Chemical analysis of refractory stratospheric aerosol particles collected
within the arctic vortex and inside polar stratospheric clouds

Ebert, Martin; Weigel, Ralf; Kandler, Konrad; Günther, G.; Molleker, Sergej; Grooß, Jens‐Uwe; Vogel, Bärbel; Weinbruch, Stephan; Borrmann, Stephan

doi:10.5194/acp-16-8405-2016

Cited by 37 publications

(49 citation statements)

References 74 publications

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“…We are aware of the fact that the stratospheric aerosol layer also contains organics and inclusions of meteoritic dust (Ebert et al, 2016) and, after volcanic events, also co-exists with volcanic ash (e.g. Pueschel et al, 1994.…”

Section: Modelling Stratospheric Aerosol: Overview and Challengesmentioning

confidence: 99%

The Interactive Stratospheric Aerosol Model Intercomparison Project (ISA-MIP): motivation and experimental design

et al. 2018

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Abstract. The Stratospheric Sulfur and its Role in Climate (SSiRC) Interactive Stratospheric Aerosol Model Intercomparison Project (ISA-MIP) explores uncertainties in the processes that connect volcanic emission of sulfur gas species and the radiative forcing associated with the resulting enhancement of the stratospheric aerosol layer. The central aim of ISA-MIP is to constrain and improve interactive stratospheric aerosol models and reduce uncertainties in the stratospheric aerosol forcing by comparing results of standardized model experiments with a range of observations. In this paper we present four co-ordinated inter-model experiments designed to investigate key processes which influence the formation and temporal development of stratospheric aerosol in different time periods of the observational record. The Background (BG) experiment will focus on microphysics and transport processes under volcanically quiescent conditions, when the stratospheric aerosol is controlled by the transport of aerosols and their precursors from the troposphere to the stratosphere. The Transient Aerosol Record (TAR) experiment will explore the role of small-to moderate-magnitude volcanic eruptions, anthropogenic sulfur emissions, and transport processes over the period 1998-2012 and their role in the warming hiatus. Two further experiments will investigate the stratospheric sulfate aerosol evolution after major volcanic eruptions. The Historical Eruptions SO 2 Emission Assessment (HErSEA) experiment will focus on the uncertainty in the initial emission of recent large-magnitude volcanic eruptions, while the Pinatubo Em-

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Section: Modelling Stratospheric Aerosol: Overview and Challengesmentioning

confidence: 99%

The Interactive Stratospheric Aerosol Model Intercomparison Project (ISA-MIP): motivation and experimental design

et al. 2018

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“…There are, however, several previous publications which describe the presence of a variety of other refractory particle groups in addition to carbonaceous particles. These additional particle groups include metallic particles (Chuan and Woods, 1984;Sheridan et al, 1994;Chen et al, 1998;Baumgardner et al, 2004;Ebert et al, 2016), meteoritic particles (Murphy et al, 1998(Murphy et al, , 2007Renard et al, 2008, silicates (Testa et al, 1990;Ebert et al, 2016), crustal-type particles (Sheridan et al, 1994;Chen et al, 1998), and Ca-bearing particles (Della Corte et al, 2013;Ebert et al, 2016).…”

Section: Occurrence Of Refractory Carbonaceous Particles In the Stratmentioning

confidence: 99%

“…As most of the particles analyzed show no or only very little ordering, it is assumed that the particles did not change their nanostructure during their atmospheric lifetime. On the other hand, several electron microscopy studies describe soot particles in the stratosphere (Pueschel et al, 1992(Pueschel et al, , 1997Sheridan et al, 1994;Strawa et al, 1999;Ebert et al, 2016). Thus, it can be expected that soot particlesonce injected into the stratosphere -do not change their typical nanostructure under stratospheric conditions.…”

Section: Potential Sourcesmentioning

confidence: 99%

Sub-micrometer refractory carbonaceous particles in the polar stratosphere

et al. 2017

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Abstract. Eleven particle samples collected in the polar stratosphere during SOLVE (SAGE III Ozone loss and validation experiment) from January until March 2000 were characterized in detail by high-resolution transmission and scanning electron microscopy (TEM/SEM) combined with energy-dispersive X-ray microanalysis. A total of 4202 particles (TEM = 3872; SEM = 330) were analyzed from these samples, which were collected mostly inside the polar vortex in the altitude range between 17.3 and 19.9 km. Particles that were volatile in the microscope beams contained ammonium sulfates and hydrogen sulfates and dominated the samples. Some particles with diameters ranging from 20 to 830 nm were refractory in the electron beams. Carbonaceous particles containing additional elements to C and O comprised from 72 to 100 % of the refractory particles. The rest were internal mixtures of these materials with sulfates. The median number mixing ratio of the refractory particles, expressed in units of particles per milligram of air, was 1.1 (mg air) −1 and varied between 0.65 and 2.3 (mg air) −1 .Most of the refractory carbonaceous particles are completely amorphous, a few of the particles are partly ordered with a graphene sheet separation distance of 0.37 ± 0.06 nm (mean value ± standard deviation). Carbon and oxygen are the only detected major elements with an atomic O/C ratio of 0.11 ± 0.07. Minor elements observed include Si, S, Fe, Cr and Ni with the following atomic ratios relative to C: Si/C: 0.010 ± 0.011; S/C: 0.0007 ± 0.0015; Fe/C: 0.0052 ± 0.0074; Cr/C: 0.0012 ± 0.0017; Ni/C: 0.0006 ± 0.0011 (all mean values ± standard deviation).High-resolution element distribution images reveal that the minor elements are distributed within the carbonaceous matrix; i.e., heterogeneous inclusions are not observed. No difference in size, nanostructure and elemental composition was found between particles collected inside and outside the polar vortex.Based on chemistry and nanostructure, aircraft exhaust, volcanic emissions and biomass burning can certainly be excluded as sources. The same is true for the less probable but globally important sources: wood burning, coal burning, diesel engines and ship emissions.Recondensed organic matter and extraterrestrial particles, potentially originating from ablation and fragmentation, remain as possible sources of the refractory carbonaceous particles studied. However, additional work is required in order to identify the sources unequivocally.

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“…The dilution unit is build up by two valves to control the air 10 stream in and out of the system, making it possible to send air through two filters to dilute the incoming aerosol flow. Particles where sampled by the use of multi MINI cascade impactors with the same design as described in Ebert et al (2016) and Schütze et al (2017), but with the use of only one stage with a lower 50% cut-off diameter of approximately 0.1 µm (aerodynamic).…”

mentioning

confidence: 99%

“…The IPRs were collected on boron substrates to allow 15 detection of light elements including carbon (Choël et al, 2005;Ebert et al, 2016). Atmos.…”

mentioning

confidence: 99%

Composition of ice particle residuals in mixed phase clouds at Jungfraujoch (Switzerland): Enrichment and depletion of particle groups relative to total aerosol

Hammer¹,

Mertes²,

Schneider³

et al. 2018

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Ice particle residuals (IPRs) and the total aerosol particle population were sampled in parallel during mixed phase cloud events at the high altitude research station Jungfraujoch in January/February 2017. Particles were sampled on boron substrates by use of multi MINI cascade impactors operated behind an ice selective counterflow impactor (Ice-CVI) for IPRs and a heated total inlet for the total aerosol particles. Total aerosol samples were collected with a dilution setup to match the much longer 5 sampling time behind the Ice-CVI. About 4000 particles from ten Ice-CVI samples (from seven days of cloud events at temperatures between -10 °C and -18°C) were analysed and classified with operator controlled scanning electron microscopy.Contamination particles (identified by their chemical composition) most likely originating from abrasion in the Ice-CVI and collection of secondary ice, were excluded from the further analysis. Approximately 3000 total aerosol particles from five days in clouds were also analysed. Enrichment and depletion of the different particle groups (within the IPR fraction relative to total 10 aerosol reservoir) are presented as odds ratio relative to alumosilicate (particles only consisting of Al, Si and O), which was chosen as reference due to the large enrichment of this group relative to total aerosol and the relatively high number concentration of this group in both total aerosol and the IPR samples. Complex secondary particles and soot are the major particle groups in the total aerosol samples, but are not found in the IPR fraction and are hence strongly depleted. C-rich particles (most likely organic particles) showed a smaller enrichment compared to alumosilicates by a factor of ~20. The 15 particle groups with similar enrichment as alumosilicate are silica, Fe-alumosilicates, Ca-rich, Ca-sulphates, sea salt and metal/ metal oxide. Other-alumosilicates -consisting of variable amounts of Na, K, Ca, Si, Al, O, Ti and Fe-are somewhat more (factor ~2) and Pb-rich more (factor ~8) enriched than alumosilicates. None of the sampled IPR groups showed a temperature or size dependence in respect to ice activity, which might be due to the limited sampling temperature interval and the similar size of the particles. Footprint plots and wind roses could explain the different total aerosol composition in one sample 20 (carbonaceous particle emission from the urban/industrial area of Po Valley), but this did not affect the IPR composition. Taken into account the relative abundance of the particle groups in total aerosol and the ice nucleation ability, we found that silica, alumosilicates and other-alumosilicates were the most important ice particle residuals at Jungfraujoch during the mixed phase cloud events in winter 2017. 30Atmos. Chem. Phys. Discuss., https://doi

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Chemical analysis of refractory stratospheric aerosol particles collected within the arctic vortex and inside polar stratospheric clouds

Cited by 37 publications

References 74 publications

The Interactive Stratospheric Aerosol Model Intercomparison Project (ISA-MIP): motivation and experimental design

The Interactive Stratospheric Aerosol Model Intercomparison Project (ISA-MIP): motivation and experimental design

Sub-micrometer refractory carbonaceous particles in the polar stratosphere

Composition of ice particle residuals in mixed phase clouds at Jungfraujoch (Switzerland): Enrichment and depletion of particle groups relative to total aerosol

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