Phase partitioning of aerosol constituents in cloud based on single-particle and bulk analysis

Gieray, R.; Wieser, P.; Engelhardt, Thomas; Swietlicki, Erik; Hansson, H.‐C.; Mentes, Besim; Orsini, D.; Martinsson, Bengt G.; Svenningsson, Birgitta; Noone, Kevin J.; Heintzenberg, Jost

doi:10.1016/s1352-2310(96)00298-1

Cited by 60 publications

(34 citation statements)

References 29 publications

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“…The same is true for measurements by Coe et al (2006), which were limited by unitary resolution of the mass spectra due to the use of a quadrupole mass spectrometer as analyzer. Gieray et al (1997) did identify methane sulfonate, the neutralized ion of methanesulfonic acid, most likely because they took samples at a remote coastal area and the aerosol had been neutralized by the time it was analyzed. Topping et al (2004) did not identify MSA from their online aerosol mass spectrometric measurements.…”

Section: Discussionmentioning

confidence: 99%

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Characterization of the South Atlantic marine boundary layer aerosol using an aerodyne aerosol mass spectrometer

et al. 2008

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Abstract. Measurements of the submicron fraction of the atmospheric aerosol in the marine boundary layer were performed from January to March 2007 (Southern Hemisphere summer) onboard the French research vessel Marion Dufresne in the Southern Atlantic and Indian Ocean (20 • S-60 • S, 70 • W-60 • E). We used an Aerodyne HighResolution-Time-of-Flight AMS to characterize the chemical composition and to measure species-resolved size distributions of non-refractory aerosol components in the submicron range.Within the "standard" AMS compounds (ammonium, chloride, nitrate, sulfate, organics) "sulfate" is the dominant species in the marine boundary layer with concentrations ranging between 50 ng m −3 and 3 µg m −3 . Furthermore, what is seen as "sulfate" by the AMS is likely comprised mostly of sulfuric acid.Another sulfur containing species that is produced in marine environments is methanesulfonic acid (MSA). There have been previously measurements of MSA using an Aerodyne AMS. However, due to the use of an instrument equipped with a quadrupole detector with unit mass resolution it was not possible to physically separate MSA from other contributions to the same m/z. In order to identify MSA within the HR-ToF-AMS raw data and to extract mass concentrations for MSA from the field measurements the standard high-resolution MSA fragmentation patterns for the measurement conditions during the ship campaign (e.g. vaporizer temperature) needed to be determined.To identify characteristic air masses and their source regions backwards trajectories were used and averaged concentrations for AMS standard compounds were calculated for Correspondence to: S. R. Zorn (zorns@mpch-mainz.mpg.de) each air mass type. Sulfate mass size distributions were measured for these periods showing a distinct difference between oceanic air masses and those from African outflow. While the peak in the mass distribution was roughly at 250 nm (vacuum aerodynamic diameter) in marine air masses, it was shifted to 470 nm in African outflow air. Correlations between the mass concentrations of sulfate, organics and MSA show a narrow correlation for MSA with sulfate/sulfuric acid coming from the ocean, but not with continental sulfate.

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Section: Discussionmentioning

confidence: 99%

“…Gieray et al (1997) used LAMMS (Laser microprobe mass spectrometry) for the analysis of individual aerosol particles collected in marine influenced clouds at Great Dunn Fell (Cumbria, UK). They found not only cloud droplets nucleated on sea salt particles but also cloud droplets formed on sulfate and methane sulfonate containing particles.…”

Section: Introductionmentioning

confidence: 99%

Characterization of the South Atlantic marine boundary layer aerosol using an aerodyne aerosol mass spectrometer

et al. 2008

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“…Sonnblick, Austria [27] Mid altitude (3106 m) 0.45 Rax, Austria [22] Mid altitude (1644 m) 0.54 Great Dun Fell, UK [28] Rural-Coastal 0.57 Jungfraujoch, Switzerland [23] High altitude (3850 m) 0.61 Mt. Sonnblick, Austria [29] High altitude (3106 m) 0.74 Spitzbergen, Norway [30] Arctic 0.80 Mt.…”

Section: Sampling Sitementioning

confidence: 99%

Quantifying Impacts of Aerosol Mixing State on Nucleation-Scavenging of Black Carbon Aerosol Particles

2018

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Abstract:Recent observational studies suggest that nucleation-scavenging is the principal path to removing black carbon-containing aerosol from the atmosphere, thus affecting black carbon's lifetime and radiative forcing. Modeling the process of nucleation-scavenging is challenging, since black carbon (BC) forms complex internal mixtures with other aerosol species. Here, we examined the impacts of black carbon mixing state on nucleation scavenging using the particle-resolved aerosol model PartMC-MOSAIC. This modeling approach has the unique advantage that complex aerosol mixing states can be represented on a per-particle level. For a scenario library that comprised hundreds of diverse aerosol populations, we quantified nucleation-scavenged BC mass fractions. Consistent with measurements, these vary widely, depending on the amount of BC, the amount of coating and coating material, as well as the environmental supersaturation. We quantified the error in the nucleation-scavenged black carbon mass fraction introduced when assuming an internally mixed distribution, and determined its bounds depending on environmental supersaturation and on the aerosol mixing state index χ. For a given χ value, the error decreased at higher supersaturations. For more externally mixed populations (χ < 20%), the nucleation-scavenged BC mass fraction could be overestimated by more than 1000% at supersaturations of 0.1%, while for more internally mixed populations (χ > 75%), the error was below 100% for the range of supersaturations (from 0.02% to 1%) investigated here. Accounting for black carbon mixing state and knowledge of the supersaturation of the environment are crucial when determining the amount of black carbon that can be incorporated into clouds.

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“…They found that sulfate-containing particles were scavenged by cloud droplets three times more efficiently than EC, although they were unable to determine whether this difference was due solely to chemical composition or to differences in the size distribution of the two aerosol species. In a different study in a more remote location, Gieray et al (1997) found that sulfate and soot aerosol had similar scavenging fractions, although sulfate aerosol was still The uncertainties in EC scavenging reported in the literature may be due to the fact that the characteristics of EC particles can change during their lifetime in the atmosphere. Condensation of soluble materials on the surface of EC particles and/or coagulation with soluble particles can increase the hygroscopicity of the EC-containing particles.…”

Section: Aerosol Absorption and Single Scattering Albedomentioning

confidence: 94%

Cloud-Driven Changes in Aerosol Optical Properties - Final Technical Report

Ogren¹,

Sheridan²,

Andrews³

2007

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Abstract:The optical properties of aerosol particles are the controlling factors in determining direct aerosol radiative forcing. These optical properties depend on the chemical composition and size distribution of the aerosol particles, which can change due to various processes during the particles' lifetime in the atmosphere. Over the course of this project we have studied how cloud processing of atmospheric aerosol changes the aerosol optical properties. A counterflow virtual impactor was used to separate cloud drops from interstitial aerosol and parallel aerosol systems were used to measure the optical properties of the interstitial and cloud-scavenged aerosol. Specifically, aerosol light scattering, back-scattering and absorption were measured and used to derive radiatively significant parameters such as aerosol single scattering albedo and backscatter fraction for cloud-scavenged and interstitial aerosol. This data allows us to demonstrate that the radiative properties of cloud-processed aerosol can be quite different than pre-cloud aerosol. These differences can be used to improve the parameterization of aerosol forcing in climate models.

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Phase partitioning of aerosol constituents in cloud based on single-particle and bulk analysis

Cited by 60 publications

References 29 publications

Characterization of the South Atlantic marine boundary layer aerosol using an aerodyne aerosol mass spectrometer

Characterization of the South Atlantic marine boundary layer aerosol using an aerodyne aerosol mass spectrometer

Quantifying Impacts of Aerosol Mixing State on Nucleation-Scavenging of Black Carbon Aerosol Particles

Cloud-Driven Changes in Aerosol Optical Properties - Final Technical Report

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