Computer modelling of clouds at Kleiner Feldberg

The airflow, cloud microphysics and gas- and aqueous-phase chemistry on Kleiner Feldberg have been modelled for the case study of the evening of 1 November 1990, in order to calculate parameters that are not easily measured in the cloud and thus to aid the interpretation of the GCE experimental data-set. An airflow model has been used to produce the updraught over complex terrain for the cloud model, with some care required to ensure realistic modelling of the strong stable stratification of the atmosphere. An extensive set of measurements has been made self-consistent and used to calculate gas and aerosol input parameters for the model. A typical run of the cloud model has calculated a peak supersaturation of 0.55% which occurs about 20 s after entering cloud where the updraught is 0.6 m s^–1. This figure has been used to calculate the efficiency with which aerosol particles were scavenged; it is higher than that calculated by other methods, and produces a cloud with slightly too many droplets. A broad cloud droplet size spectrum has been produced by varying the model inputs to simulate turbulent mixing and fluctuations in cloud parameters in space and time, and the ability of mixing processes near cloud-base to produce a lower peak supersaturation is discussed. The scavenging of soluble gases by cloud droplets has been observed and departures from Henry's Law in bulk cloud-water samples seen to be caused by variation of pH across the droplet spectrum and the inability of diffusion to adjust initial distributions of highly soluble substances across the spectrum in the time available. Aqueous-phase chemistry has been found to play a minor role in the cloud as modelled, but circumstances in which these processes would be more important are identified.     

气溶胶核化清除的化学效应 I：云滴化学非均匀性的研究

本文将水汽在云滴上凝结增长的物理过程与气溶胶、气体的化学过程相结合，对气溶胶核化清除的化学效应进行了研究。 计算结果表明:气溶胶的核化清除造成了云滴化学成分随云滴大小分布的非均匀性，这种非均匀性又对云滴内发生的气体吸收、液相氧化产生影响。 本文还比较了不同污染状况下，不同大小的云滴内气溶胶核化清除与液相氧化对云滴化学的相对贡献的差异。 因此，这种云滴化学的非均匀性(云微化学)的研究对于云化学的野外观测及数值模拟都是重要的。     

On the effect of the chemical composition of atmospheric aerosol particles on nucleation scavenging and the formation of a cloud interstitial aerosol

Nucleation scavenging and the formation of a cloud interstitial aerosol (CIA) were theoretically studied in terms of the chemical composition of atmospheric aerosol particles. For this study, we used our air-parcel cloud model, which includes the entrainment of air and detailed microphysics, for determining the growth and interaction of aerosol particles and drops. Maritime and remote continental aerosol particle spectrums were used whose size distributions were superpositions of three log-normal distributions, each of a prescribed chemical composition. Our results show (1) that the CIA exhibits a size distribution with a distinctive cut-off at a specific radius of the dry as well as of the wet particle size distribution. All particles above this limiting size become activated to cloud drops and, thus, are not present in the CIA spectrum. This limiting size was found to be independent of the chemical composition of the particles and only dependent on the prevailing supersaturation. Below this specific size, the CIA spectrum becomes depleted of dry aerosol particles in a manner which does depend on their chemical composition and on the supersaturation in the air. (2) The number of aerosol particles nucleated to cloud drops depends critically on the chemical composition of the particles and on the prevailing supersaturation.     

Phase partitioning of aerosol particles in clouds at Kleiner Feldberg

The partitioning of aerosol particles between cloud droplets and interstitial air by number and volume was determined both in terms of an integral value and as a function of size for clouds on Mt. Kleiner Feldberg (825 m asl), in the Taunus Mountains north-west of Frankfurt am Main, Germany. Differences in the integral values and the size dependent partitioning between two periods during the campaign were observed. Higher number and volume concentrations of aerosol particles in the accumulation mode were observed during Period II compared to Period I. In Period I on average 87±11% (±one standard deviation) and 73±7% of the accumulation mode volume and number were incorporated into cloud droplets. For Period II the corresponding fractions were 42±6% and 12±2% in one cloud event and 64±4% and 18±2% in another cloud event. The size dependent partitioning as a function of time was studied in Period II and found to have little variation. The major processes influencing the partitioning were found to be nucleation scavenging and entrainment.     

Disequilibria between 210Po and 210Pb in surface waters of the southern South China Sea and their implications

Activities of the naturally occurring radionuclides, ²¹⁰Pb and ²¹⁰Po, were measured in both dissolved (<0.45 μm) and particulate (>0.45 μm) phases from surface waters of the southern South China Sea. The average activity of particulate ²¹⁰Pb, 0.23 Bq/m³ (n=23), accounted for about 12% of the total ²¹⁰Pb, which corresponds with values of open oceans. Particulate ²¹⁰Po, with an average activity of 0.43 Bq/m³, accounted for about 40% of the total ²¹⁰Po, which was much higher than those of open and eutrophic oceans. The residence times of total ²¹⁰Po and ²¹⁰Pb in surface waters estimated from an irreversible steady-state model were 0.82 a and 1.16 a, respectively. The consistently high fractionation factor calculated either by scavenging rate constants (5.42) or K_d values (6.69) suggested that a significant fractionation occurred between ²¹⁰Po and ²¹⁰Pb during their removal from solution to particles and that the two radionuclides had different biogeochemical cycling pathways in the oligotrophic South China Sea. Furthermore, our results indicated that there exist different fractionation mechanisms between ²¹⁰Po and ²¹⁰Pb in different marine environments: in eutrophic ocean, plankton detritus and fecal pellets are the main carrier of ²¹⁰Po and ²¹⁰Pb, by which ²¹⁰Po and ²¹⁰Pb have been scavenged and removed; while in oligotrophic ocean, microbes could become the main carrier of ²¹⁰Po and fractionate ²¹⁰Po and ²¹⁰Pb significantly as a result of scarce plankton detritus and fecal pellets. These results suggest the use of ²¹⁰Po to trace marine biogeochemical processes relating to microbial activities and the cycling of sulfur group elements (S, Se, Te and Po).     

Laboratory studies about the interaction of ammonia with ice crystals at temperatures between 0 and −20°C

In laboratory experiments the interactions of ammonia with ice crystals were studied within the temperature range between 0 and −20°C. In a first series of experiments dendritic ice crystals were grown from water vapor in presence of ammonia gas in various concentrations between 4 and 400 ppbv. In a second series of experiments pure ice crystals were exposed to a humidified ammonia–air mixture inside a horizontal flow tube. The influence of temperature, ammonia gas concentration (0.6, 1.5, and 10 ppmv), exposure time, and the presence of impurities such as sulfate on the ammonia uptake by the ice surface was investigated by determining the ammonium content in the melt water of the ice crystals by ion chromatography. During the growth of ice crystals significant amounts of ammonia (around 200 μg/l) were taken up even at small gas concentrations. In contrast, even at high gas concentrations the uptake of ammonia by non-growing ice crystals was lower by approximately one order of magnitude. The presence of sulfate on the ice surface affected an enhanced uptake of ammonia by a factor of 5–10. A model is presented which describes the uptake of ammonia by ice considering the chemical processes occurring in the ice surface layer and simultaneous diffusion of ammonia into bulk ice. Even the increased uptake of ammonia by growing ice is rather small compared to the uptake by water droplets; thus, the major process for scavenging of ammonia from the atmosphere via the ice phase might not be the direct uptake by ice crystals but the riming involving super-cooled droplets containing ammonia.     

Acid Rain and Below-Cloud Scavenging in South-Western China

Major urban areas in south-western China exhibit unique air pollutionproblems due to increasing use of high sulphur-content fuels in an environmentof unfavourable topography and climate. Ambient levels of sulphur dioxideexceed the air quality objectives, and this gas is the major precursor of acidrain. Cloudwater chemistry studies are reported for urban, suburban andcountryside locations, during the period 1985–1989. Although cloudwateracidity was found to increase towards the cloud base, the acidity was muchgreater for rainwater samples collected simultaneously, and was morepronounced in urban rather than neighbouring suburban or countryside regions.The main contribution to the acidity arises from below-cloud scavenging of gasand aerosol and model calculations are able to simulate this behaviour.     

An intercomparison of four wet deposition schemes used in dust transport modeling

The characteristics of four wet deposition schemes widely used in dust modeling studies are examined within the framework of a regional scale dust model. Since these schemes are based on different formulations, the scavenging coefficients of them deviate by a factor of 10³ depending on precipitation rate and particle size. The four schemes coupled with the dust model are applied to simulate a 2002 Asian dust event. The corresponding wet deposition patterns and scavenging efficiencies are compared. It is found that apart from the scheme derived from scavenging coefficient measurements, the other three schemes give similar wet deposition patterns although their scavenging efficiencies are different depending on the particle-size range. The results suggest that the performances of these schemes are affected by the particle size distribution of the dust emission, together with the model's performance of precipitation prediction.     

On the scavenging of gaseous nitrogen compounds by large and small rain drops: II. Wind tunnel and theoretical studies of the simultaneous uptake of NH3, SO2 and CO2 by water drops

An experimental investigation of the simultaneous absorption of NH₃ and SO₂ from the ambient atmosphere by freely falling water drops has been carried out in the Mainz vertical wind tunnel. The experimental results were found to be in good agreement with the results derived from computations with the Kronig-Brink convective diffusion model and also with a model which assumes a drop to be well mixed at all times. Encouraged by this agreement, these computation schemes for the uptake of gas by single drops where incorporated in a pollution washout model with realistic SO₂, NH₃ and CO₂ gas profiles. This model allows an entire raindrop size distribution to fall through a gas layer. The results of this plume-model show that the SO₂ uptake is strongly dependent on the NH₃ concentration in the atmosphere and on the rainrate. We also find that the small drops contribute more towards the washout of these gases. In the case of simultaneous presence of NH₃ and SO₂, desorption of these gases is negligible.     

Feeding ecology of whelks on an intertidal sand flat in north‐eastern New Zealand

The dispersion patterns and feeding behaviour of intertidal whelks were investigated in north‐eastern New Zealand. Aggregations of whelks feeding on clams occurred regularly, with an average of 15–20 individuals per aggregation. Death of clams was attributable to predation in up to 50% of the aggregations, although scavenging of dead and moribund animals was the main activity of whelks. Laboratory and field studies showed that Lepsiella scobina (generally not considered a soft shore species) was the main whelk predator at Lews Bay, Whangateau Harbour, drilling a small neat hole through the clam shell. The distinction between Cominella spp. as predators or scavengers is not so clear. Reseeding of intertidal clams, Austrovenus stutchburyi, has been proposed as a technique for reestablishing populations in some degraded New Zealand estuaries. The impact of whelk predation has many implications for A. stutchburyi reseeding. Both L. scobina and Cominella adspersa may potentially prey on newly reseeded clams as they preferentially attacked small clams in the laboratory. On‐growing to a larger size before reseeding may be advantageous although large size was not found to protect prey from predation. Additionally, no seasonal trend in whelk activity was found.