Depositional ice nucleation on solid ammonium sulfate and glutaric acid particles

Baustian, K. J.; Wise, Matthew E.; Tolbert, Margaret A.

doi:10.5194/acp-10-2307-2010

Cited by 100 publications

(71 citation statements)

References 47 publications

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“…This extensive surface structure might be the reason that the particles acted as efficient ice nuclei for heterogeneous deposition nucleation with S ice,crit as low as 1.05 at T = 240 K. Also Parsons et al (2004) considered that the investigated saturated dicarboxylic acids C3-C6 might be more important in ice cloud formation if the particles had more defects than those generated in their study. And indeed, deposition mode ice nucleation on solid glutaric acid particles (C5) with S ice,crit as low as 1.20 at 235 K has recently been observed (Baustian et al, 2010). The active site explanation would also account for the observed dependence of f ice on the size of the oxalic acid dihydrate particles.…”

Section: Ice Nucleation Ability Of Oxalic Acid Dihydrate Crystallisamentioning

confidence: 84%

High variability of the heterogeneous ice nucleation potential of oxalic acid dihydrate and sodium oxalate

et al. 2010

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Abstract. The heterogeneous ice nucleation potential of airborne oxalic acid dihydrate and sodium oxalate particles in the deposition and condensation mode has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 244 and 228 K. Previous laboratory studies have highlighted the particular role of oxalic acid dihydrate as the only species amongst a variety of other investigated dicarboxylic acids to be capable of acting as a heterogeneous ice nucleus in both the deposition and immersion mode. We could confirm a high deposition mode ice activity for 0.03 to 0.8 µm sized oxalic acid dihydrate particles that were either formed by nucleation from a gaseous oxalic acid/air mixture or by rapid crystallisation of highly supersaturated aqueous oxalic acid solution droplets. The critical saturation ratio with respect to ice required for deposition nucleation was found to be less than 1.1 and the size-dependent ice-active fraction of the aerosol population was in the range from 0.1 to 22%. In contrast, oxalic acid dihydrate particles that had crystallised from less supersaturated solution droplets and had been allowed to slowly grow in a supersaturated environment from still unfrozen oxalic acid solution droplets over a time period of several hours were found to be much poorer heterogeneous ice nuclei. We speculate that under these conditions a crystal surface structure with less-active sites for the initiation of ice nucleation was generated. Such particles partially proved to be almost ice-inactive in both the deposition and condensation mode. At times, the heterogeneous ice nucleation ability of oxalic acid dihydrate significantly changed when the particles had been processed in preceding cloud droplet activation steps. Such behaviour was also observed for the second investiCorrespondence to: R. Wagner (robert.wagner2@kit.edu) gated species, namely sodium oxalate. Our experiments address the atmospheric scenario that coating layers of oxalic acid or its salts may be formed by physical and chemical processing on pre-existing particulates such as mineral dust and soot. Given the broad diversity of the observed heterogeneous ice nucleability of the oxalate species, it is not straightforward to predict whether an oxalate coating layer will improve or reduce the ice nucleation ability of the seed aerosol particles.

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Section: Ice Nucleation Ability Of Oxalic Acid Dihydrate Crystallisamentioning

confidence: 84%

High variability of the heterogeneous ice nucleation potential of oxalic acid dihydrate and sodium oxalate

et al. 2010

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“…The Raman spectrometer was equipped with an Olympus BX51 research-grade optical microscope which had the capability to magnify particles 10X, 20X, 50X and 100X. The experimental setup and procedure is similar to that used in Baustian et al (2010) and Wise et al (2010). Additional details are provided when the current experiment differs from that of Baustian et al (2010) and Wise et al (2010).…”

Section: Methodsmentioning

confidence: 99%

Depositional ice nucleation onto crystalline hydrated NaCl particles: a new mechanism for ice formation in the troposphere

et al. 2012

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Abstract. Sea-salt aerosol (SSA) particles are ubiquitous in the marine boundary layer and over coastal areas. Therefore SSA have ability to directly and indirectly affect the Earth's radiation balance. The influence SSA have on climate is related to their water uptake and ice nucleation characteristics. In this study, optical microscopy coupled with Raman spectroscopy was used to detect the formation of a crystalline NaCl hydrate that could form under atmospheric conditions. NaCl (s) particles (∼1 to 10 µm in diameter) deliquesced at 75.7 ± 2.5 % RH which agrees well with values previously established in the literature. NaCl (aq) particles effloresced to a mixture of hydrated and non-hydrated particles at temperatures between 236 and 252 K. The aqueous particles effloresced into the non-hydrated form at temperatures warmer than 252 K. At temperatures colder than 236 K all particles effloresced into the hydrated form. The deliquescence relative humidities (DRH) of hydrated NaCl (s) particles ranged from 76.6 to 93.2 % RH. Based on the measured DRH and efflorescence relative humidities (ERH), we estimate crystalline NaCl particles could be in the hydrated form 40-80 % of the time in the troposphere. Additionally, the ice nucleating abilities of NaCl (s) and hydrated NaCl (s) were determined at temperatures ranging from 221 to 238 K. Here, depositional ice nucleation is defined as the onset of ice nucleation and represents the conditions at which the first particle on the substrate nucleated ice. Thus the values reported here represent the lower limit of depositional ice nucleation. NaCl (s) particles depositionally nucleated ice at an average S ice value of 1.11 ± 0.07. Hydrated NaCl (s) particles depositionally nucleated ice at an average S ice value of 1.02 ± 0.04. When a mixture of hydrated and anhydrous NaCl (s) particles was present in the same sample, ice preferentially nucleated on the hydrated particles 100 % of the time. While both types of particles are efficient ice nuclei, hydrated NaCl (s) particles are better ice nuclei than NaCl (s) particles.

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“…Under similarly supersaturated conditions, oxalic acid or ammonium sulphate solution aerosol would be expected to slowly crystallise (Wagner et al, , 2011Abbatt et al, 2006). This is important because crystalline solid salts are known to catalyse ice nucleation (Wise et al, 2009Abbatt et al, 2006;Baustian et al, 2010;Shilling et al, 2006b;Eastwood et al, 2009), as are crystalline hydrates (Wise et al, 2012). However, nucleation and crystal growth in highly viscous or glassy aqueous aerosol particles is much slower.…”

Section: T W Wilson Et Al: Glassy Aerosols Nucleate Ice Heterogenementioning

confidence: 99%

Glassy aerosols with a range of compositions nucleate ice heterogeneously at cirrus temperatures

et al. 2012

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Abstract. Atmospheric secondary organic aerosol (SOA) is likely to exist in a semi-solid or glassy state, particularly at low temperatures and humidities. Previously, it has been shown that glassy aqueous citric acid aerosol is able to nucleate ice heterogeneously under conditions relevant to cirrus in the tropical tropopause layer (TTL). In this study we test if glassy aerosol distributions with a range of chemical compositions heterogeneously nucleate ice under cirrus conditions. Three single component aqueous solution aerosols (raffinose, 4-hydroxy-3-methoxy-DL-mandelic acid (HMMA) and levoglucosan) and one multi component aqueous solution aerosol (raffinose mixed with five dicarboxylic acids and ammonium sulphate) were studied in both the liquid and glassy states at a large cloud simulation chamber. The investigated organic compounds have similar functionality to oxidised organic material found in atmospheric aerosol and have estimated temperature/humidity induced glass transition thresholds that fall within the range predicted for atmospheric SOA. A small fraction of aerosol particles of all compositions were found to nucleate ice heterogeneously in the deposition mode at temperatures relevant to the TTL (< 200 K). Raffinose and HMMA, which form glasses at higher temperatures, nucleated ice heterogeneously at temperatures as high as 214.6 and 218.5 K respectively. We present the calculated ice active surface site density, n s , of the aerosols tested here and also of glassy citric acid aerosol as a function of relative humidity with respect to ice (RH i ). We also propose a parameterisation which can be used to estimate heterogeneous ice nucleation by glassy aerosol for use in cirrus cloud models up to ∼ 220 K. Finally, we show that heterogeneous nucleation by glassy aerosol may compete with ice nucleation on mineral dust particles in midlatitudes cirrus.

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Depositional ice nucleation on solid ammonium sulfate and glutaric acid particles

Cited by 100 publications

References 47 publications

High variability of the heterogeneous ice nucleation potential of oxalic acid dihydrate and sodium oxalate

High variability of the heterogeneous ice nucleation potential of oxalic acid dihydrate and sodium oxalate

Depositional ice nucleation onto crystalline hydrated NaCl particles: a new mechanism for ice formation in the troposphere

Glassy aerosols with a range of compositions nucleate ice heterogeneously at cirrus temperatures

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