High molecular weight SOA formation during limonene ozonolysis: insights from ultrahigh-resolution FT-ICR mass spectrometry characterization

Kundu, Shuvashish; Fisseha, R.; Putman, Annie L.; Rahn, T.; Mazzoleni, Lynn

doi:10.5194/acp-12-5523-2012

Cited by 111 publications

(158 citation statements)

References 40 publications

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“…Using the above values for molecular weight, density and van't Hoff factor as input the estimated values of κ i becomes: κ SOA = 0.1265 for SOA, κ POA = 0 for POA and κ BC = 0 for the soot core, respectively. The calculated κ SOA value is similar as reported in the literature for isoprene-derived secondary organic material particles (κ = 0.12 ± 0.06; Kuwata et al, 2013, and references therein), laboratory smog chamber SOA from trimethylbenzene (κ ≈ 0.04-0.15; Jimenez et al, 2009), κ values of SOA formed from m-xylene and toluene (κ ≈ 0.1-0.27; Lambe et al, 2011) and photochemically aged diesel soot particles (κ = 0-0.13; Tritscher et al, 2011).…”

Section: Ccn Activation Modellingsupporting

confidence: 87%

“…The mean molar mass (M) is a difficult property to measure, as pointed out by Hallquist et al (2009). In the literature a variety of average molar mass (M) for both SOA (∼ 0.15-0.480 kg mol −1 ; Hallquist et al, 2009;Kuwata et al, 2013) and POA (0.25-0.7 kg mol −1 for lubrication oil; e.g. Stubington et al, 1995) are reported.…”

Section: Ccn Activation Modellingmentioning

confidence: 99%

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Cloud droplet activity changes of soot aerosol upon smog chamber ageing

Wittbom¹,

Pagels²,

Rissler³

et al. 2014

Preprint

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Abstract. Particles containing soot, or black carbon, are generally considered to contribute to global warming. However, large uncertainties remain in the net climate forcing resulting from anthropogenic emissions of black carbon (BC), to a large extent due to the fact that BC is co-emitted with gases and primary particles, both organic and inorganic, and subject to atmospheric ageing processes. In this study, diesel exhaust particles and particles from a flame soot generator spiked with light aromatic secondary organic aerosol (SOA) precursors were processed by UV-radiation in a 6 m3 Teflon chamber in the presence of NOx. The time-dependent changes of the soot nanoparticle properties were characterised using a Cloud Condensation Nuclei Counter, an Aerosol Particle Mass Analyzer and a Soot Particle Aerosol Mass Spectrometer. The results show that freshly emitted soot particles do not activate into cloud droplets at supersaturations ≤ 2%, i.e. the black carbon core coated with primary organic aerosol (POA) from the exhaust is limited in hygroscopicity. Before the onset of UV radiation it is unlikely that any substantial SOA formation is taking place. An immediate change in cloud-activation properties occurs at the onset of UV exposure. This change in hygroscopicity is likely attributed to SOA formed from intermediate volatile organic compounds (IVOC) in the diesel engine exhaust. The change of cloud condensation nuclei (CCN) properties at the onset of UV radiation implies that the lifetime of soot particles in the atmosphere is affected by the access to sunlight, which differs between latitudes. The ageing of soot particles progressively enhances their ability to act as cloud condensation nuclei, due to changes in: (I) organic fraction of the particle, (II) chemical properties of this fraction (POA or SOA), (III) particle size, and (IV) particle morphology. Applying κ-Köhler theory, using a κSOA value of 0.13 (derived from independent input parameters describing the organic material), showed good agreement with cloud droplet activation measurements for particles with a SOA mass fraction (mfSOA(APM)) ≥ 0.12 (slightly aged particles). The activation properties are enhanced with only a slight increase in organic material coating the soot particles (mfSOA(APM) < 0.12), however not as much as predicted with Köhler theory. The discrepancy between theory and experiments might be due to solubility limitations, unevenly distributed organic material or hindering particle morphology. The change in properties of soot nanoparticles upon photochemical processing clearly increases their hygroscopicity, which affects their behaviour both in the atmosphere and in the human respiratory system.

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Section: Ccn Activation Modellingsupporting

confidence: 87%

Section: Ccn Activation Modellingmentioning

confidence: 99%

Cloud droplet activity changes of soot aerosol upon smog chamber ageing

Wittbom¹,

Pagels²,

Rissler³

et al. 2014

Preprint

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“…According to several studies SOA particles may contain oligomers, polymers and other high molecular weight molecules (Tolocka et al, 2004;Gao et al, 2004;Kalberer et al, 2004;Hallquist et al, 2009;Hall IV and Johnston, 2011;Kundu et al, 2012). Such oligomers and polymers are likely to affect the phase state of SOA particles.…”

Section: Discussionmentioning

confidence: 99%

Humidity-dependent phase state of SOA particles from biogenic and anthropogenic precursors

et al. 2012

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Abstract. The physical phase state (solid, semi-solid, or liquid) of secondary organic aerosol (SOA) particles has important implications for a number of atmospheric processes. We report the phase state of SOA particles spanning a wide range of oxygen to carbon ratios (O / C), used here as a surrogate for SOA oxidation level, produced in a flow tube reactor by photo-oxidation of various atmospherically relevant surrogate anthropogenic and biogenic volatile organic compounds (VOCs). The phase state of laboratory-generated SOA was determined by the particle bounce behavior after inertial impaction on a polished steel substrate. The measured bounce fraction was evaluated as a function of relative humidity and SOA oxidation level (O / C) measured by an Aerodyne high resolution time of flight aerosol mass spectrometer (HR-ToF AMS).The main findings of the study are: (1) biogenic and anthropogenic SOA particles are found to be amorphous solid or semi-solid based on the measured bounced fraction (BF), which was typically higher than 0.6 on a 0 to 1 scale. A decrease in the BF is observed for most systems after the SOA is exposed to relative humidity of at least 80 % RH, corresponding to a RH at impaction of 55 %. (2) Long-chain alkanes have a low BF (indicating a "liquid-like", less viscous phase) particles at low oxidation levels (BF < 0.2 ± 0.05 for O / C = 0.1). However, BF increases substantially upon increasing oxidation. (3) Increasing the concentration of sulphuric acid (H 2 SO 4 ) in solid SOA particles (here tested for longifolene SOA) causes a decrease in BF levels. (4) In the majority of cases the bounce behavior of the various SOA systems did not show correlation with the particle O / C. Rather, the molar mass of the gas-phase VOC precursor showed a positive correlation with the resistance to the RH-induced phase change of the formed SOA particles.

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“…Indeed the production of many BVOCs appears species (even genotype) and condition specific (Llusia et al 2002;Yuan et al 2009). One study found that a seedling of Scots pine (Pinus sylvestris) emits at least 20 distinct monoterpenes (Heijari et al 2011) and just one of these, limonene, can become over one thousand distinct compounds in the atmosphere (Kundu et al 2012;Holopainen and Blande 2013). Our ability to detect and distinguish these compounds is improving: for example, one study over just one citrus orchard in the USA detected and tracked the varying atmospheric abundance of over 500 different organic compounds derived from the vegetation (Park et al 2013).…”

Section: Condensationmentioning

confidence: 99%

Forests, atmospheric water and an uncertain future: the new biology of the global water cycle

Sheil

2018

For. Ecosyst.

144

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Theory and evidence indicate that trees and other vegetation influence the atmospheric water-cycle in various ways. These influences are more important, more complex, and more poorly characterised than is widely realised. While there is little doubt that changes in tree cover will impact the water-cycle, the wider consequences remain difficult to predict as the underlying relationships and processes remain poorly characterised. Nonetheless, as forests are vulnerable to human activities, these linked aspects of the water-cycle are also at risk and the potential consequences of large scale forest loss are severe. Here, for non-specialist readers, I review our knowledge of the links between vegetation-cover and climate with a focus on forests and rain (precipitation). I highlight advances, uncertainties and research opportunities. There are significant shortcomings in our understanding of the atmospheric hydrological cycle and of its representation in climate models. A better understanding of the role of vegetation and tree-cover will reduce some of these shortcomings. I outline and illustrate various research themes where these advances may be found. These themes include the biology of evaporation, aerosols and atmospheric motion, as well as the processes that determine monsoons and diurnal precipitation cycles. A novel theory-the 'biotic pump'-suggests that evaporation and condensation can exert a major influence over atmospheric dynamics. This theory explains how high rainfall can be maintained within those continental land-masses that are sufficiently forested. Feedbacks within many of these processes can result in non-linear behaviours and the potential for dramatic changes as a result of forest loss (or gain): for example, switching from a wet to a dry local climate (or visa-versa). Much remains unknown and multiple research disciplines are needed to address this: forest scientists and other biologists have a major role to play. New ideas, methods and data offer opportunities to improve understanding. Expect surprises.

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High molecular weight SOA formation during limonene ozonolysis: insights from ultrahigh-resolution FT-ICR mass spectrometry characterization

Cited by 111 publications

References 40 publications

Cloud droplet activity changes of soot aerosol upon smog chamber ageing

Cloud droplet activity changes of soot aerosol upon smog chamber ageing

Humidity-dependent phase state of SOA particles from biogenic and anthropogenic precursors

Forests, atmospheric water and an uncertain future: the new biology of the global water cycle

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