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1.
Reactive halogen species (RHS = X, XO, HOX, OXO; X = Cl, Br, I) are known to have an important influence on the chemistry in the polar boundary layer (BL), where they are responsible for ozone depletion events in spring. Recent field campaigns at Mace Head, Ireland, and the Dead Sea, Israel, identified for the first time iodine oxide (IO) at mixing ratios of up to 6.6 ppt and 90 ppt bromine oxide (BrO), respectively, by DOAS also at lower latitudes. These results intensified the discussion about the role of the RHS in the mid-latitude BL.Photochemical box model calculations show that the observed IO mixing ratios can destroy ~0.45 ppb ozone per hour. This is comparable to the rates of the known O3-loss processes in the boundary layer. The model studies also reveal that IO, at these levels, has a strong influence on the BL photochemistry, increasing the OH/HO2- and the NO2/NO - ratios. In combination these changes lead to a reduction of the photochemical ozone formation, which - in addition - reduces ozone mixing ratios by up to 0.15 ppb/h.The studies for the Dead Sea case give no information on the heterogeneous process responsible for the bromine release, but they show that a total of 2 – 4 ppb of total bromine have to be released to explain the observed complete depletion of 60 ppb ozone in 2 – 3 hours.  相似文献   

2.
During two measuring campaigns in early spring 1994 and 1995 (March/April) and one campaign in summer 1994, measurements of ozone, PAN, sulfur dioxide, nitric acid, and particulate nitrate, sulfate, and ammonium (only 1995) were recorded in the Arctic. Observations were made by aircraft at various sites in the eastern and western Arctic. Ozone concentrations showed a steady increase with altitude both in spring and summer. During five flights in springtime, low ozone events (LOEs) could be observed near the surface and up to altitudes of 2000 m. SO2 background concentrations, ranging from detection limit (0.5 nmol/m3) to 5 nmol/m3, were observed during both spring and summer. Distinct maxima up to 55 nmol/m3 in lower altitudes were only obtained in springtime. Concentrations of the organic nitrate PAN were within a similar range as those of the inorganic nitrate HNO3 during spring campaigns. In contrast, concentrations of particulate nitrate were one half an order of magnitude lower. HNO3 concentrations increased significantly with altitude. Evidently, HNO3 was intruded from the stratosphere into the troposphere. Sulfate concentrations ranged between 5 and 30 nmol/m3; ammonium concentrations were obtained within a range from 10 to 50 nmol/m3.  相似文献   

3.
A comprehensive study on the chemistry of deposition and the concentration of tropospheric ozone and particulate sulfate in the ocean atmosphere was carried out for the data sets in 1990’s. It is important to study the atmospheric situation over the past years as well as the latest, especially in the East Asian region where emission amount of anthropogenic air pollutants have increased year by year due to rapid economic growth. The survey was conducted for 5 years in East Asia and West Oceania (35°N–35°S, 100–135°E) in August and September in 1990’s. The purpose of the survey was to study and understand the chemistry of deposition and the concentration of tropospheric ozone and particulate sulfate in the ocean atmosphere comprehensively in one project. Rainfall over the ocean was insufficiently neutralized. Gas and aerosol over the ocean were mature, i.e., well-mixed, during the period of the transportation. The characteristic latitudinal dependence was observed in the tropospheric ozone concentration, namely, higher in the southern hemisphere and lower in the northern hemisphere (approximately 25 ppb in the 10–40°S region and 5–15 ppb in the 20–40°N region). On the other hand, high concentrations of tropospheric ozone of over 30 ppb were observed in the northern hemisphere, which was attributable to the long-range transportation. The TSP concentration was approximately under the level of 40 μg m?3 irrespectively of the latitude; in contrast, the nss-SO4 2- concentration showed a clear latitudinal dependence, i.e., higher in the northern hemisphere and lower in the southern hemisphere. The background levels of the nss-SO4 2- concentration were approximately 0.5 μg m?3 in the 10–40°S region and 2–3 μg m?3 and 4–5 μg m?3 in the 0–20°N and 20–40°N regions, respectively.  相似文献   

4.
Black carbon aerosols plays an important role in the earth's radiative balance and little is known of their concentrations, distributions, source strength, and especially the aerosol chemistry of the developing world. The present study addresses the impact of back carbon aerosols on different atmospheric species like CO and tropospheric ozone over an urban environment, namely Hyderabad, India. Ozone concentration varies from 14 to 63 ppbv over the study area. Diurnal variations of ozone suggest that ozone concentration starts increasing gradually after sunrise, attaining a maximum value by evening time and decreasing gradually thereafter. Black carbon (BC) aerosol mass concentrations varies from 1471 to 11,175 ng m−3. The diurnal variations of BC suggest that the concentrations are increased by a factor of 2 during morning (06:00–09:00 h) and evening hours (18:00 to 22:00 h) compared to afternoon hours. Positive correlation has been observed between BC and CO (r2=0.74) with an average slope of 6.4×10−3 g BC/g CO. The slope between black carbon aerosol mass concentration and tropospheric ozone suggests that every 1 μg m−3 increase in black carbon aerosol mass concentration causes a 3.5 μg m−3 reduction in tropospheric ozone. The results have been discussed in detail in the paper.  相似文献   

5.
Measurements of surface ozone (O3), nitric oxide (NO), nitrogen dioxide (NO2), oxides of nitrogen (NOx=NO+NO2) and meteorological parameters have been made at Agra (North Central India, 27°10??N, 78°05??E) in post monsoon and winter season. The diurnal variation in O3 concentration shows daytime in situ photochemical production with diurnal maximum in noon hours ranging from 51 to 54 ppb in post monsoon and from 76 to 82 ppb in winter, while minimum (16?C24 ppb) during nighttime and early morning hours. Average 8-h O3 concentration varied from 12.4 to 83.9 ppb. The relationship between meteorological parameters (solar radiation intensity, temperature, relative humidity, wind speed and wind direction) and surface O3 variability was studied using principal component analysis (PCA), multiple linear regression (MLR) and correlation analysis (CA). PCA and MLR of daily mean O3 concentrations on meteorological parameters explain up to 80 % of day to day ozone variability. Correlation with meteorology is strongly emphasized on days having strong solar radiation intensity and longer sunshine time.  相似文献   

6.
Given and analyzed are the results of the measuring of concentration of ozone O3, nitrogen oxides NOx, and carbon monoxide CO at the surface as well as the sum of hydrocarbons and the aerosol optical depth in Obninsk (Kaluga oblast) during the warm period 2010 and 2011. The relationship between the air temperature and the maximum daily ozone values in May–September 2010 are characterized by the higher correlation coefficient than in May–September 2011: 0.82 ± 0.05 versus 0.64 ± 0.07. Increased concentration of surface ozone in Obninsk in July–August 2010 as compared to the similar period in 2011 were caused by the higher concentrations of the compounds-predecessors of ozone. The concentration of O3 in August 2010 exceeded 200μg/m3 and was never registered in Obninsk during the observation period of 2004–2011. This is associated with the air masses that came to Obninsk from the areas with peat and forest fires that resulted in the dramatic increase in surface concentrations of NOx, CO, and hydrocarbons.  相似文献   

7.
An in-cloud scavenging case study of the major ions (NH4 +, SO4 2- and NO3 -) determining the cloudwater composition at a mountain site (1620 m.a.s.l.) is presented. A comparison between in-cloud measurements of the cloudwater composition, liquid water content, gas concentrations and aerosol concentrations and pre-cloud gas and aerosol concentrations yields the following results. Cloudwater concentrations resulted from scavenging of about half of the available NH3, aerosol NH4 +, aerosol NO3 -, and aerosol SO4 2-. Approximately a third of the SO2 was scavenged by the cloudwater and oxidized to SO4 2-. Cloud acidity during the first two hours of cloud interception (pH 3.24) was determined mostly by the scavenged gases (NH3, SO2, and HNO3); aerosol contributions to the acidity were found to be small. Observations of gas and aerosol concentrations at three elevations prior to several winter precipitation events indicated that NH3 concentrations are typically half (12–80 %) of the total (gas and aerosol) N (-III) concentrations. HNO3 typically is present at much lower concentrations (1–55 %) than aerosol NO3 -. Concentrations of SO2 are a substantial component of total sulfur, with concentrations averaging 60 % (14–76 %) of the total S (IV and VI).  相似文献   

8.
Halogens in the atmosphere chemically destroy ozone. In the troposphere, bromine has higher ozone destruction efficiency than chlorine and is the halogen species with the widest geographical spread of natural sources. We investigate the relative strength of various sources of reactive tropospheric bromine and the influence of bromine on tropospheric chemistry using a 6-year simulation with the global chemistry transport model MOZART4. We consider the following sources: short-lived bromocarbons (CHBr3, CH2BrCl, CHBr2Cl, CHBrCl2, and CH2Br2) and CH3Br, bromine from airborne sea salt particles, and frost flowers and sea salt on or in the snowpack in polar regions. The total bromine emissions in our simulations add up to 31.7 Gmol(Br)/yr: 63 % from polar sources, 24.6 % from short-lived bromocarbons and 12.4 % from airborne sea salt particles. We conclude from our analysis that our global bromine emission is likely to be on the lower end of the range, because of too low emissions from airborne sea salt. Bromine chemistry has an effect on the oxidation capacity of the troposphere, not only due to its direct influence on ozone concentrations, but also by reactions with other key chemical species like HO x and NO x . Globally, the impact of bromine chemistry on tropospheric O3 is comparable to the impact of gas-phase sulfur chemistry, since the inclusion of bromine chemistry in MOZART4 leads to a decrease of the O3 burden in the troposphere by 6 Tg, while we get an increase by 5 Tg if gas-phase sulfur chemistry is switched off in the standard model. With decreased ozone burden, the simulated oxidizing capacity of the atmosphere decreases thus affecting species associated with the oxidation capacity of the atmosphere (CH3OOH, H2O2).  相似文献   

9.
利用中尺度大气化学模式WRF/Chem对2013年3月6日华南地区一次平流层入侵事件及其对对流层低层臭氧的影响进行模拟研究。通过加入UBC（Upper Boundary Condition）上边界处理方案,弥补WRF/Chem模式未考虑平流层臭氧化学反应的不足。结合臭氧探空廓线资料、地面O3、CO、NOx、相对湿度、温度和风速等观测资料以及再分析资料对模拟结果进行定量评估,结果表明模式能较为真实地模拟本次平流层入侵过程。模拟分析进一步揭示:（1）副热带高空急流是本次平流层入侵的主要原因。当华南地区处在副热带急流入口区左侧下沉区域时,平流层入侵将富含臭氧的干燥空气输送到对流层中低层。（2）本次平流层入侵对对流层低层臭氧收支有重要影响,导致香港地区近地层臭氧体积混合比浓度明显上升,如塔门站夜间臭氧浓度升高21.3 ppb（1 ppb=1×10-9）。地面气象场和化学物种的分析进一步确认了平流层入侵的贡献。（3）采用动力学对流层顶高度时零维箱式模型和Wei公式计算得到的平流层入侵通量相当,分别为-1.42×10-3 kg m-2 s-1和-1.59×10-3 kg m-2 s-1,这一结果与前人研究相吻合,且与采用热力学对流层顶高度计算所得到的结果具有可比性。  相似文献   

10.
As part of the Polar Sunrise Experiment (PSE) 1997, concentrations of halogen species thought to be involved in ground level Arctic ozone depletion were made at Alert, NWT, Canada (82.5°N, 62.3°W) during the months of March and April, 1997. Measurements were made of photolyzable chlorine (Cl2 and HOCl) and bromine (Br2 and HOBr) using the Photoactive Halogen Detector (PHD), and bromine radicals (BrOx) using a modified radical amplifier. During the sampling period between Julian Day 86 (March 27) and Day 102 (April 12), two ozone depletion episodes occurred, the most notable being on days 96-99, when ozone levels were below detectable limits (1 ppbv). Concentrations of BrOx above the 4 pptv detection limit were found for a significant part of the study, both during and outside of depletion events. The highest BrOx concentrations were observed at the end of the depletion event, when the concentration reached 15 pptv. We found substantial amounts of Br2 in the absence of O3, indicating that O3 is not a necessary requirement for production of Br2. There is also Br2 present when winds are from the south, implying local scale (e.g. from the snowpack) production. During the principal O3 depletion event, the HOBr concentration rose to 260 pptv, coincident with the BrOx maximum. This implies a steady state HO2 concentration of 6 pptv. During a partial O3 depletion event, we estimate that the flux of Br2 from the surface is about 10 times greater than that for Cl2.  相似文献   

11.
During the summer (8 June through 3 September) of 2008, 9 ozone profiles are examined from Dakar, Senegal (14.75°N, 17.49°W) to investigate ozone (O3) variability in the lower/middle troposphere during the pre-monsoon and monsoon periods. Results during June 2008 (pre-monsoon period) show a reduction in O3 concentrations, especially in the 850–700 hPa layer with Saharan Air Layer (SAL) events. However, O3 concentrations are increased in the 950–900 hPa layer where the peak of the inversion is found and presumably the highest dust concentrations. We also use the WRF-CHEM model to gain greater insights for observations of reduced O3 concentrations during the monsoon periods. In the transition period between 26 June and 2 July in the lower troposphere (925–600 hPa), a significant increase in O3 concentrations (10–20 ppb) occur which we suggest is caused by enhanced biogenic NOX emissions from Sahelian soils following rain events on 28 June and 1 July. The results suggest that during the pre-monsoon period ozone concentrations in the lower troposphere are controlled by the SAL, reducing ozone concentrations through heterogeneous chemical processes. At the base of the SAL we also find elevated levels of ozone, which we attribute to biogenic sources of NOX from Saharan dust that are released in the presence of moist conditions. Once the monsoon period commences, lower ozone concentrations are observed and modeled which we attribute to the dry deposition of ozone and episodes of ozone poor air that is horizontally transported into the Sahel from low latitudes by African Easterly Waves (AEWs).  相似文献   

12.
Surface ozone data from 25 Europeanlow-altitude sites and mountain sites located between79°N and 28°N were studied. The analysiscovered the time period March 1989–February 1993.Average summer and winter O3 concentrations inthe boundary layer over the continent gave rise togradients that were strongest in the north-west tosouth-east direction and west-east direction, respectively. WintertimeO3 ranged from 19 to 27 ppbover the continent, compared to about 32 ppb at thewestern border, while for summer the continentalO3 values ranged between 39 and 56 ppb and theoceanic mixing ratios were around 37 ppb. In the lowerfree troposphere average wintertime O3 mixingratios were around 38 ppb, with only an 8 ppbdifference between 28°N and 79°N. For summerthe average O3 levels decreased from about 55 ppbover Central Europe to 32 ppb at 79°N. Inaddition, O3 and Ox(= O3 + NO2)in polluted and clean air were compared. Theamplitudes of the seasonal ozone variations increasedin the north-west to south-east direction, while thetime of the annual maximum was shifted from spring (atthe northerly sites) to late summer (at sites inAustria and Hungary), which reflected the contributionof photochemical ozone production in the lower partsof the troposphere.  相似文献   

13.
Temporal variations in atmospheric hydrogen sulphide concentrations and its biosphere-atmosphere exchanges were studied in the World’s largest mangrove ecosystem, Sundarbans, India. The results were used to understand the possible contribution of H2S fluxes in the formation of atmospheric aerosol of different size classes (e.g. accumulation, nucleation and coarse mode). The mixing ratio of hydrogen sulphide (H2S) over the Sundarban mangrove atmosphere was found maximum during the post-monsoon season (October to January) with a mean value of 0.59?±?0.02 ppb and the minimum during pre-monsoon (February to May) with a mean value of 0.26?±?0.01 ppb. This forest acted as a perennial source of H2S and the sediment-air emission flux ranged between 1213?±?276 μg S m?2 d?1(December) and 457?±?114 μg S m?2 d?1 (August) with an annual mean of 768?±?240 μg S m?2d?1. The total annual emissions of H2S from the Indian Sundarban were estimated to be 1.2?±?0.6 Tg S. The accumulation mode of aerosols was found to be more enriched with non-sea salt sulfate with an average loading of 5.74 μg m?3 followed by the coarse mode (5.18 μg m?3) and nucleation mode (1.18 μg m?3). However, the relative contribution of Non-sea salt sulfate aerosol to total sulfate aerosol was highest in the nucleation mode (83%) followed by the accumulation (73%) and coarse mode (58%). Significant positive relations between H2S flux and different modes of NSS indicated the likely link between H2S, a dominant precursor for the non-sea salt sulfate, and non-sea sulfate aerosol particles. An increase in H2S emissions from the mangrove could result in an increase in enhanced NSS in aerosol and associated cloud albedo, and a decrease in the amount of incoming solar radiation reaching the Sundarban mangrove forest.  相似文献   

14.
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15.
Surface O3 concentration and its precursors have been observed at Longfengshan station,Heilongjiang Province for a period of one year from August 13,1994 to July 30,1995. Relationship between surface O3 and the meteorological conditions during this period is analyzed in this study.Observation results show that diurnal variation of surface O3 follows a pattern of double-peaks with amplitude of 27-28 ppb under fine days in summer and autumn.Although the diurnal variation is small(14 ppb),it is still detectable when it is overcast.Diurnal variation of O3 is irregular under rainy days.Surface O3 concentration rises when wind speed starts to increase at 0800 BT(Beijing Time)from 0 to 6 m s-1in autumn,winter and summer.Relative high surface O3 concentration is noticed frequently when S,SSW,SW and WSW wind are encountered at the station during all seasons.At 0800 BT and 1400 BT the surface O3 concentration increases with the increase of global radiation accordingly during fine days in winter,spring and autumn.During fine days average peak of O3 concentration in summer is 20 ppb higher than that in winter while the average peak of global radiation in summer is almost twice as high as that in winter.The average surface O3 concentration under fine days in autumn at Longfengshan station is 14 ppb lower in comparison to the observation results from Lin'an station where Lin'an is at about the same longitude and lower latitude,with same environment,which is mainly caused by the difference of global radiation due to different latitudes in these two areas(difference of average peak global radiation about 100 W m-2).  相似文献   

16.
The spatial variability and temporal behavior of the vertical flux of ozone have been investigated from turbulence measurements collected on aircraft flight legs in the daytime period during two consecutive summer experimental field programs. The data were obtained during horizontal flight legs conducted over agricultural crops and forested land in three different regions of the eastern United States.Results from individual experimental cases and statistics derived from all cases in each region are presented. Ozone flux generally exhibited a significant height dependency. The strongest negative (downward) fluxes in the lowest-level flight legs were primarily attributed to the uptake of ozone by the surface and vegetative cover. Fluxes were near-zero in the middle of the convective boundary layer (CBL) in the afternoon period. As ozone flux was proportional to concentration, slightly stronger fluxes were found in low-level urban plume segments where ozone concentrations were 10–20 ppb higher than in the surrounding area. The derived deposition velocity showed no such bias as a function of position across the urban plume. Ozone flux differences were not apparent between the more heavily forested sections and the primarily agricultural cropland areas in these regions. During the afternoon period when no clear temporal trend was evident, means from values obtained below 0.15Z i (Z i being the CBL height) were -0.421 and -0.431 ppb m-2 s-1 for ozone flux and 0.81 and 0.82 cm s-1 for the derived mean deposition velocity in the southeastern Pennsylvania and central Ohio areas, respectively. These experimental results for ozone provide support to a dry deposition parameterization module which computes grid-area averaged deposition velocities for use in regional-scale models.On assignment from the National Oceanic and Atmospheric Administration, U.S. Department of Commerce.  相似文献   

17.
The photochemical activation of chlorine by dissolved iron in artificial sea-salt aerosol droplets and by highly dispersed iron oxide (Fe2O3) aerosol particles (mainly hematite, specific surface ~150 m2 g?1) exposed to gaseous HCl, was investigated in humidified air in a Teflon simulation chamber. Employing the radical-clock technique, we quantified the production of gaseous atomic chlorine (Cl) from the irradiated aerosol. When the salt aerosol contained Fe2O3 at pH 6, no significant Cl production was observed, even if the dissolution of iron was forced by “weathering” (repeatedly freezing and thawing for five times). Adjusting the pH in the stock suspension to 2.6, 2.2, and 1.9 and equilibrating for one week resulted in a quantifiable amount of dissolved iron (0.03, 0.2, and 0.6 mmol L?1, respectively) and in gaseous Cl production rates of ~1.6, 6, and 8?×?1021 atoms cm?2 h?1, respectively. In a further series of experiments, the pure Fe2O3 aerosol was exposed to various levels of gaseous hydrogen chloride (HCl). The resulting Cl production rates ranged from 8?×?1020 Cl atoms cm?2 h?1 (at ~4 ppb HCl) to 5?×?1022 Cl atoms cm?2 h?1 (at ~350 ppb HCl) and confirmed the uptake and conversion of HCl to atomic Cl (at HCl to Cl conversion yields of 2–5 %, depending on the relative humidity). The Fe2O3 experiments indicate that iron-induced Cl formation may be important for highly soluble combustion-aerosol particles in marine environments in the presence of gaseous HCl.  相似文献   

18.
A unified chemistry-aerosol-climate model is applied in this work to compare climate responses to chang- ing concentrations of long-lived greenhouse gases(GHGs,CO2,CH4,N2O),tropospheric O3,and aerosols during the years 1951–2000.Concentrations of sulfate,nitrate,primary organic carbon(POA),secondary organic carbon(SOA),black carbon(BC)aerosols,and tropospheric O3 for the years 1950 and 2000 are obtained a priori by coupled chemistry-aerosol-GCM simulations,and then monthly concentrations are in- terpolated ...  相似文献   

19.
During the BERLIOZ field phase on 20 July 1998 a 40 km wide ozone-plume 30 to 70 km north of Berlin in the lee of the city was detected. The ozone mixing ratio inside the plume was app. 15 ppb higher than outside, mainly caused by high ozone precursor emissions in Berlin, resulting in a net chemical ozone production of 6.5 ppb h–1, which overcompensates ozone advection of –3.6 ppb h–1 andturbulent diffusion of –1.1 ppb h–1. That means, although moreozone leaves the control volume far in the lee of Berlin than enters it at the leeside cityborder and although turbulent diffusion causes a loss of ozone in the leeside control volume the chemical production inside the volume leads to a net ozone increase. Using a semi-Lagrangian mass budget method to estimate the net ozone production, 5.0 ppb h–1 are calculated for theplume. This means a fraction of about 20% of ozone in the plume is producedby local emissions, therefore called `home made' by the Berlin emissions. For the same area KAMM/DRAIS simulations using an observation based initialisation, results in a net production rate between 4.0 and 6.5 ppbh–1, while the threefold nested EURAD model gives 6.0 ppbh–1. The process analysis indicates in many cases goodagreement (10% or better) between measurements and simulations not only in the ozone concentrations but also with respect to the physical and chemical processes governing the total change. Remaining differences are caused by different resolution in time and space of the models and measurements as well as by errors in the emission calculation.The upwind-downwind differences in PAN concentrations are partly similar to those of ozone, because in the BERLIOZ case they are governed mainly by photochemical production. While in the stable boundary layer at night and windward of Berlin 0.1 to 0.3 ppb are detected, in the centre of the plume at noon concentrations between 0.75 ppb and 1.0 ppb are measured. The O3/PAN ratio is about 80 to 120 and thus due to the relatively lowPAN concentrations significantly higher than found in previous studies. The low PAN formation on 20 July, was mainly restricted by the moderate nonmethane hydrocarbon levels, whereas high PAN concentrations of 3.0 ppb on 21 July, are caused by local production in the boundary layer and by large scale advection aloft.  相似文献   

20.
This paper reports aerosol chemical properties for the first time over a Korean Global Atmosphere Watch (GAW) supersite, Anmyeon (36°32′N; 126° 19′E), during 2003–2004 period. Total suspended Particulates (TSP) showed significant seasonal variation with consistent higher mass concentrations during spring season (average of up to 230?±?190 μg/m3). PM10 also followed similar trend with higher concentrations during spring (average of up to 170?±?130 μg/m3) and showed reduced concentrations during summer. PM2.5 showed a significant increase during summer (average of up to 60?±?25 μg/m3), which could be due to the influx of fine mode sea salt aerosols associated with the Changma front (summer monsoon). Chemical composition analysis showed enhanced presence of acidic fractions, majorly contributed by sulphates (SO 4 2- ) and nitrates (NO 3 - ) in TSP, PM10 and PM2.5 during different seasons. Enhanced presence of Calcium (Ca2+) was observed during sand storm days during spring. The high correlation obtained on matrix analysis between crustal ions and acidic ions suggests that the ionic compositions over the site are mainly contributed by terrestrial sources of similar origin. The neutralization factors has been estimated to find the extend of neutralization of acidicity by main basic components, and found to have higher value for Ammonium (up to 1.1) in different seasons, indicating significant neutralization of acidic components over the region by NH 4 + . Back trajectory analysis has been performed during different seasons to constrain the possible sources of aerosol origin and the results are discussed in detail.  相似文献   

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