scholarly journals Condensed-phase biogenic–anthropogenic interactions with implications for cold cloud formation

2017 ◽  
Vol 200 ◽  
pp. 165-194 ◽  
Author(s):  
Joseph C. Charnawskas ◽  
Peter A. Alpert ◽  
Andrew T. Lambe ◽  
Thomas Berkemeier ◽  
Rachel E. O’Brien ◽  
...  
Keyword(s):  
Freezing Temperature ◽  
Organic Aerosol ◽  
Ice Nucleation ◽  
Mixed Phase ◽  
Cloud Formation ◽  
Fossil Fuel Combustion ◽  
Soot Particles ◽  
Ice Nuclei ◽  
Deliquescence Relative Humidity ◽  
Homogeneous Freezing

Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil fuel combustion can acquire a coating of SOA. We investigate SOA–soot biogenic–anthropogenic interactions and their impact on ice nucleation in relation to the particles’ organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without the presence of sulfate or soot particles. Corresponding particle glass transition (Tg) and full deliquescence relative humidity (FDRH) were estimated using a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfate mixtures exhibit a core–shell configuration (i.e.a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation, in agreement with respectiveTgand FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid, inducing ice nucleation. Naphthalene SOA coated soot particles acted as ice nuclei above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate renders this even less likely. However, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during pre-industrial times or in pristine areas.

scholarly journals Insights into the role of soot aerosols in cirrus cloud formation

2007 ◽  
Vol 7 (16) ◽  
pp. 4203-4227 ◽  
Author(s):  
B. Kärcher ◽  
O. Möhler ◽  
P. J. DeMott ◽  
S. Pechtl ◽  
F. Yu
Keyword(s):  
Environmental Parameters ◽  
Supercooled Liquid ◽  
Critical Discussion ◽  
Cloud Formation ◽  
Cirrus Cloud ◽  
Atmospheric Conditions ◽  
Soot Particles ◽  
Ice Nuclei ◽  
Homogeneous Freezing

Abstract. Cirrus cloud formation is believed to be dominated by homogeneous freezing of supercooled liquid aerosols in many instances. Heterogeneous ice nuclei such as mineral dust, metallic, and soot particles, and some crystalline solids within partially soluble aerosols are suspected to modulate cirrus properties. Among those, the role of ubiquitous soot particles is perhaps the least understood. Because aviation is a major source of upper tropospheric soot particles, we put emphasis on ice formation in dispersing aircraft plumes. The effect of aircraft soot on cirrus formation in the absence of contrails is highly complex and depends on a wide array of emission and environmental parameters. We use a microphysical-chemical model predicting the formation of internally mixed, soot-containing particles up to two days after emission, and suggest two principal scenarios: high concentrations of original soot emissions could slightly increase the number of ice crystals; low concentrations of particles originating from coagulation of emitted soot with background aerosols could lead to a significant reduction in ice crystal number. Both scenarios assume soot particles to be moderate ice nuclei relative to cirrus formation by homogeneous freezing in the presence of few efficient dust ice nuclei. A critical discussion of laboratory experiments reveals that the ice nucleation efficiency of soot particles depends strongly on their source, and, by inference, on atmospheric aging processes. Mass and chemistry of soluble surface coatings appear to be crucial factors. Immersed soot particles tend to be poor ice nuclei, some bare ones nucleate ice at low supersaturations. However, a fundamental understanding of these studies is lacking, rendering extrapolations to atmospheric conditions speculative. In particular, we cannot yet decide which indirect aircraft effect scenario is more plausible, and options suggested to mitigate the problem remain uncertain.

scholarly journals The deposition ice nucleation and immersion freezing potential of amorphous secondary organic aerosol: Pathways for ice and mixed-phase cloud formation

2012 ◽  
Vol 117 (D16) ◽  
pp. n/a-n/a ◽  
Author(s):  
Bingbing Wang ◽  
Andrew T. Lambe ◽  
Paola Massoli ◽  
Timothy B. Onasch ◽  
Paul Davidovits ◽  
...  
Keyword(s):  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Ice Nucleation ◽  
Mixed Phase ◽  
Cloud Formation ◽  
Immersion Freezing ◽  
Freezing Potential

scholarly journals On the ice nucleation spectrum

2011 ◽  
Vol 11 (11) ◽  
pp. 29601-29646 ◽  
Author(s):  
D. Barahona
Keyword(s):  
Surface Composition ◽  
Ice Nucleation ◽  
Atmospheric Modeling ◽  
Cloud Formation ◽  
Volume Distribution ◽  
Ice Crystal ◽  
Ice Nuclei ◽  
New Formulation ◽  
Homogeneous Freezing ◽  
Heterogeneous Ice Nucleation

Abstract. This work presents a novel formulation of the ice nucleation spectrum, i.e. the function relating the ice crystal concentration to cloud formation conditions and aerosol properties. The new formulation relies on a statistical view of the ice nucleation process and explicitly accounts for the dependency of the ice crystal concentration on temperature, supersaturation, cooling rate, and particle size, and, in the case of heterogeneous ice nucleation, on the distributions of particle area and surface composition. The new formulation is used to generate ice nucleation parameterizations for the homogeneous freezing of cloud droplets and the heterogeneous deposition ice nucleation on dust and soot ice nuclei. For homogeneous freezing, it was found that by increasing the dispersion in the droplet volume distribution the fraction of supercooled droplets in the population increases. For heterogeneous ice nucleation it was found that ice nucleation on efficient ice nuclei (IN) shows features consistent with the singular hypothesis (characterized by a lack of temporal dependency of the ice nucleation spectrum) whereas less efficient IN tend to display stochastic behavior. Analysis of empirical nucleation spectra suggested that inferring the aerosol heterogeneous ice nucleation properties from measurements of the onset supersaturation and temperature may carry significant error as the variability in ice nucleation properties within the aerosol population is not accounted for. This work provides a simple and rigorous ice nucleation framework were theoretical predictions, laboratory measurements and field campaign data can be reconciled, and that is suitable for application in atmospheric modeling studies.

scholarly journals Insights into the role of soot aerosols in cirrus cloud formation

2007 ◽  
Vol 7 (3) ◽  
pp. 7843-7905 ◽  
Author(s):  
B. Kärcher ◽  
O. Möhler ◽  
P. J. DeMott ◽  
S. Pechtl ◽  
F. Yu
Keyword(s):  
Environmental Parameters ◽  
Supercooled Liquid ◽  
Critical Discussion ◽  
Cloud Formation ◽  
Cirrus Cloud ◽  
Atmospheric Conditions ◽  
Soot Particles ◽  
Ice Nuclei ◽  
Homogeneous Freezing

Abstract. Cirrus cloud formation is believed to be domi\\-nated by homogeneous freezing of supercooled liquid aerosols in many instances. Heterogeneous ice nuclei such as mineral dust, metallic, and soot particles, and some crystalline solids within partially soluble aerosols are suspected to modulate cirrus properties. Among those, the role of ubiqui\\-tous soot particles is perhaps the least understood. Because aviation is a major source of upper tropospheric soot particles, we put emphasis on ice formation in dispersing aircraft plumes. The effect of aircraft soot on cirrus formation in the absence of contrails is highly complex and depends on a wide array of emission and environmental parameters. We use a microphysical-chemical model predicting the formation of internally mixed, soot-containing particles up to two days after emission, and suggest two principal scenarios, both assuming soot particles to be moderate ice nuclei relative to cirrus formation by homogeneous freezing in the presence of few efficient dust ice nuclei: high concentrations of original soot emissions could slightly increase the number of ice crystals; low concentrations of particles originating from coagulation of emitted soot with background aerosols could lead to a significant reduction in ice crystal number. A critical discussion of laboratory experiments reveals that the ice nucleation efficiency of soot particles depends strongly on their source, and, by inference, on atmospheric aging processes. Mass and chemistry of soluble surface coatings appear to be crucial factors. Immersed soot particles tend to be poor ice nuclei, some bare ones nucleate ice at low supersaturations. However, a fundamental understanding of these studies is lacking, rendering extrapolations to atmospheric conditions speculative. In particular, we cannot yet decide which indirect aircraft effect scenario is more plausible, and options suggested to mitigate the problem remain uncertain.

scholarly journals Ice nucleation properties of volcanic ash from Eyjafjallajökull

2011 ◽  
Vol 11 (6) ◽  
pp. 17201-17243 ◽  
Author(s):  
C. R. Hoyle ◽  
V. Pinti ◽  
A. Welti ◽  
B. Zobrist ◽  
C. Marcolli ◽  
...  
Keyword(s):  
Volcanic Ash ◽  
Freezing Point ◽  
Ice Nucleation ◽  
Cloud Formation ◽  
Atmospheric Conditions ◽  
Model Calculations ◽  
Airborne Measurements ◽  
Ice Cloud ◽  
Ice Nuclei ◽  
Homogeneous Freezing

Abstract. The ice nucleation ability of volcanic ash particles collected close to the Icelandic volcano Eyjafjallajökull during its eruptions in April and May 2010 is investigated experimentally, in the immersion and deposition modes, and applied to atmospheric conditions by comparison with airborne measurements and microphysical model calculations. The number of ash particles which are active as ice nuclei (IN) is strongly temperature dependent, with a very small minority being active in the immersion mode at temperatures of 250–263 K. Average ash particles show only a moderate effect on ice nucleation, by inducing freezing at temperatures between 236 K and 240 K (i.e. approximately 3–4 K higher than temperatures required for homogeneous ice nucleation, measured with the same instrument). By scaling the results to aircraft and lidar measurements of the conditions in the ash plume days down wind of the eruption and by applying a simple microphysical model, it was found that the IN active in the immersion mode in the range 250–263 K generally occurred in atmospheric number densities at the lower end of those required to have an impact on ice cloud formation. However, 3–4 K above the homogeneous freezing point, immersion mode IN number densities a few days down wind of the eruption were sufficiently high to have a moderate influence on ice cloud formation. The efficiency of IN in the deposition mode was found to be poor except at very cold conditions (< 238 K), when they reach an efficiency similar to that of mineral dust with the onset of freezing at 10 % supersaturation with respect to ice, and with the frozen fraction nearing its maximum value at a supersaturation 20 %. In summary, these investigations suggest volcanic ash particles to have only moderate effects on atmospheric ice formation.

scholarly journals The effects of hygroscopicity of fossil fuel combustion aerosols on mixed-phase clouds

2012 ◽  
Vol 12 (8) ◽  
pp. 19987-20006
Author(s):  
Y. Yun ◽  
J. E. Penner ◽  
O. Popovicheva
Keyword(s):  
Fossil Fuel ◽  
Laboratory Data ◽  
Ice Nucleation ◽  
Mixed Phase ◽  
Liquid Water Path ◽  
Anthropogenic Forcing ◽  
Soot Particles ◽  
Cloud Forcing ◽  
Ice Nuclei ◽  
Mixed Phase Clouds

Abstract. Fossil fuel black carbon and organic matter (ffBC/OM) are often emitted together with sulfate, which coats the surface of these particles and changes their hygroscopicity. Observational studies show that the hygroscopicity of soot particles can modulate their ice nucleation ability. To address this, we implemented a scheme that uses 3 levels of soot hygroscopicity (hydrophobic, hydrophilic and hygroscopic) and used laboratory data to specify their ice nuclei abilities. The new scheme results in significant changes to anthropogenic forcing in mixed-phase clouds. The net forcing in off-line studies varies from 0.111 to 1.059 W m−2 depending on the ice nucleation capability of hygroscopic soot particles. The total anthropogenic cloud forcing and whole-sky forcing with the new scheme is 0.06 W m−2 and −2.45 W m−2, respectively, but could be more positive if hygroscopic soot particles are allowed to nucleate ice particles. The change in liquid water path dominates the anthropogenic forcing in mixed-phase clouds.

scholarly journals Ice nucleation properties of volcanic ash from Eyjafjallajökull

2011 ◽  
Vol 11 (18) ◽  
pp. 9911-9926 ◽  
Author(s):  
C. R. Hoyle ◽  
V. Pinti ◽  
A. Welti ◽  
B. Zobrist ◽  
C. Marcolli ◽  
...  
Keyword(s):  
Volcanic Ash ◽  
Freezing Point ◽  
Ice Nucleation ◽  
Cloud Formation ◽  
Atmospheric Conditions ◽  
Model Calculations ◽  
Airborne Measurements ◽  
Ice Cloud ◽  
Ice Nuclei ◽  
Homogeneous Freezing

Abstract. The ice nucleation ability of volcanic ash particles collected close to the Icelandic volcano Eyjafjallajökull during its eruptions in April and May 2010 is investigated experimentally, in the immersion and deposition modes, and applied to atmospheric conditions by comparison with airborne measurements and microphysical model calculations. The number of ash particles which are active as ice nuclei (IN) is strongly temperature dependent, with a very small minority being active in the immersion mode at temperatures of 250–263 K. Average ash particles show only a moderate effect on ice nucleation, by inducing freezing at temperatures between 236 K and 240 K (i.e. approximately 3–4 K higher than temperatures required for homogeneous ice nucleation, measured with the same instrument). By scaling the results to aircraft and lidar measurements of the conditions in the ash plume days down wind of the eruption, and by applying a simple microphysical model, it was found that the IN active in the immersion mode in the range 250–263 K generally occurred in atmospheric number densities at the lower end of those required to have an impact on ice cloud formation. However, 3–4 K above the homogeneous freezing point, immersion mode IN number densities a few days down wind of the eruption were sufficiently high to have a moderate influence on ice cloud formation. The efficiency of IN in the deposition mode was found to be poor except at very cold conditions (<238 K), when they reach an efficiency similar to that of mineral dust with the onset of freezing at 10 % supersaturation with respect to ice, and with the frozen fraction nearing its maximum value at a supersaturation 20 %. In summary, these investigations suggest volcanic ash particles to have only moderate effects on atmospheric ice formation.

scholarly journals Ice nucleation abilities of soot particles determined with the Horizontal Ice Nucleation Chamber

2018 ◽  
Vol 18 (18) ◽  
pp. 13363-13392 ◽  
Author(s):  
Fabian Mahrt ◽  
Claudia Marcolli ◽  
Robert O. David ◽  
Philippe Grönquist ◽  
Eszter J. Barthazy Meier ◽  
...  
Keyword(s):  
Particle Size ◽  
Water Saturation ◽  
Particle Surface ◽  
Water Vapor Sorption ◽  
Contact Angles ◽  
Ice Nucleation ◽  
Particle Surface Area ◽  
Soot Particles ◽  
Microphysical Properties ◽  
Homogeneous Freezing

Abstract. Ice nucleation by different types of soot particles is systematically investigated over the temperature range from 218 to 253 K relevant for both mixed-phase (MPCs) and cirrus clouds. Soot types were selected to represent a range of physicochemical properties associated with combustion particles. Their ice nucleation ability was determined as a function of particle size using relative humidity (RH) scans in the Horizontal Ice Nucleation Chamber (HINC). We complement our ice nucleation results by a suite of particle characterization measurements, including determination of particle surface area, fractal dimension, temperature-dependent mass loss (ML), water vapor sorption and inferred porosity measurements. Independent of particle size, all soot types reveal absence of ice nucleation below and at water saturation in the MPC regime (T>235 K). In the cirrus regime (T≤235 K), soot types show different freezing behavior depending on particle size and soot type, but the freezing is closely linked to the soot particle properties. Specifically, our results suggest that if soot aggregates contain mesopores (pore diameters of 2–50 nm) and have sufficiently low water–soot contact angles, they show ice nucleation activity and can contribute to ice formation in the cirrus regime at RH well below homogeneous freezing of solution droplets. We attribute the observed ice nucleation to a pore condensation and freezing (PCF) mechanism. Nevertheless, soot particles without cavities of the right size and/or too-high contact angles nucleate ice only at or well above the RH required for homogeneous freezing conditions of solution droplets. Thus, our results imply that soot particles able to nucleate ice via PCF could impact the microphysical properties of ice clouds.

scholarly journals Ice nucleation efficiency of AgI: review and new insights

2016 ◽  
Author(s):  
Claudia Marcolli ◽  
Baban Nagare ◽  
André Welti ◽  
Ulrike Lohmann
Keyword(s):  
Water Saturation ◽  
Experimental Studies ◽  
Freezing Temperature ◽  
Nucleating Agent ◽  
Companion Paper ◽  
Chem Phys ◽  
Ice Nucleation ◽  
Lattice Match ◽  
Ice Nuclei ◽  
Immersion Freezing

Abstract. AgI is one of the best investigated ice nuclei. It has relevance for the atmosphere since it is used for glaciogenic cloud seeding. Theoretical and experimental studies over the last sixty years provide a complex picture of silver iodide as ice nucleating agent with conflicting and inconsistent results. This review compares experimental ice nucleation studies in order to analyse the factors that influence the ice nucleation ability of AgI. We have performed experiments to compare contact and immersion freezing by AgI. This is one of three papers that describe and analyse contact and immersion freezing experiments with AgI. In Nagare et al. (Nagare, B., Marcolli, C., Stetzer, O., and Lohmann, U.: Comparison of measured and calculated collision efficiencies at low temperatures, Atmos. Chem. Phys., 15, 13759–13776, doi:10.5194/acp-15-13759-2015, 2015) collision efficiencies based on contact freezing experiments with AgI are determined and compared with theoretical formulations. In a companion paper, contact freezing experiments are compared with immersion freezing experiments conducted with AgI, kaolinite, and ATD as ice nuclei. The following picture emerges from this analysis: The ice nucleation ability of AgI seems to be enhanced when the AgI particle is on the surface of a droplet, which is indeed the position that a particle takes when it can freely move in a droplet. Ice nucleation by particles with surfaces exposed to air, depends on water adsorption. AgI surfaces seem to be most efficient as ice nuclei when they are exposed to relative humidity at or even above water saturation. For AgI particles that are totally immersed in water, the freezing temperature increases with increasing AgI surface area. Higher threshold freezing temperature seem to correlate with improved lattice matches as can be seen for AgI-AgCl solid solutions and 3AgI•NH4I•6H2O, which have slightly better lattice matches with ice than AgI and also higher threshold freezing temperatures. However, the effect of a good lattice match is annihilated when the surfaces have charges. Also, the ice nucleation ability seems to decrease during dissolution of AgI particles. This introduces an additional history and time dependence of ice nucleation in cloud chambers with short residence times.

scholarly journals Discrimination of water, ice and aerosols by light polarisation in the CLOUD experiment

2015 ◽  
Vol 15 (21) ◽  
pp. 31433-31469 ◽  
Author(s):  
L. Nichman ◽  
C. Fuchs ◽  
E. Järvinen ◽  
K. Ignatius ◽  
N. F. Höppel ◽  
...  
Keyword(s):  
General Circulation ◽  
Simultaneous Detection ◽  
Organic Aerosol ◽  
General Circulation Models ◽  
Mixed Phase ◽  
Cloud Formation ◽  
Potential Contribution ◽  
Particle Size Range ◽  
Cloud Particle ◽  
Small Cloud

Abstract. Cloud microphysical processes involving the ice phase in tropospheric clouds are among the major uncertainties in cloud formation, weather and General Circulation Models (GCMs). The simultaneous detection of aerosol particles, liquid droplets, and ice crystals, especially in the small cloud-particle size range below 50 μm, remains challenging in mixed phase, often unstable ice-water phase environments. The Cloud Aerosol Spectrometer with Polarisation (CASPOL) is an airborne instrument that has the ability to detect such small cloud particles and measure their effects on the backscatter polarisation state. Here we operate the versatile Cosmics-Leaving-OUtdoor-Droplets (CLOUD) chamber facility at the European Organisation for Nuclear Research (CERN) to produce controlled mixed phase and other clouds by adiabatic expansions in an ultraclean environment, and use the CASPOL to discriminate between different aerosols, water and ice particles. In this paper, optical property measurements of mixed phase clouds and viscous Secondary Organic Aerosol (SOA) are presented. We report observations of significant liquid – viscous SOA particle polarisation transitions under dry conditions using CASPOL. Cluster analysis techniques were subsequently used to classify different types of particles according to their polarisation ratios during phase transition. A classification map is presented for water droplets, organic aerosol (e.g., SOA and oxalic acid), crystalline substances such as ammonium sulphate, and volcanic ash. Finally, we discuss the benefits and limitations of this classification approach for atmospherically relevant concentration and mixtures with respect to the CLOUD 8–9 campaigns and its potential contribution to Tropical Troposphere Layer (TTL) analysis.

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