Cloud processing of soluble gases

Laj, Paolo; Fuzzi, S.; Facchini, M. C.; Lind, John A.; Orsi, G.; Preiss, M.; Maser, R.; Jaeschke, W.; Seyffer, E.; Helas, G.; Acker, K.; Wieprecht, W.; Möller, Detlev; Arends, B. G.; Möls, J.J.; Colvile, R. N.; Gallagher, Martin; Beswick, K.M.; Hargreaves, K. J.; Storeton-West, Robert; Sutton, Mark A.

doi:10.1016/s1352-2310(97)00040-x

Cited by 63 publications

(30 citation statements)

References 24 publications

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“…1, a consistent fraction of cloud samples have consistent solute concentrations between 18 and 50 mg l −1 . These concentrations are slightly lower than ionic concentrations measured at mountain sites under the influence of medium range pollution, such as Great Dun Fell (23 mg l −1 just for sulphate, Laj et al, 1997b), Aubure in the Vosges Mountains (eastern France; 66 mg l −1 measured by , Whiteface Mountain (60 mg l −1 Khwaja et al, 1995) and the eastern part of United States (Weathers al., 1988). This also corresponds to the range of concentrations found during the CIME campaign, and to levels measured by Voisin et al (2000) at PDD.…”

Section: Inorganic Substancesmentioning

confidence: 74%

Cloud chemistry at the Puy de Dôme: variability and relationships with environmental factors

et al. 2004

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Abstract. The chemical composition of cloud water was investigated during the winter-spring months of 2001 and 2002 at the Puy de Dôme station (1465 m above sea level, 45 • 46 22 N, 2 • 57 43 E) in an effort to characterize clouds in the continental free troposphere. Cloud droplets were sampled with single-stage cloud collectors (cut-off diameter approximately 7 µm) and analyzed for inorganic and organic ions, as well as total dissolved organic carbon. Results show a very large variability in chemical composition and total solute concentration of cloud droplets, ranging from a few mg l −1 to more than 150 mg l −1 . Samplings can be classified in three different categories with respect to their total ionic content and relative chemical composition: background continental (BG, total solute content lower than 18 mg l −1 ), anthropogenic continental (ANT, total solute content from 18 to 50 mg l −1 ), and special events (SpE, total solute content higher than 50 mg l −1 ). The relative chemical composition shows an increase in anthropogenic-derived species (NO We observed a high contribution of solute in cloud water derived from the dissolution of gas phase species in all cloud events. This was evident from large solute fractions of nitrate, ammonium and mono-carboxylic acids in cloud water, relative to their abundance in the aerosol phase. The comparison between droplet and aerosol composition clearly shows the limited ability of organic aerosols to act as cloud condensation nuclei. The strong contribution of gas-phase species limits the establishment of direct relationships between cloud water solute concentration and LWC that are expected from nucleation scavenging.

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Section: Inorganic Substancesmentioning

confidence: 74%

Cloud chemistry at the Puy de Dôme: variability and relationships with environmental factors

et al. 2004

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“…Numerous studies have investigated gas/liquid phase partitioning in clouds and fogs, with nearly all showing significant discrepancies, both supersaturation and subsaturation, between measured aqueous concentrations and expected concentrations based on Henry's law equilibrium with the gas phase (Acker et al, 2008;Moore et al, 2004b;Sellegri et al, 2003;Jaeschke et al, 1998;Laj et al, 1997;Winiwarter et al, 1994;Facchini et al, 1992a;1992b;Winiwarter et al, 1992;Pandis and Seinfeld, 1991;Winiwarter et al, 1988;Jacob et al, 1986). These studies have shown that deviations from equilibrium can result from mixing of droplets that are individually in equilibrium with the gas phase, variations in liquid water content over the course of the sampling period, mass transfer limitations, or some combination of these phenomena.…”

Section: Charge Balancementioning

confidence: 99%

Radiation fog chemical composition and its temporal trend over an eight year period

Straub

2017

Atmospheric Environment

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Radiation fog samples have been collected at a rural site in Central Pennsylvania from 2007 through 2015 in order to document chemical composition, assess concentration changes over time, and to provide insight into emission sources that influence the region. The collection of samples over multiple years makes this one of the few long duration radiation fog studies that have been completed.During the course of the campaign, 146 samples were obtained and analyzed for pH, major inorganic ions, low molecular weight organic acids, total organic carbon (TOC) and total nitrogen (TN).Ammonium (median concentration = 209 µN), sulfate (69 µN), calcium (51 µN), and nitrate (31 µN) were the most abundant inorganic ions, although these were present at much lower concentrations than for radiation fog studies conducted in other locations. Organic acids, of which formate (20 µM) and acetate (21 µM) were the most abundant, were closer in magnitude to measurements made during previous studies. Organic acids accounted for 15% of TOC, which had a median concentration of 6.6 mgC l -1 . The median concentration of TN was 3.6 mgN l -1 , 18% of which was determined to be organic nitrogen.Statistically significant decreasing trends from 2007 to 2015 were noted for sulfate, ammonium, chloride, and nitrate. For the same period, an increase in pH was observed. Seasonal trends were identified for a number of species as well. The partitioning of ammonia between the gas and aqueous phases was also investigated and found to deviate significantly from equilibrium.

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“…Mass is added to aerosols as they pass through clouds by a variety of processes, summarised in Table 1 along with abbreviations that will be used throughout this paper. The uptake of gas-phase species (DISS) such as H 2 SO 4 , HCl, HNO 3 and ammonia can contribute the majority of in-cloud mass gain in some conditions (Flynn et al, 2000), but the aqueous oxidation of SO 2 to sulfate in cloud droplets (AQOX) is generally considered to be the most important in-cloud mass production pathway (Bradbury et al, 1999;Laj et al, 1997a, b;Mertes et al, 2005a). SO 2 is oxidised to sulfate in the aqueous phase by O 3 , H 2 O 2 and transition metal-catalysed oxidation by O 2 (Sander et al, 1995;Bower et al, 1997).…”

Section: E Harris Et Al: Cloud Processing During Hcct-2010mentioning

confidence: 99%

In-cloud sulfate addition to single particles resolved with sulfur isotope analysis during HCCT-2010

et al. 2014

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Abstract. In-cloud production of sulfate modifies aerosol size distribution, with important implications for the magnitude of indirect and direct aerosol cooling and the impact of SO 2 emissions on the environment. We investigate which sulfate sources dominate the in-cloud addition of sulfate to different particle classes as an air parcel passes through an orographic cloud. Sulfate aerosol, SO 2 and H 2 SO 4 were collected upwind, in-cloud and downwind of an orographic cloud for three cloud measurement events during the Hill Cap Cloud Thuringia campaign in autumn 2010 (HCCT-2010). Combined SEM and NanoSIMS analysis of single particles allowed the δ 34 S of particulate sulfate to be resolved for particle size and type.The most important in-cloud SO 2 oxidation pathway at HCCT-2010 was aqueous oxidation catalysed by transition metal ions (TMI catalysis), which was shown with single particle isotope analyses to occur primarily in cloud droplets nucleated on coarse mineral dust. In contrast, direct uptake of H 2 SO 4 (g) and ultrafine particulate were the most important sources modifying fine mineral dust, increasing its hygroscopicity and facilitating activation. Sulfate addition to "mixed" particles (secondary organic and inorganic aerosol) and coated soot was dominated by in-cloud aqueous SO 2 oxidation by H 2 O 2 and direct uptake of H 2 SO 4 (g) and ultrafine particle sulfate, depending on particle size mode and time of day. These results provide new insight into in-cloud sulfate production mechanisms, and show the importance of single particle measurements and models to accurately assess the environmental effects of cloud processing.

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Cloud processing of soluble gases

Cited by 63 publications

References 24 publications

Cloud chemistry at the Puy de Dôme: variability and relationships with environmental factors

Cloud chemistry at the Puy de Dôme: variability and relationships with environmental factors

Radiation fog chemical composition and its temporal trend over an eight year period

In-cloud sulfate addition to single particles resolved with sulfur isotope analysis during HCCT-2010

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