How well can we predict cluster fragmentation inside a mass spectrometer?

Passananti, Monica; Zapadinsky, Evgeni; Zanca, Tommaso; Kangasluoma, Juha; Myllys, Nanna; Rissanen, Matti; Kurtén, Theo; Ehn, Mikael; Attoui, Michel; Vehkamäki, Hanna

doi:10.1039/c9cc02896j

Cited by 60 publications

(59 citation statements)

References 18 publications

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“…This is due to the large acceleration acquired by the cluster in region III, with subsequent possible collision at high energy in the beginning of the next region. These results are complementary to previous data reported in literature (Passananti et al, 2019;Lopez-Hilfiker et al, 2016) and help to define the terms "declustering voltages" as the voltages that induce decomposition (between the region II and III) and the "declustering region" as the region of the APi where the decomposition takes place (region IV).…”

Section: Generationsupporting

confidence: 80%

“…Although the decomposition is mainly induced by the voltages applied between regions II and III as shown in Passananti et al (2019), these results demonstrate that the decomposition takes place mainly in region IV (Fig. 9a).…”

Section: Generationmentioning

confidence: 75%

“…Recently, a numerical model to study decomposition in the APi-TOF has been developed by Zapadinsky et al (2018). The decomposition model has been tested on simple clusters involving one bisulfate anion and two sulfuric acid molecules, giving very good agreement with experimental results (Passananti et al, 2019).…”

mentioning

confidence: 80%

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HOM cluster decomposition in APi-TOF mass spectrometers

Zanca

Kubečka

Zapadinsky

et al. 2020

Preprint

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Abstract. Identification of atmospheric molecular clusters and measurement of their concentrations by APi-TOF mass spectrometers may be affected by systematic error due to possible decomposition of clusters inside the instrument. Here, we perform numerical simulations of decomposition in an APi-TOF and formation in the atmosphere of a set of clusters which involve a representative kind of highly-oxygenated organic molecule (HOM), with molecular formula C10H16O8. This elemental composition corresponds to one of the most common mass peaks observed in experiments on ozone-initiated autoxidation of α-pinene. Our results show that decomposition is highly unlikely for the considered clusters, provided their bonding energy is large enough to allow formation in the atmosphere in the first place.

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Section: Generationsupporting

confidence: 80%

Section: Generationmentioning

confidence: 75%

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HOM cluster decomposition in APi-TOF mass spectrometers

Zanca

Kubečka

Zapadinsky

et al. 2020

Preprint

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“…Here we introduce a significant progress in the CIMS methodology by enabling atmospheric pressure sampling and ionization with multiple consecutive reagent ions in fast repetition, and without any pretreatment of the sampled gas mixture. When considering the detection of low-volatile, in situ aerosol precursor compounds such as HOM (i) that lack analytical standards, (ii) that have a range of individual detection sensitivities (Hyttinen et al, 2015(Hyttinen et al, , 2018, (iii) whose transmission and (iv) fragmentation are dependent on the detailed MS settings Zapadinsky et al, 2019;Passananti et al, 2019) and (v) whose detection is sensitive to changes in temperature (Frege et al, 2018), it becomes evident that retrieving complementary data depending on only one instrument calibration factor is extremely valuable. In the newly developed Multi-scheme chemical IONization inlet (MION) described here, the only changing parameter between the ionization stages is the ion-specific sensitivity to the target compounds as a function of the ion-molecule reaction time -which does not differ between applications.…”

Section: Introductionmentioning

confidence: 99%

Multi-scheme chemical ionization inlet (MION) for fast switching of reagent ion chemistry in atmospheric pressure chemical ionization mass spectrometry (CIMS) applications

et al. 2019

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Abstract. A novel chemical ionization inlet named the Multi-scheme chemical IONization inlet (MION), Karsa Ltd., Helsinki, Finland) capable of fast switching between multiple reagent ion schemes is presented, and its performance is demonstrated by measuring several known oxidation products from much-studied cyclohexene and α-pinene ozonolysis systems by applying consecutive bromide (Br−) and nitrate (NO3-) chemical ionization. Experiments were performed in flow tube reactors under atmospheric pressure and room temperature (22 ∘C) utilizing an atmospheric pressure interface time-of-flight mass spectrometer (APi-ToF-MS, Tofwerk Ltd., Thun, Switzerland) as the detector. The application of complementary ion modes in probing the same steady-state reaction mixture enabled a far more complete picture of the detailed autoxidation process; the HO2 radical and the least-oxidized reaction products were retrieved with Br− ionization, whereas the highest-oxidized reaction products were detected in the NO3- mode, directly providing information on the first steps and on the ultimate endpoint of oxidation, respectively. While chemical ionization inlets with multiple reagent ion capabilities have been reported previously, an application in which the charging of the sample occurs at atmospheric pressure with practically no sample pretreatment, and with the potential to switch the reagent ion scheme within a second timescale, has not been introduced previously. Also, the ability of bromide ionization to detect highly oxygenated organic molecules (HOM) from atmospheric autoxidation reactions has not been demonstrated prior to this investigation.

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“…For the further analysis, we assume that deprotonation is the only mechanism of declustering, as it is one known to potentially follow already from relatively soft collisions. Additional declustering may happen by more energetic collisions in the lower-pressure regions of the mass spectrometer (Passananti et al, 2019).…”

Section: Soa Particles Characterizationmentioning

confidence: 99%

Composition and volatility of SOA formed from oxidation of real tree emissions compared to single VOC-systems

Ylisirniö¹,

Buchholz²,

Mohr³

et al. 2019

Preprint

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<p><strong>Abstract.</strong> Secondary organic aerosol (SOA) is an important constituent of the atmosphere where SOA particles are formed chiefly by the condensation or reactive uptake of oxidation products of volatile organic compounds (VOC). The mass yield in SOA particle formation, as well as the chemical composition and volatility of the particles are determined by the identity of the VOC precursor(s) and the oxidation conditions they experience. In this study, we used an oxidation flow reactor to generate biogenic SOA from the oxidation of Scots pine emissions. Mass yields, chemical composition, and volatility of the SOA particles were characterized and compared with SOA particles formed from oxidation of &#945;-pinene and of a mixture of acyclic/monocyclic sesquiterpenes (farnesenes and bisabolenes), which are significant components of the Scots pine emissions. SOA mass yields for Scots pine emissions dominated by farnesenes were lower than for &#945;-pinene, but higher than for the artificial mixture of farnesenes and bisabolenes. The reduction in the SOA yield in the farnesenes and bisabolenes dominated mixtures is due to C=C bond scission in these acyclic/monocyclic sesquiterpenes during ozonolysis leading to smaller and generally more volatile products. SOA particles from the oxidation of Scots pine emission had similar or lower volatility than SOA particles formed from either of single precursor. Applying physical stress to the Scots pine plants increased monoterpene emissions, which further decreased SOA particle volatility and increased SOA mass yield. Our results highlight the need to account for the chemical complexity and structure of real-world biogenic VOC emissions and stress-induced changes to plant emissions when modelling SOA production and properties in the atmosphere. These results emphasize that simple increase or decrease of relative monoterpene and sesquiterpene emissions should not be used as indicator of SOA particle volatility.</p>

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How well can we predict cluster fragmentation inside a mass spectrometer?

Abstract: We measured the fragmentation of clusters inside an MS and we developed a model to describe and predict their fragmentation.

Cited by 60 publications

References 18 publications

HOM cluster decomposition in APi-TOF mass spectrometers

HOM cluster decomposition in APi-TOF mass spectrometers

Multi-scheme chemical ionization inlet (MION) for fast switching of reagent ion chemistry in atmospheric pressure chemical ionization mass spectrometry (CIMS) applications

Composition and volatility of SOA formed from oxidation of real tree emissions compared to single VOC-systems

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