Crystallization of Aqueous Inorganic−Malonic Acid Particles:  Nucleation Rates, Dependence on Size, and Dependence on the Ammonium-to-Sulfate Ratio

Parsons, Matthew T.; Riffell, Jenna L.; Bertram, Allan K.

doi:10.1021/jp057074n

Cited by 70 publications

(85 citation statements)

References 59 publications

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“…Interactions between organic and inorganic components within an aerosol particle can influence DRH and ERH of inorganic salts or even totally suppress crystallization (Marcolli et al, 2004;Parsons et al, 2006). Furthermore, liquid-liquid phase separation (LLPS) into a mainly polar inorganic and a less polar organicrich phase during humidity cycles may occur (Marcolli and Krieger, 2006).…”

Section: Song Et Al: Liquid-liquid Phase Separation and Morphologymentioning

confidence: 99%

“…Previous studies on phase transitions of single aerosol particles have mostly been performed with one organic substance in the presence of AS (Parsons et al, 2006;Ling and Chan, 2008;Ciobanu et al, 2009;Yeung et al, 2009;Bertram et al, 2011). Studies on more complex organic mixtures are needed to obtain insight into the phase transitions of organic/inorganic aerosols considering atmospheric aerosol composition.…”

Section: Song Et Al: Liquid-liquid Phase Separation and Morphologymentioning

confidence: 99%

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Liquid-liquid phase separation and morphology of internally mixed dicarboxylic acids/ammonium sulfate/water particles

et al. 2012

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Abstract. Knowledge of the physical state and morphology of internally mixed organic/inorganic aerosol particles is still largely uncertain. To obtain more detailed information on liquid-liquid phase separation (LLPS) and morphology of the particles, we investigated complex mixtures of atmospherically relevant dicarboxylic acids containing 5, 6, and 7 carbon atoms (C5, C6 and C7) having oxygen-to-carbon atomic ratios (O:C) of 0.80, 0.67, and 0.57, respectively, mixed with ammonium sulfate (AS). With micrometer-sized particles of C5/AS/H 2 O, C6/AS/H 2 O and C7/AS/H 2 O as model systems deposited on a hydrophobically coated substrate, laboratory experiments were conducted for various organic-to-inorganic dry mass ratios (OIR) using optical microscopy and Raman spectroscopy. When exposed to cycles of relative humidity (RH), each system showed significantly different phase transitions. While the C5/AS/H 2 O particles showed no LLPS with OIR = 2:1, 1:1 and 1:4 down to 20 % RH, the C6/AS/H 2 O and C7/AS/H 2 O particles exhibit LLPS upon drying at RH 50 to 85 % and ∼90 %, respectively, via spinodal decomposition, growth of a second phase from the particle surface or nucleation-and-growth mechanisms depending on the OIR. This suggests that LLPS commonly occurs within the range of O:C < 0.7 in tropospheric organic/inorganic aerosols. To support the comparison and interpretation of the experimentally observed phase transitions, thermodynamic equilibrium calculations were performed with the AIOMFAC model. For the C7/AS/H 2 O and C6/AS/H 2 O systems, the calculated phase diagrams agree well with the observations while for the C5/AS/H 2 O system LLPS is predicted by the model at RH below 60 % and higher AS concentration, but was not observed in the experiments.Both core-shell structures and partially engulfed structures were observed for the investigated particles, suggesting that such morphologies might also exist in tropospheric aerosols.

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Section: Song Et Al: Liquid-liquid Phase Separation and Morphologymentioning

confidence: 99%

Section: Song Et Al: Liquid-liquid Phase Separation and Morphologymentioning

confidence: 99%

Liquid-liquid phase separation and morphology of internally mixed dicarboxylic acids/ammonium sulfate/water particles

et al. 2012

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“…Many studies on phase transitions of mixed organicinorganic salt particles of atmospheric relevance have focused on deliquescence and efflorescence (see for example Brooks et al, 2002Brooks et al, , 2003Choi and Chan, 2002;Chan and Chan, 2003;Wise et al, 2003;Braban and Abbatt, 2004;Pant et al, 2004;Parsons et al, 2004aParsons et al, , 2006Badger et al, 2006;Marcolli and Krieger, 2006;Salcedo, 2006;Ling and Chan, 2008;Treuel et al, 2009;Bertram et al, 2011;Smith et al, 2012). These studies have shown that when liquidliquid phase separation does not occur, the addition of organics to inorganic salts lowers the deliquescence and efflorescence relative humidities of the salts.…”

Section: Y You Et Al: Liquid-liquid Phase Separation In Particles Cmentioning

confidence: 99%

Liquid–liquid phase separation in particles containing organics mixed with ammonium sulfate, ammonium bisulfate, ammonium nitrate or sodium chloride

2013

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Abstract. As the relative humidity varies from high to low values in the atmosphere, particles containing organic species and inorganic salts may undergo liquid-liquid phase separation. The majority of the laboratory work on this subject has used ammonium sulfate as the inorganic salt. In the following we studied liquid-liquid phase separation in particles containing organics mixed with the following salts: ammonium sulfate, ammonium bisulfate, ammonium nitrate and sodium chloride. In each experiment one organic was mixed with one inorganic salt and the liquid-liquid phase separation relative humidity (SRH) was determined. Since we studied 23 different organics mixed with four different salts, a total of 92 different particle types were investigated. Out of the 92 types, 49 underwent liquid-liquid phase separation. For all the inorganic salts, liquid-liquid phase separation was never observed when the oxygen-to-carbon elemental ratio (O : C) ≥ 0.8 and was always observed for O : C < 0.5. For 0.5 ≤ O : C < 0.8, the results depended on the salt type. Out of the 23 organic species investigated, the SRH of 20 organics followed the trend: (NH 4 ) 2 SO 4 ≥ NH 4 HSO 4 ≥ NaCl ≥ NH 4 NO 3 . This trend is consistent with previous salting out studies and the Hofmeister series. Based on the range of O : C values found in the atmosphere and the current results, liquid-liquid phase separation is likely a frequent occurrence in both marine and non-marine environments.

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“…Zhang and Chan, 2000;Lee et al, 2008), hygroscopicity and phase transition (e.g. Tang and Munkelwitz, 1994;Choi and Chan, 2002;Li et al, 2005;Parsons et al, 2006;Pope et al, 2010a;Zobrist et al, 2011), measurement of vapour pressure (e.g. Pope et al, 2010b;Soonsin et al, 2010), oxidation chemistry (e.g.…”

Section: H-j Tong Et Al: a New Electrodynamic Balance (Edb) Designmentioning

confidence: 99%

A new electrodynamic balance (EDB) design for low-temperature studies: application to immersion freezing of pollen extract bioaerosols

et al. 2015

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Abstract. In this paper we describe a newly designed cold electrodynamic balance (CEDB) system, built to study the evaporation kinetics and freezing properties of supercooled water droplets. The temperature of the CEDB chamber at the location of the levitated water droplet can be controlled in the range −40 to +40 • C, which is achieved using a combination of liquid nitrogen cooling and heating by positive temperature coefficient heaters. The measurement of liquid droplet radius is obtained by analysing the Mie elastic light scattering from a 532 nm laser. The Mie scattering signal was also used to characterise and distinguish droplet freezing events; liquid droplets produce a regular fringe pattern, whilst the pattern from frozen particles is irregular. The evaporation rate of singly levitated water droplets was calculated from time-resolved measurements of the radii of evaporating droplets and a clear trend of the evaporation rate on temperature was measured. The statistical freezing probabilities of aqueous pollen extracts (pollen washing water) are obtained in the temperature range −4.5 to −40 • C. It was found that that pollen washing water from water birch (Betula fontinalis occidentalis) pollen can act as ice nuclei in the immersion freezing mode at temperatures as warm as −22.45 (±0.65) • C. Furthermore it was found that the protein-rich component of the washing water was significantly more iceactive than the non-proteinaceous component.

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Crystallization of Aqueous Inorganic−Malonic Acid Particles: Nucleation Rates, Dependence on Size, and Dependence on the Ammonium-to-Sulfate Ratio

Cited by 70 publications

References 59 publications

Liquid-liquid phase separation and morphology of internally mixed dicarboxylic acids/ammonium sulfate/water particles

Liquid-liquid phase separation and morphology of internally mixed dicarboxylic acids/ammonium sulfate/water particles

Liquid–liquid phase separation in particles containing organics mixed with ammonium sulfate, ammonium bisulfate, ammonium nitrate or sodium chloride

A new electrodynamic balance (EDB) design for low-temperature studies: application to immersion freezing of pollen extract bioaerosols

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