A general circulation model based calculation of HCl and ClNO<sub>2</sub> production from sea salt dechlorination: Reactive Chlorine Emissions Inventory

Erickson, D. J.; Seuzaret, Christophe; Keene, W. C.; Gong, S. L.

doi:10.1029/98jd01384

Cited by 119 publications

(147 citation statements)

References 62 publications

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“…Since Br activation is relatively insensitive to pH variability in acidic aerosol, small to negligible influences are expected in polluted regions (such as the western North Atlantic Ocean) where most sea-salt aerosols are currently acidified within seconds to minutes anyway (e.g. Erickson et al, 1999). However, in more remote regions such as the high latitude southern oceans where Br activation may be limited by available acidity (e.g.…”

Section: Future Projectionsmentioning

confidence: 99%

“…Since sea-salt aerosol production strongly depends on wind speed (Gong et al, 2002(Gong et al, , 1997, and references therein), temporal variability in wind fields leads to large changes in sea-salt aerosol concentrations (e.g. Erickson et al, 1999). Finally, the relative amounts of sea salt and of acids and bases (both natural and anthropogenic) in the multiphase system vary as functions of proximity to and strengths of their respective upwind sources.…”

Section: Aerosol Measurementsmentioning

confidence: 99%

“…Increased wind velocities lead to increased production fluxes of sea-salt aerosols and associated alkalinity, higher concentrations of atmospheric sea salt, increased mean sea-salt sizes and total aerosol surface areas (but decreased mean surface/volume ratio), decreased sea-salt lifetimes, decreased rates of gaseous uptake and loss from individual particles, and increased overall scavenging and deposition of acids (e.g. Woodcock, 1953;Erickson et al, 1999). It is evident from the above discussion that all of these effects will influence the rate and degree of aerosol acidification and associated debromination.…”

Section: Correlation To Sea-salt Concentrationmentioning

confidence: 99%

“…Chemical interactions of this mixture together with ambient relative humidity control aerosol pH (Keene Table 1. Concentrations of selected elements in sea water at 3.5% salinity (Wilson, 1975) and Savoie, 1998Savoie, , 1999Erickson et al, 1999;Keene et al, 2002) and related pH-dependent processes involving particulate Br (e.g. Ayers et al, 1999).…”

Section: Aerosol Measurementsmentioning

confidence: 99%

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Inorganic bromine in the marine boundary layer: a critical review

et al. 2003

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Abstract. The cycling of inorganic bromine in the marine boundary layer (mbl) has received increased attention in recent years. Bromide, a constituent of sea water, is injected into the atmosphere in association with sea-salt aerosol by breaking waves on the ocean surface. Measurements reveal that supermicrometer sea-salt aerosol is substantially depleted in bromine (often exceeding 50%) relative to conservative tracers, whereas marine submicrometer aerosol is often enriched in bromine. Model calculations, laboratory studies, and field observations strongly suggest that the supermicrometer depletions reflect the chemical transformation of particulate bromide to reactive inorganic gases that influence the processing of ozone and other important constituents of marine air. Mechanisms for the submicrometer enrichments are not well understood. Currently available techniques cannot reliably quantify many Br-containing compounds at ambient concentrations and, consequently, our understanding of inorganic Br cycling over the oceans and its global significance are uncertain. To provide a more coherCorrespondence to: R. Sander (sander@mpch-mainz.mpg.de) ent framework for future research, we have reviewed measurements in marine aerosol, the gas phase, and in rain. We also summarize sources and sinks, as well as model and laboratory studies of chemical transformations. The focus is on inorganic bromine over the open oceans outside the polar regions. The generation of sea-salt aerosol at the ocean surface is the major tropospheric source producing about 6.2 Tg/a of bromide. The transport of Br from continents (as mineral aerosol, and as products from biomass-burning and fossil-fuel combustion) can be of local importance. Transport of degradation products of long-lived Br-containing compounds from the stratosphere and other sources contribute lesser amounts. Available evidence suggests that, following aerosol acidification, sea-salt bromide reacts to form Br 2 and BrCl that volatilize to the gas phase and photolyze in daylight to produce atomic Br and Cl. Subsequent transformations can destroy tropospheric ozone, oxidize dimethylsulfide (DMS) and hydrocarbons in the gas phase and S(IV) in aerosol solutions, and thereby potentially influence climate. Inorganic bromine in the mbl gas phase during daytime are consistent with expectations based on photochemistry. We expect that the importance of inorganic Br cycling will vary in the future as a function of both increasing acidification of the atmosphere (through anthropogenic emissions) and climate changes. The latter affects bromine cycling via meteorological factors including global wind fields (and the associated production of sea-salt aerosol), temperature, and relative humidity.

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Section: Future Projectionsmentioning

confidence: 99%

Section: Aerosol Measurementsmentioning

confidence: 99%

Section: Correlation To Sea-salt Concentrationmentioning

confidence: 99%

Section: Aerosol Measurementsmentioning

confidence: 99%

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Inorganic bromine in the marine boundary layer: a critical review

et al. 2003

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“…Surface total HNO 3 and NH 3 mixing ratios (over the gas and particle phase) are at most 10 ppb in polluted regions and typically around 1 ppb or less over remote oceans (Adams et al, 1999). Gas-phase HCl ranges typically from 0.001 to 0.1 ppb over the Southern Hemisphere oceans (Erickson III et al, 1999), and is less than 10 ppb under polluted continental conditions (e.g., Eldering et al, 1991;Nemitz et al, 2004). The concentration ranges for HCl, NH 3 , and HNO 3 were not primarily chosen as being representative of any particular region or environment but rather with numerical stability testing considerations in mind.…”

Section: Evaluation In the Equilibrium Operationmentioning

confidence: 99%

Size-resolved simulations of the aerosol inorganic composition with the new hybrid dissolution solver HyDiS-1.0: description, evaluation and first global modelling results

et al. 2016

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Abstract. The dissolution of semi-volatile inorganic gases such as ammonia and nitric acid into the aerosol aqueous phase has an important influence on the composition, hygroscopic properties, and size distribution of atmospheric aerosol particles. The representation of dissolution in global models is challenging due to inherent issues of numerical stability and computational expense. For this reason, simplified approaches are often taken, with many models treating dissolution as an equilibrium process. In this paper we describe the new dissolution solver HyDiS-1.0, which was developed for the global size-resolved simulation of aerosol inorganic composition. The solver applies a hybrid approach, which allows for some particle size classes to establish instantaneous gas-particle equilibrium, whereas others are treated time dependently (or dynamically). Numerical accuracy at a competitive computational expense is achieved by using several tailored numerical formalisms and decision criteria, such as for the time-and size-dependent choice between the equilibrium and dynamic approaches. The new hybrid solver is shown to have numerical stability across a wide range of numerical stiffness conditions encountered within the atmosphere. For ammonia and nitric acid, HyDiS-1.0 is found to be in excellent agreement with a fully dynamic benchmark solver. In the presence of sea salt aerosol, a somewhat larger bias is found under highly polluted conditions if hydrochloric acid is represented as a third semi-volatile species. We present first results of the solver's implementation into a global aerosol microphysics and chemistry transport model. We find that (1) the new solver predicts surface concentrations of nitrate and ammonium in reasonable agreement with observations over Europe, the USA, and East Asia, (2) models that assume gas-particle equilibrium will not capture the partitioning of nitric acid and ammonia into Aitken-mode-sized particles, and thus may be missing an important pathway through which secondary particles may grow to radiation-and cloudinteracting size, and (3) the new hybrid solver's computational expense is modest, at around 10 % of total computation time in these simulations.

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Seasonally resolved ice core records from West Antarctica indicate a sea ice source of sea‐salt aerosol and a biomass burning source of ammonium

et al. 2014

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The sources and transport pathways of aerosol species in Antarctica remain uncertain, partly due to limited seasonally resolved data from the harsh environment. Here, we examine the seasonal cycles of major ions in three high-accumulation West Antarctic ice cores for new information regarding the origin of aerosol species. A new method for continuous acidity measurement in ice cores is exploited to provide a comprehensive, charge-balance approach to assessing the major non-sea-salt (nss) species. The average nss-anion composition is 41% sulfate (SO 4 2À ), 36% nitrate (NO 3 À ), 15% excess-chloride (ExCl À ), and 8% methanesulfonic acid (MSA). Approximately 2% of the acid-anion content is neutralized by ammonium (NH 4 + ), and the remainder is balanced by the acidity (Acy ≈ H + À HCO 3 À ). The annual cycle of NO 3 À shows a primary peak in summer and a secondary peak in late winter/spring that are consistent with previous air and snow studies in Antarctica. The origin of these peaks remains uncertain, however, and is an area of active research. A high correlation between NH 4 + and black carbon (BC) suggests that a major source of NH 4 + is midlatitude biomass burning rather than marine biomass decay, as previously assumed. The annual peak in excess chloride (ExCl À ) coincides with the late-winter maximum in sea ice extent. Wintertime ExCl À is correlated with offshore sea ice concentrations and inversely correlated with temperature from nearby Byrd station. These observations suggest that the winter peak in ExCl À is an expression of fractionated sea-salt aerosol and that sea ice is therefore a major source of sea-salt aerosol in the region.

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A general circulation model based calculation of HCl and ClNO₂ production from sea salt dechlorination: Reactive Chlorine Emissions Inventory

Cited by 119 publications

References 62 publications

Inorganic bromine in the marine boundary layer: a critical review

Inorganic bromine in the marine boundary layer: a critical review

Size-resolved simulations of the aerosol inorganic composition with the new hybrid dissolution solver HyDiS-1.0: description, evaluation and first global modelling results

Seasonally resolved ice core records from West Antarctica indicate a sea ice source of sea‐salt aerosol and a biomass burning source of ammonium

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A general circulation model based calculation of HCl and ClNO2 production from sea salt dechlorination: Reactive Chlorine Emissions Inventory

Cited by 119 publications

References 62 publications

Inorganic bromine in the marine boundary layer: a critical review

Inorganic bromine in the marine boundary layer: a critical review

Size-resolved simulations of the aerosol inorganic composition with the new hybrid dissolution solver HyDiS-1.0: description, evaluation and first global modelling results

Seasonally resolved ice core records from West Antarctica indicate a sea ice source of sea‐salt aerosol and a biomass burning source of ammonium

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A general circulation model based calculation of HCl and ClNO₂ production from sea salt dechlorination: Reactive Chlorine Emissions Inventory