| 1. |
- Flynn, Michael J., et al.
(författare)
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Modelling cloud processing of aerosol during the ACE-2 HILLCLOUD experiment
- 2000
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Ingår i: Tellus. Series B: Chemical and Physical Meteorology. - : Stockholm University Press. - 0280-6509. ; 52:2, s. 779-800
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Tidskriftsartikel (refereegranskat)abstract
- A numerical model has been used to simulate the conditions observed during the ACE-2 Hillcloud experiment and to study the processes which may be taking place. The model incorporates gas phase chemistry of sulphur and nitrogen compounds upstream of the cloud, and the interaction of aerosol, precursor trace gases and oxidants within the cloud. Gas phase and aerosol inputs to the model have been provided from measurements made in the field. Dynamics of the air flow over the hill consisted of simple prescribed dynamics based on wind speed measurements, and also for some cases modelled dynamics. In this modelling study, it was found that during clean case studies particles down to 40-55 nm diameter were activated to form cloud droplets, the total number of droplets formed ranging from 200 to 400 drops/cm3. Significant modification of the aerosol spectra due to cloud processing was observed. In polluted cases particles down to 65-80 nm diameter were activated to form cloud droplets, the total number of droplets ranging from 800 to 2800 drops/cm3. Modification of the aerosol spectra due to cloud processing was slight. In all cases, changes in the aerosol spectra were due to both the uptake of HNO3, HCl, NH3 and SO2 from the gas phase, (the SO2 being oxidised to sulphate) and the repartitioning of species such as HNO3, HCl, and NH3 from larger particles onto smaller ones. Modelling results have been compared with observations made. Modelled droplet numbers are typically within 20% of the best measured values. The mode of the droplet distribution typically around 10-20 μm for clean cases and 4-8 μm for polluted cases was found to be in good agreement with the measured values of 10-25 μm for clean cases, but not in such good agreement for polluted cases. Measurements of upwind and interstitial aerosol distributions showed that the smallest particles activated were 30 and 50 nm for clean and polluted cases respectively, slightly smaller than the model values quoted above. Measured upwind and downwind aerosol spectra showed similar modification to that predicted by the model in eight out of the eleven model runs carried out. Chemistry measurements also give general evidence for both the uptake of species from the gas phase, and repartitioning of species from large particles onto smaller ones, though comparisons for individual cases are more difficult. From this modelling study, it can be concluded that in general, in the remote environment the exchange of hydrochloric acid, nitric acid and ammonia between aerosol particles and take up from the gas phase in the vicinity of cloud may be a very important mechanism in regulating the evolution of the aerosol spectrum. Further, the much more linear relationship between cloud droplet and accumulation mode aerosol number, which was observed in the measurements made during the ACE-2 HILLCLOUD project is supported by these modelling results. The implications of this for the indirect effect will be explored in future work.
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| 2. |
- Fuzzi, Sandro, et al.
(författare)
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Overview of the Po valley fog experiment 1994 (CHEMDROP)
- 1998
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Ingår i: Contributions to Atmospheric Physics. - 0005-8173. ; 71:1, s. 3-19
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Forskningsöversikt (refereegranskat)abstract
- The paper presents an outline of the CHEMDROP field experiment, carried out in November 1994 at the field station of S. Pietro Capofiume in the Po Valley, Italy. The main objective of the project was to address the issue of the size-dependent chemical composition of fog droplets, by experimentally investigating the following processes, which are expected to affect (or be affected by) the chemical composition of fog droplets as a function of size: a) the connection of the size-dependent chemical composition of CCN to the size-dependent composition of fog droplets; b) the gas/liquid partitioning of the gaseous species NH3, SO2, HCHO, HNO3 in fog; c) the Fe(II)/Fe(III) redox cycle in fog water. Some general results and overall conclusions of the experiment are reported in this paper, while more specific scientific questions are discussed in other companion papers in this issue. CHEMDROP results show that several processes concur in determining the size-dependence of fog droplets chemical composition: nucleation scavenging of pre-existing CCN, fog dynamical evolution and gas/liquid exchange between interstitial air and fog droplets. Chemical transformations in the liquid phase can cause further changes in the chemical composition of the droplets. Only by taking into account the combination of all these processes, is it possible to explain the inhomogeneities in fog droplet chemical composition.
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| 3. |
- Laj, Paolo, et al.
(författare)
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The size dependent composition of fog droplets
- 1998
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Ingår i: Contributions to Atmospheric Physics. - 0005-8173. ; 71:1, s. 115-130
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Tidskriftsartikel (refereegranskat)abstract
- The size dependency of fog droplet concentration and composition was studied using newly developed droplet impactors during the CHEMDROP campaign in the Po Valley (Italy). A strong size dependency of solute concentrations was measured during several fog episodes. The ionic strength of the droplet solutions varies as a function of droplet diameter, showing maximum values in the 9-19 μm diameter range. The solute concentration varies up to a factor of 10 among droplets of different diameter. Similarly, differences of up to 2 pH units are found among droplets of different diameter. The solute dependency of aerosol and droplets species from 0.1 μm to 50 μm is investigated. The monomodal behaviour of the solute concentration in droplets can be explained by both diffusional condensation of the aerosols serving as cloud condensation nuclei (CCN) and the air/liquid transfer of volatile species, in particular for HNO3 and NH3. The distribution of sulphur species is also size-dependent and is directly linked to the pH variations across the droplet spectrum, resulting in HMSA formation in small droplets and S(IV) oxidation large droplets.
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| 4. |
- Wendish, Manfred, et al.
(författare)
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Drop size distribution and LWC in Po valley fog
- 1998
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Ingår i: Contributions to Atmospheric Physics. - 0005-8173. ; 71:1, s. 87-100
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Tidskriftsartikel (refereegranskat)abstract
- In this paper results are presented of ground-based fog microphysical measurements obtained during the CHEMDROP experiment in the Po Valley (Northern Italy) in November 1994. Altogether about 85 hours of drop microphysical data are analyzed. At the beginning of the experiment a comparison of some of the different microphysical instruments, operated during the experiment, was performed. It has revealed some differences between the Liquid Water Content LWC measured by Particle Volume Monitors (PVMs), and by several Forward Scattering Spectrometer Probes (FSSPs). Possible explanations for the discrepancies are discussed. The FSSP derived drop size distributions (number and mass) were parameterized in terms of log-normal distributions. The statistical analysis of the fittings has shown that the overwhelming majority of the drop mass size distributions was characterized by a bimodal shape. The most frequent values of the mode parameters (median diameter, geometric standard deviation) are given in Table 3 of this paper. An investigation of the temporal evolution of the drop size distribution revealed two typical phases of fog formation. In the first step both modes of the drop mass size distribution increase more or less uniform, whereas in the second phase the large drop mode drastically rises. Furthermore, the second phase is characterized by quasi-periodic oscillations in nearly all mode parameters of the drop size distribution with a period between ten and 15 minutes. In the last part of the paper the frequent occurrence of drizzle within the fog was studied by comparing the measurements with respective model calculations.
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| 5. |
- Yuskiewicz, Brett A., et al.
(författare)
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Changes in submicrometer particle distributions and light scattering during haze and fog events in a highly polluted environment
- 1998
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Ingår i: Contributions to Atmospheric Physics. - 0005-8173. ; 71:1, s. 33-45
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Tidskriftsartikel (refereegranskat)abstract
- The changes in submicrometer atmospheric particle size distributions measured with a Differential Mobility Particle Sizer (DMPS) system during a polluted fog experiment during November, 1994 are presented in this study. Results reveal three modes commonly evident in the size distribution (3 < DN < 843 nm) measurements; the ultrafine, Aitken and accumulation with respective geometric diameters, (Dgn), of 17, 110 and 400 nm. An additional mode, appears between the ultrafine and Aitken modes (Dgn = 52 nm) in approximately one quarter of the measurements and is linked to several industrial cities upwind of the measurement site. A stabile ultrafine mode appears consistently (84% of measurements) at 16-17 nm throughout the campaign, suggestive of a source, such as a highway in the near vicinity. During fog and haze periods number concentrations for particles less than 25 nm and greater than 400 nm decrease by 78 and 95%, respectively. These changes do not affect the aerosol scattering efficiency significantly. The overall aerosol mass scattering efficiency determined for the Po Valley region is 4.3 ± 0.6 m2 g-1. Closure is achieved for light extinction predicted from droplet distributions and measured with a transmissiometer in 37 of 39 cases during fog periods. Measured and calculated light extinction, bext, covary strongly with an R2 of 0.92.
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