Some approximations for the wet and dry removal of particles and gases from the atmosphere

Semi-empirical formulae are presented which can be used to estimate precipitation scavenging and dry deposition of particles and gases. The precipitation scavenging formulae are appropriate both for in- and below-cloud scavenging and comparisons with data indicate the importance of accounting for aerosol particle growth by water vapor condensation and attachment of the pollutant to plume or cloud particles. It is suggested that both wet and dry removal of gases is usually dictated by other than atmospheric processes. Dry deposition of particles to a canopy is shown to depend on canopy height, biomass, vegetative type and mean wind. Two large-scale practical problems are addressed dealing with the relative importance of wet and dry deposition and with the sources which contribute to deposition in a specific location.     

Fog precipitation and rainfall interception in the natural forests of Madeira Island (Portugal)

Situated in the Atlantic Ocean, Madeira is a within-plate volcanic island, approximately 600 km northwest of the Western African coast. Cloud cover formed mainly of orographic origin persists on Madeira for more than 200 days per year between 800 m and 1600 m altitude. Since vegetation occupies 2/3 of the island's surface, fog precipitation, which occurs when fog droplets are filtered by the forest canopy and coalesce on the vegetation surfaces to form larger droplets that drip to the forest floor, is an important hydrological input. Rainfall interception and fog precipitation data were collected between 1996 and 2005 in the natural forests of Madeira. Six throughfall gauges were placed under the canopy of three different types of forest: high altitude tree heath forest (1580 m), secondary tree heath forest (1385 m) and humid laurisilva forest (1050 m). Fog precipitation is higher under high altitude heath forest (average canopy interception was ?225% of gross precipitation) and dependent both on altitude and vegetation type, due to different tree architecture and leaf shape. Although results are conservative estimates of fog precipitation, they point towards the importance of fog-water as a source of groundwater recharge in the water balance of the main forest ecosystems of Madeira.     

Scientific goals and experiments of the project “winter precipitation at Mount Rigi”: An overview

Wet deposition plays an important role as a mechanism for cleansing of the polluted troposphere. Fluxes of pollutants from the atmosphere to earth's surface can affect soil and aquatic ecosystems. The investigation of the pollutant incorporation into wet deposition is therefore of considerable interest for environmental research. The project “Winter precipitation at Mount Rigi” addresses the processes determining the chemical composition of wet deposition through an integrated approach considering atmospheric physical and chemical processes and their complex interactions. The investigated topics include: aerosol and gas scavenging, atmospheric chemistry (cloud water chemistry), cloud physics and dynamics. The design of the experiment, using three ground based measuring stations at the northwestern slope of the mountain, and the conceptual ideas using case study investigations are discussed.     

Orographic enhancement of wet deposition in the United Kingdom: Continuous monitoring

Continuous monitoring of cloud and rain samples at three mountain sites in the UK has allowed consideration of the long term impact of the enhancement of the wet deposition of pollutants by orographie effects, specifically the scavenging of cap cloud droplets by rain falling from above (the seeder-feeder effects). The concentration of the major pollutant ions in the cloud water is related to the relative proximity of each site to marine and anthropogenic sources of aerosol. In general, the concentrations of major ions in precipitation at summit sites exceed those in precipitation to low ground nearby by 20% to 50%. Concentrations in orographie cloud exceed those in upwind rain by between a factor of five and ten. The results are consistent with seeder-feeder scavenging of hill cloud by falling precipitation in which the average concentration of ions in scavenged hill cloud exceed those in precipitation upwind by a factor of 1.7 to 2.3 for sulphate and nitrate respectively at Dunslair Heights and 1.5 to 1.8 for sulphate and nitrate at Holme Moss. The results suggest that the parameterisation of this relationship with scavenged feeder cloud water concentrations assumed to exceed those in seeder rain by a factor of two for the production of predictive maps of wet deposition in mountainous regions of the U.K. is satisfactory.     

Monitoring of Acid Rain over Korean Peninsula

In order to investigate the temporal and spacial deposition characteristics of acid rain, five monitoring sites were set up in the central part of Korean Peninsula. Rainwater samples were collected by wet-only sampler from 1992 to 1997. The pH and conductivity values were measured and the major water soluble ionic components were also analyzed. Ion balance between anion and cation sum was calculated to check out the data quality of samples. The acidity of rainwater was influenced by the local sources and meteorological factors such as surface wind, moving path of storm, precipitation process, and so on. Backward trajectories were depicted to investigate the effect due to moving path of weather system. The rainwater shows strong acidity in winter and weak in summer. The pH and ion concentrations were highly dependent on synoptic weather system. In addition, we sampled fog/cloud at Mt. Sobaek (BAPMoN Station) from June to August 1995 and characterized the fog/cloud chemistry according to surface wind system of sampling site. The volume-weighted mean pH of fog/cloud samples is 4.39 at Mt. Sobaek during the sampling period.     

Chemical deposition to a high elevation red spruce forest

A preliminary analysis of O₃, SO₂, SO _inf4 ^sup2? , and total NO _inf3 ^sup? deposition to the red spruce forest on the summit of Whitetop Mountain, Virginia, illustrates uncertainties in analysis methodologies, establishes the relative importance of three deposition pathways, and suggests areas for further research. Results are presented here for an analysis of the dry, wet (precipitation), and cloud water deposition pathways for the four chemical species during a 26-day period in April and May 1986. Dry and cloud water depositions are estimated using available models along with air and cloud water chemistry measurements made at the summit. For water soluble species, depositions by precipitation and cloud interception are found to be comparable in magnitude, while dry deposition appears to be about an order of magnitude less. High levels of atmospheric O₃ lead to a large estimate of 03 deposition (on a mass flux basis) when compared to the estimated deposition of gaseous SO₂. This is in spite of the fact that computed SO₂ dry deposition velocities exceed those for O₃. Model uncertainties are large for both dry deposition velocity and cloud water flux computations, and some bias in computations probably exists because of the application of the models to a complex terrain situation. Field evaluation of the cloud water deposition model is of greatest priority because of the apparent relative importance of that deposition pathway.     

Cloud Water Deposition to Forest Canopies of Cryptomeria Japonica at Mt.Rokko, Kobe, Japan

Cloud water deposition to canopies of Cryptomeria japonica at Mt.Rokko, Kobe, Japan, was estimated from throughfall measurements and fog water collections carried out during a full year. Annual cloud frequency was 11.5–15.5% and liquid water content (LWC) was 0.059 g/m³. Since cloud water deposition on to forest canopies was significantly correlated with the amount of fog water collected, the former parameter could be quantitatively derived from throughfall measurements. Annual cloud water deposition on to Cryptomeria canopies was 1420–2860 mm (Av. 2140 mm), corresponding to 90–180% (Av. 122%) of annual rainfall. The rate of deposition was higher at the mountain ridge and the forest edge than at the mountain side and the forest interior. Annual deposition of SO₄ ^2?, NO₃ ^?, H⁺ and NH₄ ⁺ from cloud water was estimated as 204, 153, 2.5 and 58 kg/ha, respectively, equivalent to 5.8–11.7 times the corresponding deposition via rain. The values are equal to, or exceed, the maximum deposition reported for Appalachian forests in the eastern United States. Multiple regression analyses indicate that cloud water deposition on to Cryptomeria canopies was significantly correlated with the following three parameters: cloud frequency, LWC, and wind speed. Thus, these three factors apparently control cloud water deposition on to forest canopies.     

Ice crystal observations and the degree of riming in winter precipitation

Since snow crystals provide information on the processes leading to their formation and growth, their observation gives insight to the microphysics of cloud and precipitation. The capture of supercooled cloud droplets by snow crystals (riming) forms an important link between precipitation and cloudwater and thus plays an important role in wet deposition. In the project ‘Winter Precipitation at Mount Rigi’ ice crystals are collected at two stations at different elevations. The shape, size and degree of riming of each crystal are analyzed for more than 10000 crystals. Differences in the degree of riming of the crystals between the higher and the lower station are discussed. With the aid of Doppler radar data the location of snow crystal origin is estimated. Furthermore a relationship between the degree of riming of snow crystals and the vertical Doppler velocities is established.     

The application of210Pb inventories in soil to measure long-term average wet deposition of pollutants in complex terrain

The radionuclide²¹⁰Pb derived from gaseous²²²Rn is present in particle form in the atmosphere attached to the same aerosols which contain the bulk of the pollutant sulphur and nitrogen. When scavenged from the atmosphere by precipitation, the²¹⁰Pb is readily attached to organic matter in the surface horizons of soil. The inventory of²¹⁰Pb in soil can be used to measure the spatial variation in wet (or cloud) deposition within a region due to orography or land use, averaged over several decades (half life of²¹⁰Pb is 22.3 years). Measurements of soil²¹⁰Pb inventories along a transect through complex terrain in north Britain were made to quantify the orographic enhancement of wet deposition, at Great Dun Fell in Cumbria. At the hill summit (～800m asl) precipitation of approximately 2000 mm year^?1 exceeds that on the low ground upwind by a factor of 2.0. The inventory of²¹⁰Pb increases along the same transect by a factor of 3.3, due to seeder-feeder scavenging of orographic cloud. The measurements show that the average ratio of concentrations in scavenged orographic cloud to rain upwind of the hills is 2.2. These data are entirely consistent with the studies of the variation in major ion concentration with altitude at Great Dun Fell and elsewhere. The modelling procedures developed to provide estimates of wet deposition throughout the UK uplands are shown to be consistent with these new field data.     

Contributions of cloud processes to precipitation chemistry in mixed phase clouds

The role clouds play as processors of atmospheric aerosols and trace gases was studied along the slope of Mt. Rigi in central Switzerland. Upon cloud formation many aerosols and trace gases are efficiently scavenged by cloud drops. The cloud drops can enhance removal of pollutants from the atmosphere by transferring them to snow or rain which falls rapidly to the ground. This often occurs through a process known as riming, where falling ice crystals capture cloud drops. When ice crystals are grown primarily via water vapor deposition, without significant capture of cloud drops, however, the cloud drops isolate atmospheric pollutants from the precipitation process, thereby inhibiting their deposition. Increased riming results in increased precipitation ion concentrations. The extent of ice crystal riming at times exhibits spatial inhomogeneities with greater riming apparent near the mountain summit. Variations in cloud chemistry with drop size indicate that bulk cloudwater composition is not an accurate predictor for the composition of cloud drops captured by the ice crystals.     

Chemical Characterization of Acid Fog and Rain in Northern Japan Using Back Trajectory and Oblique Rotational Factor Analysis

Fog/cloud and rain water were collected at the mountainside of Hachimantai range in northern Japan and rain water was also collected at Akita City in order to investigate the air pollutant scavenging mechanism. The concentrations of various ions in these samples were analyzed, and the fog drop size and the wind direction were measured at each fog event. The fog at Hachimantai range had a very high total ion concentration, and was considerably acidified by non sea salt (nss-) SO₄ ^2? and NO₃ ^?, compared with the rain at Akita and all sites in Hachimantai range. Using the oblique rotational factor analysis, three factors were extracted as the air pollutants; A: (NH₄)₂SO₄+H₂SO₄, B: sea salts+HNO₃+H₂SO₄, C: NH₄NO₃+OH^?. These salts are well-known as the cloud condensation nuclei (CCN). Combining the factor analysis with the 72h back trajectory at 850hPa level, the contribution of Factor A was closely connected to the long-range transportation of anthropogenic or natural aerosol in air masses of continental origin.     

Canopy level fog occurrence in a tropical lowland forest of French Guiana as a prerequisite for high epiphyte diversity

Fog frequency and the meteorological processes leading to fog formation have never been studied in depth in tropical lowland forest areas. This study provides detailed evidence of frequent fog occurrence in lowland valleys of central French Guiana. Fog frequency showed a clear diurnal course, with a maximum before sunrise; average fog duration was 4.6 h. The diurnal course of visibility was positively correlated with the diurnal course of humidity in the above-canopy air. Fog persistence correlated significantly with atmospheric parameters during the dry season, but not during the rainy season. The main trigger of fog development in the lowland forest seemed to be precipitation, leading to higher soil moisture, greater evapotranspiration and, thus, higher water content of air. An increasing temperature difference between valley and hill sites after sunset, together with more frequent down-slope winds during nights with long fog periods, points at some influence of katabatic flows. The frequent occurrence of fog in the valleys correlated with significantly higher epiphyte diversities in valley forests as compared to hill forests, and supported the occurrence of the hitherto undescribed, epiphyte-rich “tropical lowland cloud forest” (LCF) in the valleys. The higher epiphyte diversity in LCF coincided with significantly higher relative air humidity in LCF than in hill forest. The ecological benefits of fog for the epiphytes in LCF are surplus of moisture and delayed onset of the stress period, particularly in the dry season.     

Acid pollutants in air and precipitaion/deposition at the Sudeten Mountains,Poland

The results of several separately performed field studies on air quality in south-western Poland (Black Triangle) are presented In the period 1988–1993 atmospheric aerosol measurement and precipitation/deposition samples were collected at three locations of mountain region (810–1490 m asl). Precipitation was monitored in forest ecosystem using a 24-gauge network was carried out during June–October 1992 and 1993. The occurence of cloud at ground level over hills is difficult to categorize and quantify in mountain terrain and has constituted a basic part of our studies. Precipitation/deposition samples (seven rain and three cloud collectors) in the Karkonosze Mountains were collected over the period 1994–1995 (four field campaigns were conducted) to examine aqueous chemical interactions between constituents in samples. Meteorological data measured at the site included temperature, humidity, wind speed and direction and the amount of precipitation.     

The roles of salt (sodium nitrate) and fog in weathering: a laboratory simulation of conditions in the northern Atacama Desert, Chile

A laboratory experiment was used as a model to investigate interactions within a hyper-arid and hyper-saline weathering environment based on conditions observed in the Atacama Desert, northern Chile. The experimental design produced a matrix of 18 different weathering environments with six levels of salt (sodium nitrate) availability and three levels of fog precipitation. The experiment took place over an 11-week period. Over this time, 10 weekly fog applications modified the experimental conditions. From a theoretical perspective, the weekly fog applications generate an open rather than a closed system, which may be more representative of conditions in the field. The breakdown of the chalk blocks used was assessed in two ways. Firstly, qualitative observations were made at weekly intervals of the nature of morphological changes. Secondly, at the end of the experiment, breakdown was assessed by counting the number of discrete pieces greater than 1 g liberated by each block. The electrical conductivity at the base of each block was also measured. Collectively, the results indicate that fog appears to control the rate of breakdown and that salt availability controls the timing of the response. The style of breakdown was similar irrespective of the fog and salt levels. The morphological observations show the results of a sequence of events, with the blocks evolving as the experiment progresses; as such, they provide an experimental example of the role of inheritance in weathering processes.     

Modeling of first plume encounters with precipitation

A regional air pollutant transport model was used to simulate the fate of S emissions in the northeast United States. Hourly calculations were analyzed to describe trajectory characteristics and mass balances as pollutant trajectories first encounter precipitation during transport away from emission sources. Model results include air concentrations of SO₂ and sulfate, dry deposition values, and sulfate concentrations scavenged by precipitation, along with trajectory statistics. Results of sensitivity tests are compared to base case simulations which consider all precipitation events as a means of suggesting priorities for future regional transport model development.     

Prospective use of collected fog water in the restoration of degraded burned areas under dry Mediterranean conditions

A mountainous plot located in the interior of the Valencia region (east coast of the Iberian Peninsula) was identified for reforestation using the fog-water collection potential prevailing in the area. Fog data were obtained by means of an instrument ensemble consisting of a passive cylindrical fog-water collector, a rain gauge, a wind direction and velocity sensor and a temperature and humidity probe. Preliminary results gave rise to the additional deployment of a low-cost 18-m² flat-panel collector connected to three 1000-l tanks for larger scale fog-water collection and storage. The 2007 annual rate of fog water that could be derived from the instrument ensemble amounted to 3.3 l/m²/day, which turn out to fill up the storage tanks completely in only 5 months, even though the flat-panel collector could not be operative 100% of the time. The study made use of the in situ stored water and a micro-irrigation network to irrigate a plot of reforestation seedlings through small water pulses localized deep in the planting hole during the summer dry period. Until the present, this forest location had always shown a difficult self-recovery due to the high level of land degradation resulting from recurrent forest fires in the past. Results indicate that survival rates and seedling performance of the two species planted, Pinus pinaster and Quercus ilex, improved with the use of small timely waterings and additional treatments with composted biosolid.     

Extractable iron and organic matter in the suspended insoluble material of fog droplets

In this work the formation and composition of aggregates between metals and organic material is studied in real fog samples. In a preliminary experiment it has been found that concentrated cloud samples form a yellow-brown precipitate in the presence of Fe(III). Standards of humic acids and fulvic acids co-precipitate with Fe(III), forming similar aggregates i.e. iron-humates (Fe-HA) and iron-fulvates (Fe-FA). By comparing the solubility properties of aggregates by extracting organic carbon (OC) in different pH conditions, it has been observed that fog droplet particulate samples are characterised by solubility properties more similar to those of Fe-HA than Fe-FA. Dilute alkaline solutions can also easily extract organic refractory substances that form aggregates with metals. The recoveries of the total extractable organic matter (accounting for 12% of total insoluble carbon and 15% of particulate mass) are similar to those of humic-like substances (HULIS) from particulate samples. The chromatographic behaviour and functional group characteristics measured in the alkali-extract fraction of precipitated aggregates with iron and in the insoluble particulate of fog samples, are those of humic-like material. Thus, soluble HULIS are able to interact with iron to form particulate, but the composition of a large fraction of insoluble organic carbon is still unknown. These findings have implications on the solubility and surface tension properties of fog droplets and can therefore potentially influence droplet formation, as well as cloud chemical and photochemical processes.     

Soil acidification along a topographic gradient on Roundtop Mountain,Quebec, Canada

We examined the effects that different acidic loadings have had on soil chemistry along a toposequence on Roundtop Mountain. Due to fog interception by the forest canopy, the amount of time in the clouds is a major factor determining the amount and chemistry of precipitation reaching the soil and hence, acid precipitation loading is directly related to elevation. Soils on a transect from 520 to 850 m show a pattern of chemistry that corresponds to the loading of acidic deposition. Soil solutions collected at two elevations show different levels of both SO₄ and Cl, two of the anions in fog water as well as differences in concentrations of H ion and Al. Surface horizons of soils located at 850 m have pH in water as low as 3.7; in mineral horizons base saturation is extremely low (<5%) and Al saturation exceeds 95% in many cases. In contrast, lower on the mountain slope (below 650 m), pH is slightly higher (about 4.1) and base saturation rises to over 50% for the same soil horizons. There is a clear relationship between soil acidification and position on the mountain.     

Air Pollution Processing by Radiation Fogs

Several fog episodes occurred in California’s San Joaquin Valley during winter 2000/2001. Measurements revealed the fogs to generally be less than 50 m deep, but to contain high liquid water contents (frequently exceeding 200 mg/m³) and large droplets. The composition of the fog water was dominated by ammonium (median concentration?=?608 μN), nitrate (304 μN), and organic carbon (6.9 ppmC), with significant contributions also from nitrite (18 μN) and sulfate (56 μN). Principal organic species included formate (median concentration?=?32 μN), acetate (31 μN), and formaldehyde (21 μM). High concentrations of ammonia resulted in high fog pH values, ranging between 5.8 and 8.0 at the core measurement site. At this high pH aqueous phase oxidation of dissolved sulfur dioxide and reaction of S(IV) with formaldehyde to form hydroxymethanesulfonate are both important processes. The fogs are also effective at scavenging and removal of airborne particulate matter. Deposition velocities for key solutes in the fog are typically of the order of 1–2 cm/s, much higher than deposition velocities of precursor accumulation mode aerosol particles. Variations were observed in deposition velocities for individual constituents in the order NO₂ ^??>?fogwater?>?NH₄ ⁺?>?TOC ～ SO₄ ^2??>?NO₃ ^?. Nitrite, observed to be enriched in large fog drops, had a deposition velocity higher than the average fogwater deposition velocity, due to the increase in drop settling velocity with size. Species enriched in small fog drops (NH₄ ⁺, TOC, SO₄ ^2?, and NO₃ ^?) all had deposition velocities smaller than observed for fogwater. Typical boundary layer removal rates for major fog solute species were estimated to be approximately 0.5–1 μg m^?3 h^?1, indicating the important role regional fogs can play in reducing airborne pollutant concentrations.