp–logKOA and the Junge–Pankow model. In order to present possible interactions, a correlation matrix based on PCB congeners and meteorological parameters was constructed. Application of the Clausius–Clapeyron equation yielded a low slope value indicating possible emissions from local and regional sources originating mainly from urban/industrial areas, landfill and waste incineration plant. Then, likely dry deposition fluxes were estimated depending on reported dry deposition velocity and atmospheric concentration values.  相似文献   

19.
Vertical distributions of dimethylsulfide (DMS), sulfur dioxide (SO2), aerosol methane-sulfonate (MSA), non-sea-salt sulfate (nss-SO4 2-), and other aerosol ions were measured in maritime air west of Tasmania (Australia) during December 1986. A few cloudwater and rainwater samples were also collected and analyzed for major anions and cations. DMS concentrations in the mixed layer (ML) were typically between 15–60 ppt (parts per trillion, 10–12; 24 ppt=1 nmol m–3 (20°C, 1013 hPa)) and decreased in the free troposphere (FT) to about <1–2.4 ppt at 3 km. One profile study showed elevated DMS concentrations at cloud level consistent with turbulent transport (cloud pumping) of air below convective cloud cells. In another case, a diel variation of DMS was observed in the ML. Our data suggest that meteorological rather than photochemical processes were responsible for this behavior. Based on model calculations we estimate a DMS lifetime in the ML of 0.9 days and a DMS sea-to-air flux of 2–3 mol m–2 d–1. These estimates pertain to early austral summer conditions and southern mid-ocean latitudes. Typical MSA concentrations were 11 ppt in the ML and 4.7–6.8 ppt in the FT. Sulfur-dioxide values were almost constant in the ML and the lower FT within a range of 4–22 ppt between individual flight days. A strong increase of the SO2 concentration in the middle FT (5.3 km) was observed. We estimate the residence time of SO2 in the ML to be about 1 day. Aqueous-phase oxidation in clouds is probably the major removal process for SO2. The corresponding removal rate is estimated to be a factor of 3 larger than the rate of homogeneous oxidation of SO2 by OH. Model calculations suggest that roughly two-thirds of DMS in the ML are converted to SO2 and one-third to MSA. On the other hand, MSA/nss-SO4 2- mole ratios were significantly higher compared to values previously reported for other ocean areas suggesting a relatively higher production of MSA from DMS oxidation over the Southern Ocean. Nss-SO4 2- profiles were mostly parallel to those of MSA, except when air was advected partially from continental areas (Africa, Australia). In contrast to SO2, nss-SO4 2- values decreased significantly in the middle FT. NH4 +/nss-SO4 2- mole ratios indicate that most non-sea-salt sulfate particles in the ML were neutralized by ammonium.  相似文献   

20.
This paper deals with the atmospheric concentrations of PM5 and PM2.5 particulate matter and its water soluble constituents along with the size distribution of ions and spatial variation at three different residential environments in a semiarid region in India. Samples were collected from the indoors and outdoors of urban, rural and roadside sites of Agra during October 2007–March 2008. The mean concentrations of PM2.5 indoors and outdoors were 178 μgm−3 and 195 μgm−3 while the mean concentrations of PM5 indoors and outdoors were 231.8 μgm−3 and 265.2 μgm−3 respectively. Out of the total aerosol mass, water soluble constituents contributed an average of 80% (33% anions, 50% cations) in PM5 and 70% (29% anions, 43% cations) in PM2.5. The indoor–outdoor ratio of water soluble components suggested additional aerosol indoor sources at rural and roadside sites. Indoor–outdoor correlations were also determined which show poor relationships among concentrations of aerosol ions at all three sites. Univariate Pearson correlation coefficients among water soluble aerosols were determined to evaluate the relationship between aerosol ions in indoor and outdoor air.  相似文献   

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