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Title: A water activity based model of heterogeneous ice nucleation kinetics for freezing of water and aqueous solution droplets

Journal Article · · Faraday Discussions
DOI:https://doi.org/10.1039/C3FD00035D· OSTI ID:1349435
 [1];  [1]
  1. Stony Brook Univ., Stony Brook, NY (United States)

Immersion freezing of water and aqueous solutions by particles acting as ice nuclei (IN) is a common process of heterogeneous ice nucleation which occurs in many environments, especially in the atmosphere where it results in the glaciation of clouds. Here we experimentally show, using a variety of IN types suspended in various aqueous solutions, that immersion freezing temperatures and kinetics can be described solely by temperature, T, and solution water activity, aw, which is the ratio of the vapour pressure of the solution and the saturation water vapour pressure under the same conditions and, in equilibrium, equivalent to relative humidity (RH). This allows the freezing point and corresponding heterogeneous ice nucleation rate coefficient, Jhet, to be uniquely expressed by T and aw, a result we term the aw based immersion freezing model (ABIFM). This method is independent of the nature of the solute and accounts for several varying parameters, including cooling rate and IN surface area, while providing a holistic description of immersion freezing and allowing prediction of freezing temperatures, Jhet, frozen fractions, ice particle production rates and numbers. Our findings are based on experimental freezing data collected for various IN surface areas, A, and cooling rates, r, of droplets variously containing marine biogenic material, two soil humic acids, four mineral dusts, and one organic monolayer acting as IN. For all investigated IN types we demonstrate that droplet freezing temperatures increase as A increases. Similarly, droplet freezing temperatures increase as the cooling rate decreases. The log10(Jhet) values for the various IN types derived exclusively by T and aw, provide a complete description of the heterogeneous ice nucleation kinetics. Thus, the ABIFM can be applied over the entire range of T, RH, total particulate surface area, and cloud activation timescales typical of atmospheric conditions. Finally, we demonstrate that ABIFM can be used to derive frozen fractions of droplets and ice particle production for atmospheric models of cirrus and mixed phase cloud conditions.

Research Organization:
Stony Brook Univ., NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
Grant/Contract Number:
SC0008613
OSTI ID:
1349435
Journal Information:
Faraday Discussions, Vol. 165; ISSN 1359-6640
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 77 works
Citation information provided by
Web of Science

References (90)

Eight Years of High Cloud Statistics Using HIRS journal January 1999
Trends in Global Cloud Cover in Two Decades of HIRS Observations journal August 2005
Cloud Microphysics and Climate journal May 1997
Small-scale cloud processes and climate journal January 2008
Advances in Understanding Clouds from ISCCP journal November 1999
Global modeling of mixed-phase clouds: The albedo and lifetime effects of aerosols journal January 2011
Predicting global atmospheric ice nuclei distributions and their impacts on climate journal June 2010
Long-term impacts of aerosols on the vertical development of clouds and precipitation journal November 2011
Impact of aerosols on convective clouds and precipitation: AEROSOL IMPACT ON CONVECTIVE CLOUDS journal April 2012
Nucleation in the atmosphere journal April 2009
Heterogeneous freezing of ammonium sulfate and sodium chloride solutions by long chain alcohols journal January 2006
Nucleation terminology journal January 1985
Upper-tropospheric relative humidity observations and implications for cirrus ice nucleation journal May 1998
The role of heterogeneous freezing nucleation in upper tropospheric clouds: Inferences from SUCCESS journal May 1998
African dust aerosols as atmospheric ice nuclei: AFRICAN DUST AEROSOLS AS ICE NUCLEI journal July 2003
In-situ observations of aerosol particles remaining from evaporated cirrus crystals: Comparing clean and polluted air masses journal January 2003
Freezing thresholds and cirrus cloud formation mechanisms inferred from in situ measurements of relative humidity journal January 2003
Single particle measurements of the chemical composition of cirrus ice residue during CRYSTAL-FACE: CHEMICAL COMPOSITION OF ICE RESIDUE journal February 2004
A Continuous-Flow Diffusion Chamber for Airborne Measurements of Ice Nuclei journal May 2001
Black carbon enrichment in atmospheric ice particle residuals observed in lower tropospheric mixed phase clouds journal January 2008
Chemical composition of ambient aerosol, ice residues and cloud droplet residues in mixed-phase clouds: single particle analysis during the Cloud and Aerosol Characterization Experiment (CLACE 6) journal January 2010
A large-eddy model for cirrus clouds with explicit aerosol and ice microphysics and Lagrangian ice particle tracking journal September 2010
Ice in Clouds Experiment–Layer Clouds. Part II: Testing Characteristics of Heterogeneous Ice Formation in Lee Wave Clouds journal March 2012
New Primary Ice-Nucleation Parameterizations in an Explicit Cloud Model journal July 1992
Nucleation Processes in Deep Convection Simulated by a Cloud-System-Resolving Model with Double-Moment Bulk Microphysics journal March 2007
Evolution of the ice phase in tropical altocumulus: SAMUM lidar observations over Cape Verde journal January 2009
A Classical-Theory-Based Parameterization of Heterogeneous Ice Nucleation by Mineral Dust, Soot, and Biological Particles in a Global Climate Model journal August 2010
Evidence that ice forms primarily in supercooled liquid clouds at temperatures > −27°C: ICE NUCLEATION IN MID-LEVEL CLOUDS journal July 2011
Water activity as the determinant for homogeneous ice nucleation in aqueous solutions journal August 2000
Freezing of HNO 3 /H 2 SO 4 /H 2 O Solutions at Stratospheric Temperatures:  Nucleation Statistics and Experiments journal February 1997
Homogeneous Ice Nucleation in Water and Aqueous Solutions journal November 2004
The homogeneous ice nucleation rate of water droplets produced in a microfluidic device and the role of temperature uncertainty journal January 2013
Parameterizations for ice nucleation in biological and atmospheric systems journal January 2009
Ice nucleation in aqueous solutions of poly[ethylene glycol] with different molar mass journal June 2003
Ice nucleation from aqueous NaCl droplets with and without marine diatoms journal January 2011
Homogeneous ice freezing temperatures and ice nucleation rates of aqueous ammonium sulfate and aqueous levoglucosan particles for relevant atmospheric conditions journal January 2009
Stimulation of ice nucleation by marine diatoms journal December 2010
Homogeneous Ice Nucleation From Aqueous Inorganic/Organic Particles Representative of Biomass Burning: Water Activity, Freezing Temperatures, Nucleation Rates journal February 2011
A parameterization of cirrus cloud formation: Homogeneous freezing of supercooled aerosols journal January 2002
A Parameterization of cirrus cloud formation: Homogeneous freezing including effects of aerosol size: CIRRUS PARAMETERIZATION journal December 2002
Physically based parameterization of cirrus cloud formation for use in global atmospheric models journal January 2006
Effects of ice nuclei on cirrus clouds in a global climate model journal January 2011
Inferring ice formation processes from global-scale black carbon profiles observed in the remote atmosphere and model simulations: INFERRING CLOUD ICE FORMATION PROCESSES journal December 2012
Thermodynamic Dissociation Constant of the Bisulfate Ion from Raman and Ion Interaction Modeling Studies of Aqueous Sulfuric Acid at Low Temperatures journal April 2003
Reply to “Comment on the ‘Thermodynamic Dissociation Constant of the Bisulfate Ion from Raman and Ion Interaction Modeling Studies of Aqueous Sulfuric Acid at Low Temperatures'” journal March 2005
A Thermodynamic Model of the System HCl-HNO3-H2SO4-H2O, Including Solubilities of HBr, from <200 to 328 K journal July 1995
Equilibrium Partial Pressures, Thermodynamic Properties of Aqueous and Solid Phases, and Cl 2 Production from Aqueous HCl and HNO 3 and Their Mixtures journal May 1999
Comment on the “Thermodynamic Dissociation Constant of the Bisulfate Ion from Raman and Ion Interaction Modeling Studies of Aqueous Sulfuric Acid at Low Temperatures” journal March 2005
Thermodynamic Model of the System H + −NH 4 + −SO 4 2- −NO 3 - −H 2 O at Tropospheric Temperatures journal March 1998
Oxalic acid as a heterogeneous ice nucleus in the upper troposphere and its indirect aerosol effect journal January 2006
Freezing of Water and Aqueous NaCl Droplets Coated by Organic Monolayers as a Function of Surfactant Properties and Water Activity journal June 2011
Microbiology and atmospheric processes: the role of biological particles in cloud physics journal January 2007
Heterogeneous ice nucleation on atmospheric aerosols: a review of results from laboratory experiments journal January 2012
Ice nucleation by particles immersed in supercooled cloud droplets journal January 2012
Phase Transitions of Aqueous Atmospheric Particles journal September 2000
Ice nucleation by surrogates for atmospheric mineral dust and mineral dust/sulfate particles at cirrus temperatures journal January 2005
Heterogeneous nucleation of ice on surrogates of mineral dust journal January 2006
Heterogeneous freezing of droplets with immersed mineral dust particles – measurements and parameterization journal January 2010
Time dependence of immersion freezing: an experimental study on size selected kaolinite particles journal January 2012
Ice nucleation efficiency of clay minerals in the immersion mode journal January 2012
Heterogeneous freezing of ice on atmospheric aerosols containing ash, soot, and soil journal January 2009
Immersion freezing of water and aqueous ammonium sulfate droplets initiated by humic-like substances as a function of water activity journal January 2013
Initiation of the ice phase by marine biogenic surfaces in supersaturated gas and supercooled aqueous phases journal January 2011
Ice Nucleation by Alcohols Arranged in Monolayers at the Surface of Water Drops journal November 1990
Preactivation in the nucleation of ice by Langmuir films of aliphatic alcohols journal June 2001
Internally mixed sulfate and organic particles as potential ice nuclei in the tropical tropopause region journal April 2010
Depositional ice nucleation on solid ammonium sulfate and glutaric acid particles journal January 2010
Importance of aerosol composition, mixing state, and morphology for heterogeneous ice nucleation: A combined field and laboratory approach: HETEROGENEOUS ICE NUCLEATION journal March 2012
Depositional Ice Nucleation on Monocarboxylic Acids: Effect of the O:C Ratio journal May 2012
The deposition ice nucleation and immersion freezing potential of amorphous secondary organic aerosol: Pathways for ice and mixed-phase cloud formation: ICE NUCLEATION BY AMORPHOUS SOA journal August 2012
Efficiency of immersion mode ice nucleation on surrogates of mineral dust journal January 2007
Influence of particle size on the ice nucleating ability of mineral dusts journal January 2009
Heterogeneous ice nucleation: exploring the transition from stochastic to singular freezing behavior journal January 2011
On the representation of immersion and condensation freezing in cloud models using different nucleation schemes journal January 2012
A parameterization of cirrus cloud formation: Heterogeneous freezing journal January 2003
Adsorption of Gases in Multimolecular Layers journal February 1938
Baseline studies of the Clay Minerals Society source clays: specific surface area by the Brunauer Emmett Teller (BET) method journal February 2006
Review of the vapour pressures of ice and supercooled water for atmospheric applications journal April 2005
Do NAD and NAT Form in Liquid Stratospheric Aerosols by Pseudoheterogeneous Nucleation? journal May 2006
Homogeneous nucleation of NAD and NAT in liquid stratospheric aerosols: insufficient to explain denitrification journal January 2002
Immersion mode heterogeneous ice nucleation by an illite rich powder representative of atmospheric mineral dust journal January 2012
Heterogeneous freezing of water droplets containing kaolinite particles journal January 2011
The ice nucleation ability of one of the most abundant types of fungal spores found in the atmosphere journal January 2011
Do atmospheric aerosols form glasses? journal January 2008
A comparison of heterogeneous ice nucleation parameterizations using a parcel model framework journal January 2009
Measurements of the concentration and composition of nuclei for cirrus formation journal December 2003
The susceptibility of ice formation in upper tropospheric clouds to insoluble aerosol components journal August 1997
Prediction of the number of cloud droplets in the ECHAM GCM journal April 1999
Sensitivity studies of different aerosol indirect effects in mixed-phase clouds journal January 2009
Influence of Saharan dust on cloud glaciation in southern Morocco during the Saharan Mineral Dust Experiment journal January 2008

Cited By (31)

Heterogeneous Ice Nucleation in the Tropical Tropopause Layer journal November 2018
Stochastic nucleation processes and substrate abundance explain time-dependent freezing in supercooled droplets journal January 2020
Ice-nucleating bacteria control the order and dynamics of interfacial water journal April 2016
Perspectives on the Future of Ice Nucleation Research: Research Needs and Unanswered Questions Identified from Two International Workshops journal July 2017
Immersion freezing of water and aqueous ammonium sulfate droplets initiated by humic-like substances as a function of water activity journal January 2013
Laboratory studies of immersion and deposition mode ice nucleation of ozone aged mineral dust particles journal January 2013
Contact freezing: a review of experimental studies journal January 2013
Kaolinite particles as ice nuclei: learning from the use of different kaolinite samples and different coatings journal January 2014
Organic matter matters for ice nuclei of agricultural soil origin journal January 2014
Technical Note: A proposal for ice nucleation terminology journal January 2015
A comprehensive laboratory study on the immersion freezing behavior of illite NX particles: a comparison of 17 ice nucleation measurement techniques journal January 2015
Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles journal January 2015
A laboratory investigation of the ice nucleation efficiency of three types of mineral and soil dust journal January 2018
Ice nucleation activity of silicates and aluminosilicates in pure water and aqueous solutions – Part 1: The K-feldspar microcline journal January 2018
Mixed-phase orographic cloud microphysics during StormVEx and IFRACS journal January 2019
Ice nucleation activity of silicates and aluminosilicates in pure water and aqueous solutions – Part 2: Quartz and amorphous silica journal January 2019
Ice nucleation activity of silicates and aluminosilicates in pure water and aqueous solutions – Part 3: Aluminosilicates journal January 2019
An instrument for quantifying heterogeneous ice nucleation in multiwell plates using infrared emissions to detect freezing journal January 2018
A technique for quantifying heterogeneous ice nucleation in microlitre supercooled water droplets journal January 2015
BINARY: an optical freezing array for assessing temperature and time dependence of heterogeneous ice nucleation journal January 2014
Contact freezing: a review of experimental studies text January 2013
A comprehensive laboratory study on the immersion freezing behavior of illite NX particles: A comparison of 17 ice nucleation measurement techniques text January 2015
Perspectives on the Future of Ice Nucleation Research: Research Needs and Unanswered Questions Identified from Two International Workshops text January 2017
Ice nucleation activity of silicates and aluminosilicates in pure water and aqueous solutions - Part 1: The K-feldspar microcline text January 2018
A laboratory investigation of the ice nucleation efficiency of three types of mineral and soil dust text January 2018
Mixed-phase orographic cloud microphysics during StormVEx and IFRACS text January 2019
Ice nucleation activity of silicates and aluminosilicates in pure water and aqueous solutions – Part 2: Quartz and amorphous silica text January 2019
Ice nucleation activity of silicates and aluminosilicates in pure water and aqueous solutions - Part 3: Aluminosilicates text January 2019
Laboratory studies of immersion and deposition mode ice nucleation of ozone aged mineral dust particles text January 2013
BINARY: an optical freezing array for assessing temperature and time dependence of heterogeneous ice nucleation journal January 2015
A technique for quantifying heterogeneous ice nucleation in microlitre supercooled water droplets text January 2015

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