scholarly journals Viscous organic aerosol particles in the upper troposphere: diffusivity-controlled water uptake and ice nucleation?

2015 ◽  
Vol 15 (17) ◽  
pp. 24473-24511 ◽  
Author(s):  
D. M. Lienhard ◽  
A. J. Huisman ◽  
U. K. Krieger ◽  
Y. Rudich ◽  
C. Marcolli ◽  
...  
Keyword(s):  
Water Uptake ◽  
Condensed Phase ◽  
Aerosol Particles ◽  
Organic Aerosol ◽  
Ice Nucleation ◽  
Water Diffusion ◽  
Tropical Tropopause ◽  
Phase Water ◽  
Very High ◽  
Heterogeneous Ice Nucleation

Abstract. New measurements of water diffusion in aerosol particles produced from secondary organic aerosol (SOA) material and from a number of organic/inorganic model mixtures (3-methylbutane-1,2,3-tricarboxylic acid (3-MBTCA), levoglucosan, levoglucosan/NH4HSO4, raffinose) indicate that water diffusion coefficients are determined by several properties of the aerosol substance and cannot be inferred from the glass transition temperature or bouncing properties. Our results suggest that water diffusion in SOA particles is faster than often assumed and imposes no significant kinetic limitation on water uptake and release at temperatures above 220 K. The fast diffusion of water suggests that heterogeneous ice nucleation on a glassy core is very unlikely in these systems. At temperatures below 220 K, model simulations of SOA droplets suggest that heterogeneous ice nucleation may occur in the immersion mode on glassy cores which remain embedded in a liquid shell when experiencing fast updraft velocities. The particles absorb significant quantities of water during these updrafts which plasticize their outer layers such that these layers equilibrate readily with the gas phase humidity before the homogeneous ice nucleation threshold is reached. Glass formation is thus unlikely to restrict homogeneous ice nucleation. Only under most extreme conditions near the very high tropical tropopause may the homogeneous ice nucleation rate coefficient be reduced as a consequence of slow condensed-phase water diffusion. Since the differences between the behavior limited or non limited by diffusion are small even at the very high tropical tropopause, condensed-phase water diffusivity is unlikely to have significant consequences on the direct climatic effects of SOA particles under tropospheric conditions.

scholarly journals Viscous organic aerosol particles in the upper troposphere: diffusivity-controlled water uptake and ice nucleation?

2015 ◽  
Vol 15 (23) ◽  
pp. 13599-13613 ◽  
Author(s):  
D. M. Lienhard ◽  
A. J. Huisman ◽  
U. K. Krieger ◽  
Y. Rudich ◽  
C. Marcolli ◽  
...  
Keyword(s):  
Water Uptake ◽  
Condensed Phase ◽  
Organic Aerosol ◽  
Ice Nucleation ◽  
Water Diffusion ◽  
Fast Diffusion ◽  
Tropical Tropopause ◽  
Phase Water ◽  
Very High ◽  
Heterogeneous Ice Nucleation

Abstract. New measurements of water diffusion in secondary organic aerosol (SOA) material produced by oxidation of α-pinene and in a number of organic/inorganic model mixtures (3-methylbutane-1,2,3-tricarboxylic acid (3-MBTCA), levoglucosan, levoglucosan/NH4HSO4, raffinose) are presented. These indicate that water diffusion coefficients are determined by several properties of the aerosol substance and cannot be inferred from the glass transition temperature or bouncing properties. Our results suggest that water diffusion in SOA particles is faster than often assumed and imposes no significant kinetic limitation on water uptake and release at temperatures above 220 K. The fast diffusion of water suggests that heterogeneous ice nucleation on a glassy core is very unlikely in these systems. At temperatures below 220 K, model simulations of SOA particles suggest that heterogeneous ice nucleation may occur in the immersion mode on glassy cores which remain embedded in a liquid shell when experiencing fast updraft velocities. The particles absorb significant quantities of water during these updrafts which plasticize their outer layers such that these layers equilibrate readily with the gas phase humidity before the homogeneous ice nucleation threshold is reached. Glass formation is thus unlikely to restrict homogeneous ice nucleation. Only under most extreme conditions near the very high tropical tropopause may the homogeneous ice nucleation rate coefficient be reduced as a consequence of slow condensed-phase water diffusion. Since the differences between the behavior limited or non limited by diffusion are small even at the very high tropical tropopause, condensed-phase water diffusivity is unlikely to have significant consequences on the direct climatic effects of SOA particles under tropospheric conditions.

scholarly journals Modelling the effect of condensed-phase diffusion on the homogeneous nucleation of ice in ultra-viscous particles

2020 ◽  
Vol 20 (2) ◽  
pp. 683-698 ◽  
Author(s):  
Kathryn Fowler ◽  
Paul Connolly ◽  
David Topping
Keyword(s):  
Aerosol Particle ◽  
Condensed Phase ◽  
Homogeneous Nucleation ◽  
Aerosol Particles ◽  
Organic Aerosol ◽  
Ice Nucleation ◽  
Cloud Formation ◽  
Water Volume ◽  
Climate Modelling ◽  
Phase Diffusion

Abstract. Computational models of cloud formation typically use homogeneous nucleation to predict the ice nucleated in supercooled water. However, the existence of ultra-viscous organic aerosol in the upper troposphere has offered alternative ice nucleation pathways, which have been observed in laboratory studies. The possible effects of aerosol viscosity on cloud microphysical properties have traditionally been interpreted from simple model simulations of an individual aerosol particle based on equilibration timescales. In this study, to gain insight into the formation of ice in an ensemble of ultra-viscous aerosol particles, we have developed the first cloud parcel model with bin microphysics to simulate condensed phase diffusion through each individual aerosol particle. Our findings demonstrate, for the first time, the complex relationship between the rate of ice formation and the viscosity of secondary organic aerosol, driven by two competing effects – which cannot be explained using existing modelling approaches. The first is inhibition of homogeneous ice nucleation below 200 K, due to restricted particle growth and low water volume. The second occurs at temperatures between 200 and 220 K, where water molecules are slightly more mobile, and a layer of water condenses on the outside of the particle, causing an increase in the number of frozen aerosol particles. Our new model provides a basis to better understand and simulate ice cloud formation on a larger scale, addressing a major source of uncertainty in climate modelling through the representation of microphysical cloud processes.

scholarly journals Competition between water uptake and ice nucleation by glassy organic aerosol particles

2014 ◽  
Vol 14 (11) ◽  
pp. 16451-16492 ◽  
Author(s):  
T. Berkemeier ◽  
M. Shiraiwa ◽  
U. Pöschl ◽  
T. Koop
Keyword(s):  
Aerosol Particles ◽  
Liquid Core ◽  
Organic Aerosol ◽  
Ice Nucleation ◽  
Empirical Method ◽  
Water Diffusion ◽  
Cloud Formation ◽  
Atmospheric Conditions ◽  
Cloud Droplets ◽  
Organic Particles

Abstract. Organic aerosol particles play a key role in climate by serving as nuclei for clouds and precipitation. Their sources and composition are highly variable, and their phase state ranges from liquid to solid under atmospheric conditions, affecting the pathway of activation to cloud droplets and ice crystals. Due to slow diffusion of water in the particle phase, organic particles may deviate in phase and morphology from their thermodynamic equilibrium state, hampering the prediction of their influence on cloud formation. We overcome this problem by combining a novel semi-empirical method for estimation of water diffusivity with a kinetic flux model that explicitly treats water diffusion. We estimate timescales for particle deliquescence as well as various ice nucleation pathways for a wide variety of organic substances, including secondary organic aerosol (SOA) from the oxidation of isoprene, α-pinene, naphthalene, and dodecane. The simulations show that in typical atmospheric updrafts, glassy states and solid/liquid core-shell morphologies can persist for long enough that heterogeneous ice nucleation in the deposition and immersion mode can dominate over homogeneous ice nucleation. Such competition depends strongly on ambient temperature and relative humidity as well as humidification rates and particle sizes. Due to relatively high glass transition temperature and low hygroscopicity, naphthalene SOA particles have a higher potential to act as heterogeneous ice nuclei than the other investigated substances. Our findings demonstrate that kinetic limitations of water diffusion into organic aerosol particles strongly affect their ice nucleation pathways and require advanced formalisms for the description of ice cloud formation in atmospheric models.

scholarly journals Competition between water uptake and ice nucleation by glassy organic aerosol particles

2014 ◽  
Vol 14 (22) ◽  
pp. 12513-12531 ◽  
Author(s):  
T. Berkemeier ◽  
M. Shiraiwa ◽  
U. Pöschl ◽  
T. Koop
Keyword(s):  
Particle Size ◽  
Relative Humidity ◽  
Molecular Diffusion ◽  
Aerosol Particles ◽  
Liquid Core ◽  
Organic Aerosol ◽  
Ice Nucleation ◽  
Water Diffusion ◽  
Cloud Formation ◽  
Atmospheric Conditions

Abstract. Organic aerosol particles play a key role in climate by serving as nuclei for clouds and precipitation. Their sources and composition are highly variable, and their phase state ranges from liquid to solid under atmospheric conditions, affecting the pathway of activation to cloud droplets and ice crystals. Due to slow diffusion of water in the particle phase, organic particles may deviate in phase and morphology from their thermodynamic equilibrium state, hampering the prediction of their influence on cloud formation. We overcome this problem by combining a novel semi-empirical method for estimation of water diffusivity with a kinetic flux model that explicitly treats water diffusion. We estimate timescales for particle deliquescence as well as various ice nucleation pathways for a wide variety of organic substances, including secondary organic aerosol (SOA) from the oxidation of isoprene, α-pinene, naphthalene, and dodecane. The simulations show that, in typical atmospheric updrafts, glassy states and solid/liquid core-shell morphologies can persist for long enough that heterogeneous ice nucleation in the deposition and immersion mode can dominate over homogeneous ice nucleation. Such competition depends strongly on ambient temperature and relative humidity as well as humidification rate and particle size. Due to differences in glass transition temperature, hygroscopicity and atomic O / C ratio of the different SOA, naphthalene SOA particles have the highest potential to act as heterogeneous ice nuclei. Our findings demonstrate that kinetic limitations of water diffusion into organic aerosol particles are likely to be encountered under atmospheric conditions and can strongly affect ice nucleation pathways. For the incorporation of ice nucleation by organic aerosol particles into atmospheric models, our results demonstrate a demand for model formalisms that account for the effects of molecular diffusion and not only describe ice nucleation onsets as a function of temperature and relative humidity but also include updraft velocity, particle size and composition.

scholarly journals Shining New Light on the Kinetics of Water Uptake by Organic Aerosol Particles

2021 ◽  
Author(s):  
Matus E. Diveky ◽  
Michael J. Gleichweit ◽  
Sandra Roy ◽  
Ruth Signorell
Keyword(s):  
Water Uptake ◽  
Aerosol Particles ◽  
Organic Aerosol ◽  
Kinetics Of

scholarly journals Measurements of Ice Nucleating Particles and Ice Residuals

2017 ◽  
Vol 58 ◽  
pp. 8.1-8.13 ◽  
Author(s):  
Daniel J. Cziczo ◽  
Luis Ladino ◽  
Yvonne Boose ◽  
Zamin A. Kanji ◽  
Piotr Kupiszewski ◽  
...  
Keyword(s):  
Electron Microscope ◽  
Condensed Phase ◽  
Atmospheric Aerosols ◽  
Aerosol Particles ◽  
Ice Crystals ◽  
Ice Formation ◽  
Similar Amount ◽  
Residual Material ◽  
History Of ◽  
Phase Water

Abstract It has been known that aerosol particles act as nuclei for ice formation for over a century and a half (see Dufour). Initial attempts to understand the nature of these ice nucleating particles were optical and electron microscope inspection of inclusions at the center of a crystal (see Isono; Kumai). Only within the last few decades has instrumentation to extract ice crystals from clouds and analyze the residual material after sublimation of condensed-phase water been available (see Cziczo and Froyd). Techniques to ascertain the ice nucleating potential of atmospheric aerosols have only been in place for a similar amount of time (see DeMott et al.). In this chapter the history of measurements of ice nucleating particles, both in the field and complementary studies in the laboratory, are reviewed. Remaining uncertainties and artifacts associated with measurements are described and suggestions for future areas of improvement are made.

scholarly journals Simulating the influence of primary biological aerosol particles on clouds by heterogeneous ice nucleation

2018 ◽  
Vol 18 (20) ◽  
pp. 15437-15450 ◽  
Author(s):  
Matthias Hummel ◽  
Corinna Hoose ◽  
Bernhard Pummer ◽  
Caroline Schaupp ◽  
Janine Fröhlich-Nowoisky ◽  
...  
Keyword(s):  
Pseudomonas Syringae ◽  
Aerosol Particles ◽  
Fungal Spores ◽  
Ice Nucleation ◽  
Ice Crystals ◽  
Atmospheric Measurements ◽  
Cloud Ice ◽  
Biological Aerosol Particles ◽  
Ice Phase ◽  
Heterogeneous Ice Nucleation

Abstract. Primary ice formation, which is an important process for mixed-phase clouds with an impact on their lifetime, radiative balance, and hence the climate, strongly depends on the availability of ice-nucleating particles (INPs). Supercooled droplets within these clouds remain liquid until an INP immersed in or colliding with the droplet reaches its activation temperature. Only a few aerosol particles are acting as INPs and the freezing efficiency varies among them. Thus, the fraction of supercooled water in the cloud depends on the specific properties and concentrations of the INPs. Primary biological aerosol particles (PBAPs) have been identified as very efficient INPs at high subzero temperatures, but their very low atmospheric concentrations make it difficult to quantify their impact on clouds. Here we use the regional atmospheric model COSMO–ART to simulate the heterogeneous ice nucleation by PBAPs during a 1-week case study on a domain covering Europe. We focus on three highly ice-nucleation-active PBAP species, Pseudomonas syringae bacteria cells and spores from the fungi Cladosporium sp. and Mortierella alpina. PBAP emissions are parameterized in order to represent the entirety of bacteria and fungal spores in the atmosphere. Thus, only parts of the simulated PBAPs are assumed to act as INPs. The ice nucleation parameterizations are specific for the three selected species and are based on a deterministic approach. The PBAP concentrations simulated in this study are within the range of previously reported results from other modeling studies and atmospheric measurements. Two regimes of PBAP INP concentrations are identified: a temperature-limited and a PBAP-limited regime, which occur at temperatures above and below a maximal concentration at around −10 ∘C, respectively. In an ensemble of control and disturbed simulations, the change in the average ice crystal concentration by biological INPs is not statistically significant, suggesting that PBAPs have no significant influence on the average state of the cloud ice phase. However, if the cloud top temperature is below −15 ∘C, PBAP can influence the cloud ice phase and produce ice crystals in the absence of other INPs. Nevertheless, the number of produced ice crystals is very low and it has no influence on the modeled number of cloud droplets and hence the cloud structure.

scholarly journals Heterogeneous ice nucleation of viscous secondary organic aerosol produced from ozonolysis of <i>α</i>-pinene

2016 ◽  
Vol 16 (10) ◽  
pp. 6495-6509 ◽  
Author(s):  
Karoliina Ignatius ◽  
Thomas B. Kristensen ◽  
Emma Järvinen ◽  
Leonid Nichman ◽  
Claudia Fuchs ◽  
...  
Keyword(s):  
Secondary Organic Aerosol ◽  
Solid Phase ◽  
Particle Surface ◽  
Amorphous Solid ◽  
Organic Aerosol ◽  
Ice Nucleation ◽  
Cloud Formation ◽  
Particle Surface Area ◽  
Semi Solid ◽  
Heterogeneous Ice Nucleation

Abstract. There are strong indications that particles containing secondary organic aerosol (SOA) exhibit amorphous solid or semi-solid phase states in the atmosphere. This may facilitate heterogeneous ice nucleation and thus influence cloud properties. However, experimental ice nucleation studies of biogenic SOA are scarce. Here, we investigated the ice nucleation ability of viscous SOA particles. The SOA particles were produced from the ozone initiated oxidation of α-pinene in an aerosol chamber at temperatures in the range from −38 to −10 °C at 5–15 % relative humidity with respect to water to ensure their formation in a highly viscous phase state, i.e. semi-solid or glassy. The ice nucleation ability of SOA particles with different sizes was investigated with a new continuous flow diffusion chamber. For the first time, we observed heterogeneous ice nucleation of viscous α-pinene SOA for ice saturation ratios between 1.3 and 1.4 significantly below the homogeneous freezing limit. The maximum frozen fractions found at temperatures between −39.0 and −37.2 °C ranged from 6 to 20 % and did not depend on the particle surface area. Global modelling of monoterpene SOA particles suggests that viscous biogenic SOA particles are indeed present in regions where cirrus cloud formation takes place. Hence, they could make up an important contribution to the global ice nucleating particle budget.

scholarly journals Heterogeneous Ice Nucleation on Simulated Secondary Organic Aerosol

2014 ◽  
Vol 48 (3) ◽  
pp. 1675-1682 ◽  
Author(s):  
Gregory P. Schill ◽  
David O. De Haan ◽  
Margaret A. Tolbert
Keyword(s):  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Ice Nucleation ◽  
Heterogeneous Ice Nucleation

scholarly journals Heterogeneous ice nucleation of viscous secondary organic aerosol produced from ozonolysis of α-pinene

2015 ◽  
Vol 15 (24) ◽  
pp. 35719-35752 ◽  
Author(s):  
K. Ignatius ◽  
T. B. Kristensen ◽  
E. Järvinen ◽  
L. Nichman ◽  
C. Fuchs ◽  
...  
Keyword(s):  
Secondary Organic Aerosol ◽  
Solid Phase ◽  
Particle Surface ◽  
Organic Aerosol ◽  
Ice Nucleation ◽  
Cloud Formation ◽  
Cirrus Cloud ◽  
Particle Surface Area ◽  
Semi Solid ◽  
Heterogeneous Ice Nucleation

Abstract. There are strong indications that particles containing secondary organic aerosol (SOA) exhibit amorphous solid or semi-solid phase states in the atmosphere. This may facilitate deposition ice nucleation and thus influence cirrus cloud properties. However, experimental ice nucleation studies of biogenic SOA are scarce. Here, we investigated the ice nucleation ability of viscous SOA particles. The SOA particles were produced from the ozone initiated oxidation of α-pinene in an aerosol chamber at temperatures in the range from −38 to −10 °C at 5–15 % relative humidity with respect to water to ensure their formation in a highly viscous phase state, i.e. semi-solid or glassy. The ice nucleation ability of SOA particles with different sizes was investigated with a new continuous flow diffusion chamber. For the first time, we observed heterogeneous ice nucleation of viscous α-pinene SOA in the deposition mode for ice saturation ratios between 1.3 and 1.4 significantly below the homogeneous freezing limit. The maximum frozen fractions found at temperatures between −36.5 and −38.3 °C ranged from 6 to 20 % and did not depend on the particle surface area. Global modelling of monoterpene SOA particles suggests that viscous biogenic SOA particles are indeed present in regions where cirrus cloud formation takes place. Hence, they could make up an important contribution to the global ice nuclei (IN) budget.

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