The Role of Organic Aerosol in Atmospheric Ice Nucleation: A Review

Knopf, Daniel A.; Alpert, Peter A.; Wang, Bingbing

doi:10.1021/acsearthspacechem.7b00120

Cited by 245 publications

(395 citation statements)

References 473 publications

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“…The C-rich particles encountered are most likely organic aerosol. This is in good accordance with the results of many field studies (see the recent review by Knopf et al (2018) and references therein) which show that organic aerosol is found in the IPR fraction, but is depleted relative to total aerosol.…”

supporting

confidence: 92%

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

Preprint

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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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supporting

confidence: 92%

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

Preprint

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“…Molecular motion can be hindered in a highly viscous matrix, slowing down photochemical reactions in particles (Lignell et al, 2014;Hinks et al, 2016). Water diffusion can still be fast even in an amorphous solid matrix under room temperature, but it can be hindered significantly under low temperatures (Mikhailov et al, 2009;Zobrist et al, 2011;Bones et al, 2012;Berkemeier et al, 2014;Price et al, 2014), affecting homogeneous vs. heterogeneous ice nucleation pathways (Murray et al, 2010;Wagner et al, 2012;Wang et al, 2012a, b;Wilson et al, 2012;Baustian et al, 2013;Schill and Tolbert, 2013;Schill et al, 2014;Lienhard et al, 2015;Ignatius et al, 2016;Knopf et al, 2018). Despite the substantial implications of the SOA particle phase state, its effects on gasparticle interactions have not yet been considered explicitly in current climate and air quality models (Shrivastava et al, 2017a).…”

Section: Introductionmentioning

confidence: 99%

Predicting the glass transition temperature and viscosity of secondary organic material using molecular composition

et al. 2018

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Abstract. Secondary organic aerosol (SOA) accounts for a large fraction of submicron particles in the atmosphere. SOA can occur in amorphous solid or semi-solid phase states depending on chemical composition, relative humidity (RH), and temperature. The phase transition between amorphous solid and semi-solid states occurs at the glass transition temperature (T g ). We have recently developed a method to estimate T g of pure compounds containing carbon, hydrogen, and oxygen atoms (CHO compounds) with molar mass less than 450 g mol −1 based on their molar mass and atomic O : C ratio. In this study, we refine and extend this method for CH and CHO compounds with molar mass up to ∼ 1100 g mol −1 using the number of carbon, hydrogen, and oxygen atoms. We predict viscosity from the T g -scaled Arrhenius plot of fragility (viscosity vs. T g /T ) as a function of the fragility parameter D. We compiled D values of organic compounds from the literature and found that D approaches a lower limit of ∼ 10 (±1.7) as the molar mass increases. We estimated the viscosity of α-pinene and isoprene SOA as a function of RH by accounting for the hygroscopic growth of SOA and applying the Gordon-Taylor mixing rule, reproducing previously published experimental measurements very well. Sensitivity studies were conducted to evaluate impacts of T g , D, the hygroscopicity parameter (κ), and the Gordon-Taylor constant on viscosity predictions. The viscosity of toluene SOA was predicted using the elemental composition obtained by high-resolution mass spectrometry (HRMS), resulting in a good agreement with the measured viscosity. We also estimated the viscosity of biomass burning particles using the chemical composition measured by HRMS with two different ionization techniques: electrospray ionization (ESI) and atmospheric pressure photoionization (APPI). Due to differences in detected organic compounds and signal intensity, predicted viscosities at low RH based on ESI and APPI measurements differ by 2-5 orders of magnitude. Complementary measurements of viscosity and chemical composition are desired to further constrain RH-dependent viscosity in future studies.

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“…after cloud processing, where the aerosol first activated to supercooled cloud droplets and then froze homogeneously (Ladino et al, 2014;Wagner et al, 2017). These and other studies on the ice-nucleating ability of SOA particles are summarized in Hoose and Möhler (2012) and Knopf et al (2018). It has to be stressed that in the above-mentioned studies and our study the SOA generation procedures and conditions can vary significantly, as can the methods used to measure ice nucleation; see the Introduction for details.…”

Section: Discussionmentioning

confidence: 93%

“…Indeed, an effect of different temperatures in the chambers or sampling lines was found and discussed by e.g. Ignatius et al (2016) and Knopf et al (2018). However, the aerosol chamber DMPS and cloud chamber SMPS aerosol size distributions do not indicate major growth of particles between transfer and cloud evacuation.…”

Section: Discussionmentioning

confidence: 99%

“…While certain aerosol particles such as dust are known to be important icenucleating particles (INPs), others are highly abundant, yet their ice-forming abilities remain poorly understood. One example of such particles is secondary organic aerosol (SOA; see also a recent review about the role of organic aerosol as INPs by Knopf et al, 2018). They originate from biogenic and anthropogenic sources, e.g.…”

Section: Introductionmentioning

confidence: 99%

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The efficiency of secondary organic aerosol particles acting as ice-nucleating particles under mixed-phase cloud conditions

Frey

Dorsey

et al. 2018

Atmos. Chem. Phys.

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Abstract. Secondary organic aerosol (SOA) particles have been found to be efficient ice-nucleating particles under the cold conditions of (tropical) upper-tropospheric cirrus clouds. Whether they also are efficient at initiating freezing under slightly warmer conditions as found in mixedphase clouds remains undetermined. Here, we study the icenucleating ability of photochemically produced SOA particles with the combination of the Manchester Aerosol Chamber and Manchester Ice Cloud Chamber. Three SOA systems were tested resembling biogenic and anthropogenic particles as well as particles of different phase state. These are namely α-pinene, heptadecane, and 1,3,5-trimethylbenzene. After the aerosol particles were formed, they were transferred into the cloud chamber, where subsequent quasi-adiabatic cloud activation experiments were performed. Additionally, the ice-forming abilities of ammonium sulfate and kaolinite were investigated as a reference to test the experimental setup.Clouds were formed in the temperature range of −20 to −28.6 • C. Only the reference experiment using dust particles showed evidence of ice nucleation. No ice particles were observed in any other experiment. Thus, we conclude that SOA particles produced under the conditions of the reported experiments are not efficient ice-nucleating particles starting at liquid saturation under mixed-phase cloud conditions.

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The Role of Organic Aerosol in Atmospheric Ice Nucleation: A Review

Cited by 245 publications

References 473 publications

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

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

Predicting the glass transition temperature and viscosity of secondary organic material using molecular composition

The efficiency of secondary organic aerosol particles acting as ice-nucleating particles under mixed-phase cloud conditions

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