Cloudwater studies at a high elevation site in the Vosges Mountains (France)

Cloud and rainwater samples have been collected at a high elevation site in the Vosges Mountains. An automated collection system has been used to collect bulk cloudwater and small cloudwater droplets. Bulk cloudwater concentrations were up to 10 times more concentrated than rainwater concentrations. Small clouddroplets showed generally higher concentrations than bulk cloudwater. Nevertheless, the enrichment factors depend on the compounds under study and appear to be related to the composition of the cloud condensation nuclei forming small or large clouddroplets. Principal component analysis and factor analysis were applied to the collected datasets and confirmed the influence of the cloud condensation nuclei on the composition difference between small and large cloudwater droplets.     

Measurements and modelling of cloudwater deposition to moorland and forests

The objective of the study was to measure the size dependence of cloudwater deposition and associated average ionic fluxes to vegetated surfaces. Measurements were made over a forest canopy at Dunslair heights in south Scotland and a moorland site, Great Dun Fell, in northern England. Measurements were made using the gradient and eddy correlation techniques. Eddy correlation measurements were made using an ultrasonic anemometer, a Knollenberg forward scattering spectrometer probe (to measure liquid water fluxes and fluxes of droplets in 1 microm size intervals) and a GSI particulate volume monitor (to measure liquid-water fluxes). Measurements were made at Great Dun Fell of the size dependence of droplet deposition velocity, using the gradient technique with two Knollenberg probes. Simultaneous gradient and eddy correlation measurements were also made at Great Dun Fell of average cloud-water fluxes, together with chemical analysis of cloud water composition, using a continuous analysis system. At Dunslair Heights, eddy correlation measurements were made using both the Knollenberg and Gerber Scientific Instruments (GSI) probes, while simultaneous gradient measurements using two GSI probes were also attempted. Samples of cloud water were collected at Dunslair Heights, using passive string collectors for chemical analysis by ion chromatography. The major findings of the study were: 1. The droplet deposition velocities measured by the two techniques were similar. 2. The deposition velocities were a strong function of droplet size. Considerable resistance to deposition was evident for droplets of less than 5 microm radius. Deposition velocities for particles from about 6 to 8 microm exceeded those for momentum. 3. Except when the droplets were very small or the winds very light, bulk cloud-water deposition velocities were about 80% or more of the momentum deposition velocities to forests.     

Direct damage to vegetation caused by acid rain and polluted cloud: definition of critical levels for forest trees

The concept of critical levels was developed in order to define short-term and long-term average concentrations of gaseous pollutants above which plants may be damaged. Although the usual way in which pollutants in precipitation (wet deposition) influence vegetation is by affecting soil processes, plant foliage exposed to fog and cloud, which often contain much greater concentrations of pollutant ions than rain, may be damaged directly. The idea of a critical level has been extended to define concentrations of pollutants in wet deposition above which direct damage to plants is likely. Concentrations of acidity and sulphate measured in mountain and coastal cloud are summarised. Vegetation at risk of injury is identified as montane forest growing close to the cloud base, where ion concentrations are highest. The direct effects of acidic precipitation on trees are reviewed, based on experimental exposure of plants to simulated acidic rain, fog or mist. Although most experiments have reported results in terms of pH (H(+) concentration), the accompanying anion is important, with sulphate being more damaging than nitrate. Both conifers and broadleaved tree seedlings showing subtle changes in the structural characteristics of leaf surfaces after exposure to mist or rain at or about pH 3.5, or sulphate concentration of 150 micromol litre(-1). Visible lesions on leaf surfaces occur at around pH 3 (500 micromol litre(-1) sulphate), broadleaved species tending to be more sensitive than conifers. Effects on photosynthesis and water relations, and interactions with other stresses (e.g. frost), have usually been observed only for treatments which have also caused visible injury to the leaf surface. Few experiments on the direct effects of polluted cloud have been conducted under field conditions with mature trees, which unlike seedlings in controlled conditions, may suffer a growth reduction in the absence of visible injury. Although leaching of cations (Ca(2+), Mg(2+), K(+)) is stimulated by acidic precipitation, amounts leached are small compared with root uptake, unless soils have been impoverished. This aspect of the potential effects of acidic precipitation is best considered in terms of the long-term critical-load of pollutants to the soil. Given the practical difficulties in monitoring cloud water composition, a method for defining critical levels is proposed, which uses climatological average data to identify the duration and frequency of hill cloud, and combines this information with measured or modelled concentrations of particulate sulphate in the atmosphere, to derive cloud water concentrations as a function of cloud liquid water content. For forests within 100 m of the cloud base the critical levels of particulate sulphate, corresponding to solution concentrations in the range 150-500 micromol litre(-1), are in the range 1-3.3 microg S m(-3). These concentrations are observed over much of central Europe, suggesting that many montane forests are at risk of direct effects of fossil-fuel-derived pollutants in cloud.     

Removal of sulphur dioxide in a two-dimensional rain system based on a scale analysis of the conservation equations

Since rain systems show a wide variation in structure in both time and space, it is virtually impossible to model in detail the behaviour of sulphur passing through a rain system. Instead, an attempt has been made to determine the scale of the major processes going on in a frontal rain system based on the conservation equations for cloudwater, rainwater, SO₂ in air, sulphate in cloud and sulphate in rainwater. When this procedure is followed it is found that cloud and rainwater amounts are determined largely as a dynamic balance between cloudwater condensation and accretion of cloud drops by rain. The removal of SO₂ in rain is mainly determined by the oxidation of SO₂ in cloud, enhanced by oxidation in rain. In the case when oxidation of SO₂ by O₃ is the primary oxidation pathway a simple formula is derived for the fractional removal efficiency, which shows which parameters are of greatest importance and has potential use in the current generation of long-range transport models. This formula shows that the removal efficiency is a strongly non-linear function of sulphur dioxide concentration. At regional average SO₂ concentrations removal is efficient, but decreases rapidly at higher SO₂ concentrations.     

A winter study of air,cloud and precipitation chemistry in Ontario,Canada

During January and February 1984, a field project was conducted near North Bay, Ontario, Canada. The principal objective was to characterize the chemical and microphysical properties of the air masses, clouds and precipitation in this region of NE North America during the winter season. Two extensively instrumented aircraft with some newly designed cloudwater and snow collectors were used, as well as a surface station continuously monitoring pollutant concentrations and a precipitation event sampling network. Pollutant concentrations at the surface were found to vary with the airmass back trajectory with the highest concentrations observed for trajectories from the S and SW and the lowest from the N. Vertical profiles of aerosol particle (0.2−2 μm diameter) and NOx concentrations show similar trends with maxima of 1200 cm⁻³ and 7 ppb, respectively near ground level with air mass trajectories from the S, in comparison to values of 250 cm⁻³ and 1 ppb obtained with trajectories from the N. Cloudwater, aircraft precipitation and ground precipitation samples had a daily median pH of 3.6,4.6 and 4.2, respectively with the cloudwater having the highest sulphate and nitrate concentrations. The nitrate/sulphate equivalent concentration ratios in the cloudwater, aircraft precipitation and ground precipitation samples were 0.7,0.6 and 1.4, respectively. The data suggest that precipitation scavenging of nitric acid below cloud base is an important process during the winter season.     

Fluxes of trichloroacetic acid through a conifer forest canopy

Controlled-dosing experiments with conifer seedlings have demonstrated an above-ground route of uptake for trichloroacetic acid (TCA) from aqueous solution into the canopy, in addition to uptake from the soil. The aim of this work was to investigate the loss of TCA to the canopy in a mature conifer forest exposed only to environmental concentrations of TCA by analysing above- and below-canopy fluxes of TCA and within-canopy instantaneous reservoir of TCA. Concentrations and fluxes of TCA were quantified for one year in dry deposition, rainwater, cloudwater, throughfall, stemflow and litterfall in a 37-year-old Sitka spruce and larch plantation in SW Scotland. Above-canopy TCA deposition was dominated by rainfall (86%), compared with cloudwater (13%) and dry deposition (1%). On average only 66% of the TCA deposition passed through the canopy in throughfall and stemflow (95% and 5%, respectively), compared with 47% of the wet precipitation depth. Consequently, throughfall concentration of TCA was, on average, approximately 1.4 x rainwater concentration. There was no significant difference in below-canopy fluxes between Sitka spruce and larch, or at a forest-edge site. Annual TCA deposited from the canopy in litterfall was only approximately 1-2% of above-canopy deposition. On average, approximately 800 microg m(-2) of deposited TCA was lost to the canopy per year, compared with estimates of above-ground TCA storage of approximately 400 and approximately 300 microg m(-2) for Sitka spruce and larch, respectively. Taking into account likely uncertainties in these values ( approximately +/- 50%), these data yield an estimate for the half-life of within-canopy elimination of TCA in the range 50-200 days, assuming steady-state conditions and that all TCA lost to the canopy is transferred into the canopy material, rather than degraded externally. The observations provide strong indication that an above-ground route is important for uptake of TCA specifically of atmospheric origin into mature forest canopies, as has been shown for seedlings (in addition to uptake from soil via transpiration), and that annualized within-canopy elimination is similar to that in controlled-dosing experiments.     

Chemical climatology of high elevation spruce-fir forests in the southern Appalachian mountains

The physical and chemical climatology of high elevation (> 1500 m) spruce-fir forests in the southern Appalachian mountains was studied by establishing a weather and atmospheric chemical observatory at Mt Mitchell State Park in North Carolina (35 degrees 44' 05" N, 82 degrees 17' 15"W). Data collected during the summer and autumn (May-October) of 1986, 1987, and 1988 are reported. All measurements were made on or near a 16.5 m walk-up tower extending 10 m above the forest canopy on Mt Gibbes (2006 m msl), which is located approximately 2 km SW of Mt Mitchell. The tower was equipped with standard meteorological instrumentation, a passive cloud water collector, and gas pollutant sensors for O3, SO2, NOx. The tower and nearby forest canopy were immersed in clouds 25 to 40% of the time. Non-precipitating clouds were very acidic (pH 2.5-4.5). Precipitating clouds were less acidic (pH 3.5-5.5). The dominant wind directions were WNW and ESE. Clouds from the most common wind direction (WNW) were more acidic (mean pH 3.5) than those from the next most common wind direction (ESE, mean pH 5.5). Cloud water acidity was related to the concentration of SO4(2-), and NO3- ions. Mean concentration of H+, NH4+, SO4(2-), and NO3- ions in the cloud water varied from 330-340, 150-200, 190-200 and 120-140 micromol litre(-1) respectively. The average and range of O3 were 50 (25-100) ppbv (109) in 1986, 51 (26-102) ppbv in 1987, and 66 (30-140) during the 1988 field seasons, respectively. The daily maximum, 1-h average, and 24-h average concentrations were all greatest during June through mid-August, suggesting a correlation with the seasonal temperature and solar intensity. Throughfall collectors near the tower were used to obtain a useful estimate of deposition to the forest canopy. Between 50-60% of the total deposition of SO4(2-) was due to cloud impact.     

Lethal and sublethal toxicity of 4-nonylphenol to the common mussel (Mytilus edulis L.)

The toxicity of nonylphenol to the common mussel (Mytilus edulis L.) has been determined in both semistatic and continuous flow test systems. The LC50 values obtained were for 96 h, 30 mg litre(-1); 360 h, 0.5 mg litre(-1); and 850 h, 0.14 mg litre(-1). Sublethal effects, manifested as decreased byssus strength and change of scope for growth, were obtained at a concentration as low as 0.056 mg litre(-1). Fertilization and early developmental success were not affected at the highest concentration tested (0.2 mg litre(-1)).     

Response of abscisic acid in soybean leaves to NO2 exposure

Soybean (Glycine max L. Merril) cv. 'Williams' plants were exposed 0.0, 0.05, 0.2 and 0.4 microl litre(-1) NO(2) under controlled environment. Amount of abscisic acid (ABA) was measured after either 7 h or 5 days of exposure as well as after 18 h of recovery period. For quantitative analysis of ABA enzyme-linked immunosorbent assay was used. A significant increase (160%) was observed in plants treated with 0.4 microl litre(-1) NO(2) for 5 days compared to an increase of only 82% on exposure for 7 h. Rate of recovery for plants treated with low doses of NO(2) was higher than those treated with higher doses.     

Sulphite and sulphate concentrations in weathering products of sandy limestone and in deposition samples

The sulphite and sulphate concentrations in weathering products of limestone and in wet and total deposition samples were measured by the modified West-Gaeke method and by ion chromatography. The sulphite content in the weathering crust and in the runoff rainwater of two historical buildings in Belgium, was always much lower than the sulphate content. The maximum sulphite to sulphate ratio was 2.5%. The sulphite concentration in wet and total deposition samples was in the low or sub ppm range except during two misty periods when the sulphite concentration was 6.8 and 21 mg litre(-1). In those samples a high sulphate concentration was also found (nl. 57 and 137 mg litre(-1), respectively).     

Exposure of two upland plant species to acidic fogs

A system is described for exposing large numbers of plants to acidic fogs. The system allows low volumes of treatment solutions to be provided at particle sizes chiefly in the 5-30 microm range (equivalent to fog/cloud droplets). Plants of Poa alpina L. and Epilobium brunnescens were propagated from material collected in Snowdonia, North Wales and exposed to fog treatments at pH values of 2.5, 3.5, 4.5 and 5.6. There were 3 x 4 h exposures per week which provided a total of 6 mm deposition. Supplementary watering was with pH 4.5 simulated acid rain (24 mm per week). After 21 weeks, there was increased lowering and a greater dry weight for plants of E. brunnescens exposed to the pH 2.5 fog in comparison with other treatments. Also, the plants used assimilated material to form shoots rather than roots. A similar increase in dry weight accumulation in the pH 2.5 treatment was found in P. alpina after 63 weeks but this was not associated with changes in assimilate partitioning.     

Analysis of Hong Kong daily bulk and wet deposition data from 1994 to 1995

Results from a 1-year daily rainwater sampling program, employing both wet and bulk deposition samplers with replicate samples, from 1994 to 1995 in Hong Kong are presented and analysed. Analyte concentrations were found to vary over a wide range of several orders of magnitude, with [H⁺] for example, from 0.16 to 208.9 μeq dm^-3. Diurnal pH values less than 3.83 were measured on five occasions. A significant correlation between pH and lognormal windspeed has been found. This is taken to indicate the minor importance of long-range transport in determining rainwater acidity, since local pollutant emissions accumulate and react under conditions of atmospheric stability in the sub-tropical climate. The H⁺ wet deposition flux onto a polythene surface was 90 meq m^-2 yr^-1 during 1994–1995 at City University. Dry deposition exerts a neutralizing influence upon the acidity from this wet deposition. Although paired t-tests indicated significant differences between the bulk versus wet deposition datasets for cations, but not anions, the dataset means consequently showed such large standard deviations that t-tests indicated no significant differences. In rainwater, the charges from SO^2-₄ and NO^-₃ anions seldom balance the proton charges, implying that they are also derived from solubilization of primary and secondary airborne Ca²⁺, Mg²⁺ and NH⁺₄ particulate matter in rainwater. Use of the [SO^2-₄]/[NO^-₃] ratios in rainwater in fingerprinting pollutant origins has drawbacks, but is generally indicative of a predominantly regional contribution of these secondary pollutants to rainwater. Bulk deposition pH in Hong Kong would be in the region of 4.1 if basic Ca²⁺ compounds alone did not neutralize acidity. The regional rainout pH, inferred after exhaustive below-cloud scavenging, is about 5. The temporal trends in Hong Kong rainwater acidity are blurred.     

绿色建筑小区雨水资源化综合利用技术

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An investigation of the impact of afforestation on stream-water chemistry in the Loch Dee catchment, SW Scotland

The impact of conifer afforestation on stream-water chemistry was investigated in the acidified catchment of Loch Dee, SW Scotland. Long-term trends in stream-water chemistry were evaluated during a period of forest growth from age 6 to 17 years. A significant increase was observed for pH (0.2 units) and a significant decline for aluminium (0.05 mg litre(-1)), sulphate (1.2 mg litre(-1)) and nitrate (0.02 mg litre(-1)) concentrations. The long-term decrease in stream-water acidity was ascribed to the marked reductions in sulphur depositions during the 1970s and early 1980s. There was no evidence that this response had been attenuated by afforestation, the improvements in stream-water chemistry being of a similar magnitude to those recorded in nearby moorland lochs and exceeding that in an adjacent moorland-catchment stream. The lack of a clear forest acidification effect is consistent with deposition-model estimates which show the increased scavenging of occult and dry deposition by the growing forest to be small at this site (相似文献   

Overall dry deposition velocities of trace elements measured at harbor and traffic site in central Taiwan

For reasonable and convenient assessments of the characteristics of the dry deposition velocities between Taichung harbor site and Wuchi town site in central Taiwan, the overall dry deposition velocities of several metallic elements were calculated as the particulate diameter (D(p)) distributions of large particles (D(p) > 10 microm), coarse particles (10 microm < D(p) < 2.5 microm), and fine particles (D(p) < 2.5 microm) based on the ambient measurements during March-December of 2004. In this work, the dry deposition fluxes showed the higher correlation with coarse particle concentrations than large particle concentrations; however, the least well correlation was observed between the dry deposition fluxes and the fine particle concentrations. The calculated best-fit overall dry deposition velocities obtained using coarse particle concentrations varied from approximately 0.2 cm s(-1) for Cr to 1.5 cm s(-1) for Pb and 0.2 cm s(-1) for Fe to 2.6 cm s(-1) for Pb at Taichung harbor and Wuchi town site, respectively. In general, the crustal elements had higher deposition velocities than anthropogenic elements. In addition, overall dry deposition velocities for crustal elements were higher in Wuchi town site than in Taichung harbor site. The results identified the dry deposition flux was mainly contributed from large and coarse particles due to their high deposition velocities. The results also indicated that the best approach to estimate overall dry deposition was by depending on the characteristics of particles with diameters larger than 2.5 microm.     

Aluminium speciation in surface waters from a Welsh upland area

The complete aluminium speciation of surface waters from an acidified catchment, during dry weather and during storm episodes, is obtained. For the first time, estimates of adsorbed aluminium (Al(ad)) are reported together with other aluminium species. Al(ad) is calculated from the difference between monomeric aluminium content before and after separation of suspended solids by filtration (0.015 microm pore diameter). This fraction was very significant (Al(ad) >; 40 microg litre(-1)) for samples with high suspended solids content (ss >; 20 mg litre(-1)) collected during storm episodes. Plots of pAl(3+) versus pH for samples collected during dry weather are approximated by a straight line, close to the solubility line of synthetic gibbsite, and have a slope of 2.5, which suggests that these samples were saturated with respect to gibbsite. The cloud of pAl(3+) versus pH points for samples from storm episodes has a near zero slope, and shows a significant degree of undersaturation with respect to synthetic gibbsite. Various mechanisms of aluminium mobilisation are discussed.     

Wetfall Deposition and Precipitation Chemistry for a Central Appalachian Forest

Abstract

Although extensive research on acidic deposition has been directed toward spruce-fir forests, less research has been done on the impacts of air pollution on eastern montane hardwood forests. The purpose of this study was to describe precipitation chemistry for several Appalachian hardwood forest sites at or near the Fernow Experimental Forest (FEF) to assess the potential for problems associated with acidic deposition. Emphasis was placed on seasonal patterns of ionic concentrations (H+, Ca++, NH4+; NO3-, and SO4=) and spatial variability of ionic concentrations and deposition among sites. Seasonal patterns of most ions showed highest concentrations during the summer months and deposition of H+ was especially pronounced during this time. Deposition of all ions was generally greater (related to greater precipitation) at three montane forested sample sites compared to a nonforested riverbottom site. Precipitation chemistry at FEF was similar to other sites throughout the eastern United States and contrasted sharply with mid-western and western sites. Eastern sites, including means for FEF sites, were uniformly 3-4 times higher in H+ and SO4= concentration than the mid-western and western sites. Precipitation at FEF was chronically acidic, more so during the growing season, and highest at higher elevations where environmental stresses can be most severe. Furthermore, there were occasional large discrepancies between the low-elevation site and the higher-elevation forested sites for precipitation chemistry and acidic deposition. These results suggest that synoptic-scale (network) data may greatly underestimate the pollutant conditions to which highelevation forest trees are exposed, since network data rarely take elevation into account and typically are based on annual ionic concentration and deposition means that may be considerably lower than those of the growing season.     

Responses of bean (Phaseolus vulgaris L. cv. Pros) to chronic ozone exposure at two levels of atmospheric ammonia

Plants of bean (Phaseolus vulgaris cv. Pros) were exposed to a range of O3 concentrations up to 70 nl litre(-1) for 9 h day(-1) in the presence (45 nl litre(-1)) and absence (21 nl litre(-1)) of enhanced NH3 in 12 open-top chambers. Treatment effects on visible injury, growth and yield were assessed after 49 (intermediate harvest) and 62 days of exposure (final harvest). The proportion of leaves with visible injury at final harvest increased with increasing concentrations of O3. Enhanced NH3 did not cause any symptoms and did not affect injury by O3. The estimated seasonal mean concentration corresponding with 5% injury was circa 23 nl litre(-1) O3. Biomass production and green pod yield decreased with increasing concentrations of O3 and were generally stimulated by enhanced NH3 at both harvests. Adverse effects of O3 on biomass and pod yield did not depend on the NH3 level. Relative yield response to increasing 9-h daily mean O3 concentrations was nonlinear and yield losses of 5 and 10% were calculated to occur at seasonal daytime mean concentrations of 27 and 33 nl litre(-1) O3, respectively. Linear regression showed that the Accumulated exposures Over a Threshold of 30 (AOT30) and 40 nl litre(-1) (AOT40) O3 performed equally well. The estimated accumulated O3 exposures corresponding with a yield loss of 5% were 1600 nl litre(-1) h for AOT30 and 400 nl litre(-1) h for AOT40. The results are discussed in relation to the long-term critical level that is used as a guideline to protect crops against adverse effects by O3.     

Acidity of raindrop by uptake of gases and aerosol pollutants

Below-cloud raindrops acidification simulated with a simple model incorporating gas–liquid equilibriums, gas-phase mass transfer, and catalyzed SO₂ oxidation in aqueous phase with uptake of gases and scavenging of particles. Ionic contents of various species in raindrops of different size and pH are computed using one-dimensional time-variant model. The model results are based on SO₂ and NH₃ absorption and collection of calcium aerosols by raindrops with various collection mechanisms. Aqueous concentrations of (SO₂)_l and (NH₃)_l and their ionic components in raindrops are found to be increased with the fall distance from cloud base and decrease of drop size. The overall magnitude of pH enhances with the increase in drop size and transient position of raindrops in the atmosphere below the cloud base. The elevated ionic calcium in raindrops by impaction of calcium aerosols of higher inertia neutralizes the acidic components. Acidic ion contents in smaller droplets are found to be significant and resulted pH of raindrop increases with the size and neutralizing potential of alkaline species. The pH values of rainwater contents of predominant size raindrops in bulk samples corresponding to various rainfall intensities are higher as against the individual non-evaporating smaller raindrops. Results are important in view of the impact of showers on earth surfaces during rain containing large number of smaller droplets as compared to the acidification studies of bulk rainwater.     

Chemical Dynamics of Clouds at Mt. Mitchell,North Carolina

The role of clouds as the primary pathway for deposition of air pollutants into ecosystems has recently acquired much attention. Moreover, the acidity of clouds is highly variable over short periods of time. Cloud water collections were made at Mt. Mitchell State Park, North Carolina, using a real-time cloud and rain acidity/ conductivity (CRAC) analyzer during May to September 1987, 1988 and 1989 in an effort to explore extremes of chemical exposure. On the average, the mountain peak was exposed to cloud episodes about 70 percent of experimental days. The lowest pH of cloud water in nearly real-time (～10 min.) samples was 2.4, while that in hourly integrated samples was 2.6. The cloud pH during short cloud events (mean pH 3.1), whjch results from the orographic lifting mechanism, was lower than that during long cloud events (mean pH 3.5), which are associated with mesoscale or synoptic atmospheric disturbances. On the average, the pH values in nonprecipitating cloud events were about 0.4 pH unit lower than those in precipitating cloud events. Sulfate, nitrate, ammonium and hydrogen ions were found to be the major constituents of cloud water, and these accounted for -90 percent of the ionic concentration. Total ionic concentrations were found to be much higher in non-precipitating clouds (670-3,010 μeq/L) than those in precipitating clouds (220-370 μeq/L). At low acidity, ionic balance is sometimes not obtained. It is suggested that organic acids may provide this balance.

The profile of cloud water ionic concentration versus time was frequently observed to show decrease at the beginning and rising toward the end during short cloud events. Before the dissipation of clouds, a decrease in cloud water pH and an increase in ionic concentration were found. At the same time, temperature and solar radiation increased, and relative humidity and microphysical parameters (liquid water content, average droplet size, and droplet concentration) decreased. These observations suggest that evaporative dissipation of cloud droplets leads to acidification of cloud water. Mean pH of cloud water was 3.4 when the prevailing wind was from the northwest direction, and it was 3.9 when the wind was from the west direction. The effects of variations in cloud liquid water content have been separated from variations in pre-cloud pollutant concentrations to determine the relationship between source intensity and cloud water concentrations.