Chemical composition of radiolytically formed particles using single-particle mass spectrometry

Wonaschuetz, Anna; Kallinger, Peter; Szymanski, Wladyslaw W.; Hitzenberger, R.

doi:10.1016/j.jaerosci.2017.07.012

Cited by 9 publications

(5 citation statements)

References 20 publications

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“…4d) representing fragments of nitrogen-containing organic compounds. These markers have been attributed to compounds of biological origin (Pratt et al, 2009;Cahill et al, 2012;Creamean et al, 2013), although other studies have found these markers in aerosol where biological components were not expected (Sodeman et al, 2005;Zawadowicz et al, 2017;Wonaschuetz et al, 2017). Consequently, we describe these markers as organic-biological (org-bio hereafter).…”

Section: Subcomposition Analysis Of Internal Mixing Statementioning

confidence: 97%

“…Another, but less common, approach is to use singleparticle mass spectrometry (SPMS) to provide an online assessment of aerosol composition. An advantage of this technique is that the high temporal resolution allows the evolution of the particle composition to be measured in a dynamic setting (Cziczo et al, 2006;Zelenyuk et al, 2009;Gaston et al, 2013), and the instruments can be deployed in line with other techniques such as counterflow virtual impactor (CVI) to measure ice residuals (Cziczo et al, 2003;Gallavardin et al, 2008;Baustian et al, 2012;Zelenyuk et al, 2015;Worringen et al, 2015;Schmidt et al, 2017). However, compositional analysis with SPMS is fraught with difficulties relating to poor reproducibility and the non-quantitative nature of the measurement associated with instrument function and parti-N. A. Marsden et al: Mineralogy of north African dust cle matrix effects (Reilly et al, 2000;Sullivan and Prather, 2005;Murphy, 2007;Hatch et al, 2014).…”

Section: Introductionmentioning

confidence: 99%

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Mineralogy and mixing state of north African mineral dust by online single-particle mass spectrometry

et al. 2019

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Abstract. The mineralogy and mixing state of dust particles originating from the African continent influences climate and marine ecosystems in the North Atlantic due to its effect on radiation, cloud properties and biogeochemical cycling. However, these processes are difficult to constrain because of large temporal and spatial variability, and the lack of in situ measurements of dust properties at all stages of the dust cycle. This lack of measurements is in part due to the remoteness of potential source areas (PSAs) and transport pathways but also because of the lack of an efficient method to report the mineralogy and mixing state of single particles with a time resolution comparable to atmospheric processes, which may last a few hours or less. Measurements are equally challenging in laboratory simulations where dust particles need to be isolated and characterised in low numbers whilst conditions are dynamically controlled and monitored in real time. This is particularly important in controlled expansion cloud chambers (CECCs) where ice-nucleating properties of suspended dust samples are studied in cold and mixed phase cloud conditions. In this work, the mineralogy and mixing state of the fine fraction (<2.5 µm) in laboratory-suspended dust from PSAs in north Africa were made using novel techniques with online single-particle mass spectrometry (SPMS) and traditional offline scanning electron microscopy (SEM). A regional difference in mineralogy was detected, with material sourced from Morocco containing a high number fraction of illite-like particles in contrast to Sahelian material which contains potassium- and sodium-depleted clay minerals like kaolinite. Single-particle mixing state had a much greater local variation than mineralogy, particularly with respect to organic–biological content. Applying the same methods to ambient measurement of transported dust in the marine boundary layer at Cabo Verde in the remote North Atlantic enabled the number fractions of illite/smectite clay mineral (ISCM), non-ISCM and calcium-containing particles to be reported at a 1 h time resolution over a 20-day period. Internal mixing of silicate particles with nitrate, chlorine and organic–biological material was also measured and compared to that in the suspended soils. The results show SPMS and SEM techniques are complementary and demonstrate that SPMS can provide a meaningful high-resolution measurement of single-particle mineralogy and mixing state in laboratory and ambient conditions. In most cases, the differences in the mineralogical composition between particles within a soil sample were small. Thus, particles were not composed of discrete mineral phases. In ambient measurements, the ISCM and nitrate content was found to change significantly between distinct dust events, indicating a shift in source and transport pathways which may not be captured in offline composition analysis or remote sensing techniques.

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Section: Subcomposition Analysis Of Internal Mixing Statementioning

confidence: 97%

Section: Introductionmentioning

confidence: 99%

Mineralogy and mixing state of north African mineral dust by online single-particle mass spectrometry

et al. 2019

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“…Several studies have already described and characterized LAAPTOFs (e.g. Wonaschuetz et al, 2017, Gemayel et al, 2016Shen et al, 2018a, Ramisetty et al, 2018, Mardsen et al, 2016. In brief, the LAAFTOF comprises three different regions as shown in Fig.…”

Section: Laaptof (Laser Ablation Aerosol Particle Time Of Flight) Mass Spectrometermentioning

confidence: 99%

On-line determination of the chemical composition of single activated cloud condensation nuclei – a first investigation of single urban CCN and CCN obtained from sea water samples

España

Wonaschuetz

Steiner

et al. 2020

Preprint

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Abstract. Cloud condensation nuclei (CCN) play an important role in cloud microphysics and are crucial for the second indirect effect of aerosols on global climate. One of the uncertainties in calculations of the indirect effect is due to insufficient data on CCN activation. The formation and growth processes of aerosol particles which subsequently become CCN determine their chemical composition. Due to the numerous organic and inorganic components present in atmospheric aerosol particles, a determination of the chemical composition of individual CCN is still challenging. To expand our understanding of activation of real-world CCN we introduce a novel method to characterize the chemical composition of single activated CCN in their droplet state. This method consists of a coupling of two essential instruments, a CCN-VACES (Cloud Condensation Nuclei-Versatile Aerosol Concentration Enrichment System) which is a modification of the original VACES to select and enrich CCN concentrations, and a Laser Ablation Aerosol Particle Time of Flight mass spectrometer (LAAPTOF), a single particle mass spectrometer. In the CCN-VACES, an aerosol flow is exposed to a specific water vapour supersaturation (in this study: 0.035 %, 0.054 %, 0.1 % and 0.6 %, respectively) and the CCN in the flow grow to droplets if their critical supersaturation is exceeded. These grown droplets are subsequently enriched in concentration by means of a virtual impactor at the end of the growth region by a factor of ca. 16 and pass directly into a LAAPTOF to measure the chemical composition of individual activated droplets. Contrary to widely held beliefs, the LAAPTOF is able to analyse refractory and non-refractory components even in aqueous droplets and can therefore be used to determine the chemical composition of actually activated CCN in their droplet state. Single particle spectra (for both positive and negative ions) were obtained from activated CCN in the ambient aerosol as well as activated CCN originating from aerosolized sea water samples collected at two different regions (Palma de Mallorca and San Sebastián, Spain). Ambient CCN were found to contain sometimes highly complex mixtures of different carbonaceous and non-carbonaceous components. Sea water derived CCN show the expected content of sea salt constituents, but the presence of organics is also observed. Activated CCN from the San Sebastián water samples have stronger sulphate signals than the Mallorca water sample. The LAAPTOF was found to provide insights into the composition of individual activated CCN.

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“…The LAAPTOF is a commercially available SPMS and has been described elsewhere (Ahern et al, 2016;Gemayel et al, 2016;Marsden et al, 2016;Ramisetty et al, 2018;Reitz et al, 2016;Shen et al, 2018;Wonaschuetz et al, 2017). In brief, aerosols are sampled with a flowrate of ~80 cm 3 min -1 via an aerodynamic lens.…”

Section: Measurement Location and Instrumentationmentioning

confidence: 99%

Understanding of atmospheric aerosol particles with improved particle identification and quantification by single particle mass spectrometry

Shen¹,

Saathoff²,

Huang³

et al. 2018

Preprint

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Abstract. Single particle mass spectrometry (SPMS) is a useful, albeit not fully quantitative tool to determine chemical composition and mixing state of aerosol particles in the atmosphere. During a six-week field campaign in summer 2016 at a rural site in the upper Rhine valley near Karlsruhe city in southwest Germany, ~3.7 x 105 single particles were analyzed by a laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF). Combining fuzzy classification, marker peaks, typical peak ratios, and laboratory-based reference spectra, seven major particle classes were identified. With the precise identification and well characterized overall detection efficiency (ODE) for this instrument, particle similarity can be transferred into corrected number fractions and further transferred into mass fractions. Considering the entire measurement period, Potassium rich and aromatics coated dust (class 5) dominated the particle number (46.5 % number fraction) and mass (36.0 % mass fraction); Sodium salts like particles (class 3) were the second lowest in number (3.5 %), but the second dominating class in terms of particle mass (25.3 %). This difference demonstrates the crucial role of particle mass quantification for SPMS data. Using corrections for maximum, mean, and minimum ODE, the total mass of the quantified particles measured by LAAPTOF accounts for ~12 %, ~25 %, and ~104 % of the total mass measured by an aerosol mass spectrometer (AMS) with a collection efficiency of 0.5. These two mass spectrometers show a good correlation (correlation coefficient γ > 0.6) regarding total mass for more than 70 % of the measurement time, indicating non-refractory species measured by AMS might originate from particles consisting of internally mixed non-refractory and refractory components. In addition, specific relationships of LAAPTOF ion intensities and AMS mass concentrations for non-refractory compounds were found for specific measurement periods. Furthermore, our approach allows for the first time to assign the non-refractory compounds measured by AMS to different particle classes. Overall AMS-nitrate was mainly arising from class 3, while class 5 was dominant during events rich in organic aerosol particles.

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Chemical composition of radiolytically formed particles using single-particle mass spectrometry

Cited by 9 publications

References 20 publications

Mineralogy and mixing state of north African mineral dust by online single-particle mass spectrometry

Mineralogy and mixing state of north African mineral dust by online single-particle mass spectrometry

On-line determination of the chemical composition of single activated cloud condensation nuclei – a first investigation of single urban CCN and CCN obtained from sea water samples

Understanding of atmospheric aerosol particles with improved particle identification and quantification by single particle mass spectrometry

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