The scavenging of nitrate by clouds and precipitation

A model with spectral microphysics was developed to describe the scavenging of nitrate aerosol particles and HNO₃ gas. This model was incorporated into the dynamic framework of an entraining air parcel model with which we computed the uptake of nitrate by cloud drops whose size distribution changes with time because of condensation, collision-coalescence and break-up. Significant differences were found between the scavenging behavior of nitrate and our former results on the scavenging behavior of sulfate. These reflect the following chemical and microphysical differences between the two systems:

1. nitrate particles occur in a larger size range than sulfate particles.
2. HNO₃ has a much greater solubility than SO₂ and is taken up irreversibly inside the drops in contrast to SO₂.
3. nitric acid in the cloud water is formed directly on uptake of HNO₃ gas whereas on uptake of SO₂ sulfuric acid is formed only after the reaction with oxidizing agents such as e.g., H₂O₂ or O₃.
4. nitrate resulting from uptake of HNO₃ is confined mainly to small drops, whereas sulfate resulting from uptake of SO₂ is most concentrated in the largest, oldest drops, which have had the greatest time for reaction.

Sensitivity studies showed that the nitrate concentration of small drops is significantly affected by the mass accommodation coefficient.     

Increasing cloud in a warming world

Cloud amount records for the U.S.A. have been analyzed in the context of the warming world analogue model described by Lough et al. (1983). Cloud amount increases over practically the entire U.S.A. in all seasons. This result considerably strengthens the more tentative conclusion of Henderson-Sellers (1986) that cloud amount increases over Europe in the same warming world scenario. These results are in contrast to the few numerical model predictions of cloud changes in warming world experiments. A possible, rather tantalizing, conclusion is that current GCM cloud prediction schemes tend to enhance temperature increases through cloud-climate feedback whereas the historical data could suggest a negative feedback. Part, possibly all, of this difference may be the result of the fundamental distinction between the two experimental scenarios: the equilibrium change modelled by GCMs as compared to the smaller transient change represented by the historical analogue. On the other hand the current real-world experiment is, itself, a transient change in boundary and atmospheric conditions. At the least, surface-observed cloudiness seems to offer a useful and complementary data source with which to examine one aspect of the performance of numerical climate models.     

Fog chemistry during EUMAC Joint Cases: Analysis of routine measurements in southern Germany and model calculations

Summary The role of fog events for acid production and moist deposition in southern Germany during three EUMAC Joint Cases has been investigated by analysis of routine measurements and simulations with a one-dimensional fog-chemistry model. To identify the chemical and meteorological conditions, routine measurements by different institutions have been interpreted. The periods under consideration include a smog episode with low photooxidant concentrations during the Winter Case in February 1982. The Wet Case in spring 1986 represents a period with higher photooxidant concentrations. Conditions which are mostly characterized by low SO₂ and oxidant concentrations and comparatively high pH-values in the fog are given during the SANA 1 case in autumn 1990. Fog mostly occurs as a subscale phenomenon, but sometimes it can also cover large areas and it can contribute significantly to moist deposition.The model results indicate that the liquid phase sulfate production in the fog layer may even exceed the gas phase production during 24 hours within a layer of the same height occasionally. On the other hand, during the SANA 1 case the sulfate production in the fog was extremely low at night due to lack of oxidants and SO₂. Depending on the dissipation time of the fog a remarkable effect on the photolysis rates is possible. Since a significant amount of particulate mass is lost by moist deposition during fog, it is evident that fog events can have a noticeable effect on some of the gas phase constituents which are easily soluble.With 17 Figures     

Simulation of marine stratocumulus: effect of precipitation parameterization and sensitivity to droplet number concentration

Marine stratocumulus observations show a large variability in cloud droplet number concentration (CDNC) related to variability in aerosol concentration. Changes in CDNC modify the cloud reflectivity, but also affect cloud water content, cloud lifetime, and cloudiness, through changes in precipitation. In mesoscale models and general circulation models (GCMs), precipitation mechanisms are parameterized. Here we examine how the precipitation parameterization can affect the simulated cloud. Simulations are carried out with the one-dimensional version of the hydrostatic primitive equation model MAR (Modéle Atmosphérique Régional) developed at the Université catholique de Louvain. It includes a E- turbulence closure, a wide-band formulation of the radiative transfer, and a parameterized microphysics including prognostic equations for water vapour, cloud droplets and rain drops concentrations. In a first step, the model is used to simulate a horizontally homogeneous stratocumulus deck observed during the Atlantic Stratocumulus Transition Experiment (ASTEX) on the night of 12–13 June 1992. The observations show that the model is able to realistically reproduce the vertical structure of the cloud-topped boundary layer. In a second step, several precipitation parameterizations commonly used in mesoscale models and GCMs are tested. It is found that most parameterizations tend to overestimate the precipitation, which results in an underestimation of the vertically integrated liquid water content. Afterwards, using those parameterizations that are sensitive to CDNC, several simulations are performed to estimate the effect of CDNC variations on the simulated cloud. Based upon the simulation results, we argue that currently used parameterizations do not enable assessment of such a sensitivity.     

Effects of prescribed initial cloud droplet spectra on convective cloud and precipitation developments under different thermodynamic conditions: A modeling and observational study

A two-dimensional cloud model with bin microphysics was used to investigate the effects of cloud condensation nuclei (CCN) concentrations and thermodynamic conditions on convective cloud and precipitation developments. Two different initial cloud droplet spectra were prescribed based on the total CCN concentrations of maritime (300 cm^− 3) and continental (1000 cm^− 3) air masses, and the model was run on eight thermodynamic conditions obtained from observational soundings. Six-hourly sounding data and 1-hourly precipitation data from two nearby weather stations in Korea were analyzed for the year 2002 to provide some observational support for the model results.For one small Convective Available Potential Energy (CAPE) ( 300 J kg^− 1) sounding, the maritime and continental differences were incomparably large. The crucial difference was the production of ice phase hydrometeors in the maritime cloud and only water drops in the continental cloud. Ice phase hydrometeors and intrinsically large cloud drops of the maritime cloud eventually lead to significant precipitation. Meanwhile negligible precipitation developed from the continental cloud. For the three other small CAPE soundings, generally weak convective clouds developed but the maritime and continental clouds were of the same phases (both warm or both cold) and their differences were relatively small.Model runs with the four large CAPE ( 3000 J kg^− 1) soundings demonstrated that the depth between the freezing level (FL) and the lifting condensation level (LCL) was crucial to determine whether a cloud becomes a cold cloud or not, which in turn was found to be a crucial factor to enhance cloud invigoration with the additional supply of freezing latent heat. For two large CAPE soundings, FL–LCL was so deep that penetration of FL was prohibitive, and precipitation was only mild in the maritime clouds and negligible in the continental clouds. Two other soundings of similarly large CAPE had small FL–LCL, and both the maritime and continental clouds became cold clouds. Precipitation was strong for both but much more so in the maritime clouds, while the maximum updraft velocity and the cloud top were slightly higher in continental clouds. Although limited to small CAPE cases, more precipitation for smaller FL–LCL for a selected group of precipitation and thermodynamic sounding data from Korea was in support of these model results in its tendency.These results clearly demonstrated that the CCN effects on cloud and precipitation developments critically depended on the given thermodynamic conditions and not just the CAPE but the entire structure of the thermodynamic profiles had to be taken into account.     

Numerical study of the cloud seeding effects

The microphysical model with the bulk water parameterization is applied to simulated both contact and deposition nucleation as well as the imersion freezing for unseeded cases and the cases immediately after seeding performed for the cold continental Cb clouds with small cloud droplets. The injection of agent AgI is performed in temperature region between –8°C and –12°C. The four groups of sensitivity experiments are executed.

Regular and seasonal behaviour of atmospheric radio noise field strength (ARNFS) over low latitude station calcutta

Summary The electromagnetic radiation of cloud discharge known as atmospheric radio noise field strength (ARNFS) shows a gradual fall from a frequency of 9 kHz to 81 kHz as studied over a period of two years at Calcutta, very close to Bay of Bengal. The main characteristic features of ARNFS at Calcutta are that-(i) ARNFS shows that midday median value is smaller than midnight median value in all months, (ii) level of daily minimum is higher in February and monsoon compared to other seasons, (iii) sunrise effect and sunset effect are well correlated with local sunrise and sunset times, (iv) the magnitude of sunrise fade and sunrise fade rate are maximum in April and lowest during winter period, (v) the magnitude of sunset fade is higher in premonsoon and postmonsoon while it is lowest in monsoon, (vi) number of occurrence of both sunrise effect and sunset effect is remark-ably smaller in monsoon. The positions of the sun and of atmospheric sources are jointly the causes of seasonal and diurnal variations. The missing of sunrise effect and sunset effect are due to local cloud activity and variation of electron density during geomagnetic storms.With 7 Figures     

Advertent/inadvertent changes in the spatial distribution of rainfall in the central coastal plain of Israel

Analysis of recent rainfall normals reveals an unusual spatial pattern where the rainfall increases with the distance from the sea over the central coastal plain of Israel. Applying a multiple regression technique separately to rainfall amounts for the two randomized experiments of cloud seeding of seeded days and not seeded days, leads to the conclusion that the inadvertent influence of recent urbanization processes along the coastal plain are the cause of this phenomenon, rather than the advertent artificial cloud seeding. The seeding effect at the target area, on the other hand, seems to increase the inhomogeneity of the spatial structure of the rainfall distribution.     

Estimates of diabatic wind speed profiles from near-surface weather observations

In this paper we analyse diabatic wind profiles observed at the 213 m meteorological tower at Cabauw, the Netherlands. It is shown that the wind speed profiles agree with the well-known similarity functions of the atmospheric surface layer, when we substitute an effective roughness length. For very unstable conditions, the agreement is good up to at least 200 m or z/L–7(z is height, L is Obukhov length scale). For stable conditions, the agreement is good up to z/L1. For stronger stability, a semi-empirical extension is given of the log-linear profile, which gives acceptable estimates up to ~ 100 m. A scheme is used for the derivation of the Obukhov length scale from single wind speed, total cloud cover and air temperature. With the latter scheme and the similarity functions, wind speed profiles can be estimated from near-surface weather data only. The results for wind speed depend on height and stability. Up to 80 m, the rms difference with observations is on average 1.1 m s^–1. At 200 m, 0.8 m s^–1 for very unstable conditions increasing to 2.1 m s^–1 for very stable conditions. The proposed methods simulate the diurnal variation of the 80 m wind speed very well. Also the simulated frequency distribution of the 80 m wind speed agrees well with the observed one. It is concluded that the proposed methods are applicable up to at least 100 m in generally level terrain.     

中国区域气溶胶对东亚夏季风的可能影响（I）：硫酸盐气溶胶的影响

利用NCAR的新一代GCM CAM3.0模式离线耦合一个气溶胶同化系统,模拟研究了中国区域硫酸盐气溶胶的直接气候效应对东亚夏季风及其降水的影响。结果显示：中国区域硫酸盐气溶胶引起全球平均的直接辐射强迫为-0.25 W/m²,中国内陆约25°N以北普遍降温,而海表温度升高。由此导致海陆温差缩小,东亚夏季风强度减弱,中国地区季风降水明显减少,而尤以积云降水减少起主要作用。硫酸盐气溶胶对中国地区的对流活动起抑制作用。     

中国区域气溶胶对东亚夏季风的可能影响（I）：硫酸盐气溶胶的影响

 利用NCAR的新一代GCM CAM3.0模式离线耦合一个气溶胶同化系统,模拟研究了中国区域硫酸盐气溶胶的直接气候效应对东亚夏季风及其降水的影响。结果显示：中国区域硫酸盐气溶胶引起全球平均的直接辐射强迫为-0.25 W/m²,中国内陆约25°N以北普遍降温,而海表温度升高。由此导致海陆温差缩小,东亚夏季风强度减弱,中国地区季风降水明显减少,而尤以积云降水减少起主要作用。硫酸盐气溶胶对中国地区的对流活动起抑制作用。     

Particle size distributions of methanesulfonate in the tropical pacific marine boundary layer

Fourteen high-volume cascade impactor samples were collected during a January-February, 1990, research cruise in the tropical Pacific from Panama to 180°. Aqueous extracts of the samples were analyzed for methanesulfonate (MSA), sulfate, and the seasalt tracer ion magnesium. The majority of MSA size distributions showed no pronounced maximum on submicrometer particles, as has been observed elsewhere. Analysis of the data indicated that MSA was distributed essentially uniformly with the effective surface area of particles >0.5 m in radius, which were primarily seasalt. Relatively less MSA was found in smaller particles which were primarily sulfate. These results are consistent with those from theoretical and laboratory experimental studies reported in the literature which suggest that MSA produced from photochemical oxidation of dimethylsulfide condenses on pre-existing particles in strong preference to nucleating into new particles. This implies that MSA may not contribute appreciably to enhancing cloud condensation nucleus populations in the remote tropical marine atmosphere.     

Airborne measurements of dimethylsulfide,sulfur dioxide,and aerosol ions over the Southern Ocean South of Australia

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.     

The APE-THESEO Tropical Campaign: An Overview

The APE-THESEO campaign was held from 15 February to 15 March 1999 from the Seychelles in the western Indian Ocean. APE-THESEO stands for Airborne Platform for Earth observation — (contribution to) the Third European Stratospheric Experiment on Ozone. The campaign aimed to study processes controlling the low water content of the stratosphere, including the mechanisms of cloud formation in the tropical tropopause region, and transport processes, studied using measurements of long-lived trace gases and ozone.Two aircraft were used: the high-altitude research aircraft, M-55 Geophysica, which can fly up to 21 km, and the Falcon of the Deutsches Zentrum für Luft- und Raumfahrt, a tropospheric aircraft. Seven flights were performed, including the first simultaneous in situ and remote sensing of sub-visible cirrus clouds, the first interception of sub-visible cirrus using in-flight guidance from a path-finding aircraft, and guided descent of a high-altitude research aircraft into the anvil cloud at the top of a tropical cyclone. In this paper we describe the payload used, the objectives for each flight, and the meteorological conditions encountered. First results show that a new type of cloud, which we have dubbed ultra-thin tropical tropopause cloud (UTTC), has been observed frequently, and observed to cover areas of 10⁵ km². The frequent coincidence of the tropopause and hygropause implies that the western Indian Ocean played an important role in the dehydration of the lower tropical stratosphere during the season of the mission. UTTCs, sub-visible cirrus, and visible cirrus, have all been implicated in the observed dehydration. Tracer measurements indicate little mixing of stratospheric air into the upper tropical troposphere.     

On the scavenging of organic gases by cloud and raindrops: I. A theoretical and experimental study of acetaldehyde absorption and desorption for water drops in air

Our previously developed theoretical models for describing the rate at which water-soluble atmospheric trace gases are scavenged by cloud and rindrops were evaluated for the case of acetaldehyde being absorbed and desorbed by water drops of radii between 250 to 2500 m radius. The experimental verification of our theoretical predictions was carried out in the UCLA 33 m high precipitation shaft in which falling water drops were allowed to come to terminal velocity before passing through a chamber of variable lengths filled with air containing acetaldehyde at various partial pressures. For all drop sizes studied, the experimental results and the theoretical predictions were in reasonable agreement.     

Hydrologic-energy balance constraints on the Holocene lake-level history of lake Titicaca, South America

A basin-scale hydrologic-energy balance model that integrates modern climatological, hydrological, and hypsographic observations was developed for the modern Lake Titicaca watershed (northern Altiplano, South America) and operated under variable conditions to understand controls on post-glacial changes in lake level. The model simulates changes in five environmental variables (air temperature, cloud fraction, precipitation, relative humidity, and land surface albedo). Relatively small changes in three meteorological variables (mean annual precipitation, temperature, and/or cloud fraction) explain the large mid-Holocene lake-level decrease (85 m) inferred from seismic reflection profiling and supported by sediment-based paleoproxies from lake sediments. Climatic controls that shape the present-day Altiplano and the sediment-based record of Holocene lake-level change are combined to interpret model-derived lake-level simulations in terms of changes in the mean state of ENSO and its impact on moisture transport to the Altiplano.     

The Drop Size-Dependence of Iron and Manganese Concentrations in Clouds and Fogs: Implications for Sulfate Production

Differences in total iron and manganese concentrations between large (d > 23 m) and small (4 < d < 23 m) cloud and fog drops were investigated at four locations in the United States. The study examined coastal stratus and stratocumulus clouds in southern California and northern Oregon, frontal and orographic clouds at Mt. Mitchell, North Carolina, and radiation fogs in California's San Joaquin Valley. The speciation of iron as a function of drop size was also examined in some fog samples from the San Joaquin Valley. Total iron and manganese concentrations were generally higher in large drops than in small drops in clouds sampled at Mt. Mitchell and along the southern California coast. These species were typically enriched in small drops at the Oregon coast and San Joaquin Valley sites. Ratios of dissolved Fe(III) to total dissolved Fe ranged from 0.88 to 0.93 in small fog drops. Non-uniform distributions of iron and manganese across the drop size spectrum can influence rates of metal catalyzed S(IV) autooxidation. Approximately 50% of the sampled clouds were calculated to experience autooxidation rate enhancements greater than 30% due to variations in drop acidity and catalyst concentrations with drop size.     

On the scavenging of SO2 by cloud and raindrops: I. A theoretical study of SO2 absorption and desorption for water drops in air

An extention of our previous theory for trace gas absorption into freely-falling cloud and raindrops is presented. This theory describes the convective diffusion of a trace gas through air and into a water drop with internal circulation, the drop falling at its terminal velocity. Using flow fields for the circulating water inside and for the moving air outside the drop, obtained by numerical solutions to the Navier—Stokes equation of motion, we numerically solved the convective diffusion equation to determine the uptake of SO₂ by water drops of various sizes, time exposure to the gas phase, and concentration of SO₂ in the gas phase. It was found that for drops of radius larger than 1 mm and relatively low gas concentrations (10 ppb (v)), resistance to gas diffusion lies mainly in the gas phase; while for drops of radius less than 500 m and gas concentrations larger than those found in the atmosphere (1% (v)), the resistance to diffusion lies primarily in the liquid phase. With drop sizes and gas concentrations between these limits, the rate of SO₂ uptake is controlled by a coupled resistance to diffusion inside and outside the drop. In addition to our general model, a simplified version was formulated which allows considerable savings in computer time for evaluation and improved ease of handling without significant loss of accuracy. A comparison between our simplified model and that of Barrie (1978) shows that the boundary-layer approach of Barrie may be a useful alternate approach to estimating trace gas absorption by water drops, provided appropriate values are chosen for the thickness of the boundary layers involved.     

Seasonal variations of anthropogenic sulfate aerosol and direct radiative forcing over China

Summary Regional climate model (RegCM2) and sulfur transport model (NJUADMS) were combined to simulate the distribution of anthropogenic sulfate aerosol burden over China, where a look up table method was applied to illustrate sulfate formation from SO₂-oxidation. Direct radiative forcing of sulfate aerosol was further estimated using the scheme suggested by Charlson et al (1991). Investigations show that the annual average total sulfate column over mainland China is 2.01mg/m² with high value in East and Central areas (more than 7mg/m²). The annual average direct radiative forcing of China is about –0.85W/m². The forcing can reach –7W/m² in Central and East China during the winter season. Total sulfate column shows significant seasonal variations with winter maximum-summer minimum in the Southern part of China and spring maximum-autumn minimum in the northern part of China. Strong seasonal cycles of direct radiative forcing are also found due to the influence of total sulfate column, cloud, relative humidity and the reflectivity of underlying surfaceReceived May 16, 2001; accepted August 5, 2002 Published online: May 8, 2003     

Cloud optical properties at Bergen (Norway) based on the analysis of long-term solar irradiance records

Summary Ground-based measurements of incoming solar irradiance and cloud observations during a 26 year period (1965–1990) at Bergen, Norway were used in conjunction with a comprehensive radiation model to infer the cloud optical depth under completely overcast conditions.Month-to-month and year-to-year (April through October) statistics of the cloud optical depth and observed cloud forms are presented. Some climate-related features, specifically, diurnal and seasonal variabilities in are examined. The effects of local cloudiness are pointed out and discussed. There appears to be a slight trend towards increasing cloud optical depth at noon during the warm period of the year. The possible uncertainties due to unknown size of cloud droplets are analyzed by model simulations. Possible directions for future research are suggested provided more meteorological and/or satellite information is available.With 9 Figures