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Title: The Role of Organic Aerosol in Atmospheric Ice Nucleation: A Review

Abstract

Predicting the formation of ice crystals in the atmosphere presents one of the great challenges in physical sciences with important implications for the chemistry and composition of the Earth’s atmosphere, the hydrological cycle, and climate. Among atmospheric ice formation processes, heterogeneous ice nucleation proceeds on aerosol particles ranging from a few nanometers to micrometers in size, commonly referred to as ice nucleating particles (INPs). Research over the last two decades has demonstrated that organic matter (OM) is ubiquitous in the atmosphere, present as organic aerosol (OA) particles or as coatings on other particle types. While it is well understood that mineral dust particles can induce ice nucleation under atmospheric conditions, it is currently not clear how much OA particles including pollution aerosol and secondary organic aerosol (SOA) contributes to the ambient INP population. The physicochemical properties of OM make predicting how OM interacts with water vapor leading ultimately to ice crystals challenging. This review focuses on the role of OM in INPs, summarizing and highlighting recent advances in our understanding of the ice nucleation process gained from theoretical, laboratory, and field studies. Examination of ice residuals and INPs with analytical techniques demonstrates that OM participates in atmospheric ice crystal formation.more » Molecular dynamic simulations provide insight into the microscopic processes that initiate ice nucleation. The amorphous phase state of OM in the supercooled and metastable regime is identified as a key factor in assessing the particles’ nucleation pathways and rates. A theoretical model is advanced, based on particle water activity, to holistically predict amorphous phase changes and ice nucleation rates of particles coated by OM. The goal of this review is to synthesize our current understanding and propose future research directions needed to fully evaluate how OA particles contribute to INPs in the atmosphere.« less

Authors:
ORCiD logo [1];  [2];  [3]
  1. Stony Brook Univ., NY (United States)
  2. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  3. Xiamen Univ. (China)
Publication Date:
Research Org.:
Stony Brook Univ., NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1498735
Grant/Contract Number:  
SC0016370
Resource Type:
Accepted Manuscript
Journal Name:
ACS Earth and Space Chemistry
Additional Journal Information:
Journal Volume: 2; Journal Issue: 3; Journal ID: ISSN 2472-3452
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; organic aerosol; ice nucleation; organic matter; amorphous phase state; molecular dynamics simulation; laboratory experiments; field measurements; organic coating

Citation Formats

Knopf, Daniel A., Alpert, Peter A., and Wang, Bingbing. The Role of Organic Aerosol in Atmospheric Ice Nucleation: A Review. United States: N. p., 2018. Web. doi:10.1021/acsearthspacechem.7b00120.
Knopf, Daniel A., Alpert, Peter A., & Wang, Bingbing. The Role of Organic Aerosol in Atmospheric Ice Nucleation: A Review. United States. https://doi.org/10.1021/acsearthspacechem.7b00120
Knopf, Daniel A., Alpert, Peter A., and Wang, Bingbing. Fri . "The Role of Organic Aerosol in Atmospheric Ice Nucleation: A Review". United States. https://doi.org/10.1021/acsearthspacechem.7b00120. https://www.osti.gov/servlets/purl/1498735.
@article{osti_1498735,
title = {The Role of Organic Aerosol in Atmospheric Ice Nucleation: A Review},
author = {Knopf, Daniel A. and Alpert, Peter A. and Wang, Bingbing},
abstractNote = {Predicting the formation of ice crystals in the atmosphere presents one of the great challenges in physical sciences with important implications for the chemistry and composition of the Earth’s atmosphere, the hydrological cycle, and climate. Among atmospheric ice formation processes, heterogeneous ice nucleation proceeds on aerosol particles ranging from a few nanometers to micrometers in size, commonly referred to as ice nucleating particles (INPs). Research over the last two decades has demonstrated that organic matter (OM) is ubiquitous in the atmosphere, present as organic aerosol (OA) particles or as coatings on other particle types. While it is well understood that mineral dust particles can induce ice nucleation under atmospheric conditions, it is currently not clear how much OA particles including pollution aerosol and secondary organic aerosol (SOA) contributes to the ambient INP population. The physicochemical properties of OM make predicting how OM interacts with water vapor leading ultimately to ice crystals challenging. This review focuses on the role of OM in INPs, summarizing and highlighting recent advances in our understanding of the ice nucleation process gained from theoretical, laboratory, and field studies. Examination of ice residuals and INPs with analytical techniques demonstrates that OM participates in atmospheric ice crystal formation. Molecular dynamic simulations provide insight into the microscopic processes that initiate ice nucleation. The amorphous phase state of OM in the supercooled and metastable regime is identified as a key factor in assessing the particles’ nucleation pathways and rates. A theoretical model is advanced, based on particle water activity, to holistically predict amorphous phase changes and ice nucleation rates of particles coated by OM. The goal of this review is to synthesize our current understanding and propose future research directions needed to fully evaluate how OA particles contribute to INPs in the atmosphere.},
doi = {10.1021/acsearthspacechem.7b00120},
journal = {ACS Earth and Space Chemistry},
number = 3,
volume = 2,
place = {United States},
year = {2018},
month = {1}
}

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Understanding electrofreezing in water simulations
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Ice nucleation by electric surface fields of varying range and geometry
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Molecular Dynamics Simulations of Ice Nucleation by Electric Fields
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Heterogeneous Ice Nucleation Induced by Electric Fields
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Can Ice-Like Structures Form on Non-Ice-Like Substrates? The Example of the K-feldspar Microcline
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The Many Faces of Heterogeneous Ice Nucleation: Interplay Between Surface Morphology and Hydrophobicity
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Non-hexagonal ice at hexagonal surfaces: the role of lattice mismatch
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Pre-critical fluctuations and what they disclose about heterogeneous crystal nucleation
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Vapor deposition of water on graphitic surfaces: Formation of amorphous ice, bilayer ice, ice I, and liquid water
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Does Hydrophilicity of Carbon Particles Improve Their Ice Nucleation Ability?
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Heterogeneous Nucleation of Ice on Carbon Surfaces
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Ice nucleation on carbon surface supports the classical theory for heterogeneous nucleation
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What makes a good descriptor for heterogeneous ice nucleation on OH-patterned surfaces
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Ice Nucleation Efficiency of Hydroxylated Organic Surfaces Is Controlled by Their Structural Fluctuations and Mismatch to Ice
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Nucleation at the Contact Line Observed on Nanotextured Surfaces
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High-Speed Imaging of Freezing Drops: Still No Preference for the Contact Line
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Fast Imaging of Freezing Drops: No Preference for Nucleation at the Contact Line
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Thermodynamics of Heterogeneous Crystal Nucleation in Contact and Immersion Modes
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Ice nucleation behaviour on sol–gel coatings with different surface energy and roughness
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Homogeneous Bulk, Surface, and Edge Nucleation in Crystalline Nanodroplets
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Surface-charge-induced orientation of interfacial water suppresses heterogeneous ice nucleation on α-alumina (0001)
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Probing ice-nucleation processes on the molecular level using second harmonic generation spectroscopy
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Predicting global atmospheric ice nuclei distributions and their impacts on climate
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Measurements of the concentration and composition of nuclei for cirrus formation
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Sea spray aerosol as a unique source of ice nucleating particles
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Ice nucleating particles over the Eastern Mediterranean measured by unmanned aircraft systems
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Comparative measurements of ambient atmospheric concentrations of ice nucleating particles using multiple immersion freezing methods and a continuous flow diffusion chamber
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Rainfall drives atmospheric ice-nucleating particles in the coastal climate of southern Norway
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The measurement and parameterization of ice nucleating particles in different backgrounds of China
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An evaluation of ice nuclei characteristics from the long-term measurement data over North China
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Chemical characteristics of ice residual nuclei in anvil cirrus clouds: evidence for homogeneous and heterogeneous ice formation
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Importance of aerosol composition, mixing state, and morphology for heterogeneous ice nucleation: A combined field and laboratory approach: HETEROGENEOUS ICE NUCLEATION
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Single particle analyses of ice nucleating aerosols in the upper troposphere and lower stratosphere
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Sampling the composition of cirrus ice residuals
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Characteristics of atmospheric ice nucleating particles associated with biomass burning in the US: Prescribed burns and wildfires: Biomass burning ice nucleating particles
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In situ detection of biological particles in cloud ice-crystals
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Flight-based chemical characterization of biomass burning aerosols within two prescribed burn smoke plumes
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Biomass burning as a potential source for atmospheric ice nuclei: Western wildfires and prescribed burns: BIOMASS BURNING AS A POTENTIAL IN SOURCE
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Relative roles of biogenic emissions and Saharan dust as ice nuclei in the Amazon basin
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Ice nuclei characteristics from M-PACE and their relation to ice formation in clouds
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Online single particle analysis of ice particle residuals from mountain-top mixed-phase clouds using laboratory derived particle type assignment
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Chemical composition and mixing-state of ice residuals sampled within mixed phase clouds
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Single-particle characterization of ice-nucleating particles and ice particle residuals sampled by three different techniques
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Combustion particles as ice nuclei in an urban environment: Evidence from single-particle mass spectrometry
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Reactive intermediates revealed in secondary organic aerosol formation from isoprene
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Comment on "Unexpected Epoxide Formation in the Gas-Phase Photooxidation of Isoprene"
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An overview of the MILAGRO 2006 Campaign: Mexico City emissions and their transport and transformation
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The 2010 California Research at the Nexus of Air Quality and Climate Change (CalNex) field study: CalNex 2010 FIELD PROJECT OVERVIEW
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Measurements of natural ice nuclei with a continuous flow diffusion chamber
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Quantification of online removal of refractory black carbon using laser-induced incandescence in the single particle soot photometer
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A New Method to Determine the Number Concentrations of Refractory Black Carbon Ice Nucleating Particles
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Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)
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Ice nucleating particles at a coastal marine boundary layer site: correlations with aerosol type and meteorological conditions
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Size-resolved measurements of ice-nucleating particles at six locations in North America and one in Europe
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The characteristics of atmospheric ice nuclei measured at different altitudes in the Huangshan Mountains in Southeast China
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Atmospheric Ice Nucleating Particle measurements at the high mountain observatory Mt. Cimone (2165 m a.s.l., Italy)
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The effect of organic coating on the heterogeneous ice nucleation efficiency of mineral dust aerosols
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State transformations and ice nucleation in amorphous (semi-)solid organic aerosol
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Heterogeneous ice nucleation on phase-separated organic-sulfate particles: effect of liquid vs. glassy coatings
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Heterogeneous Ice Nucleation on Simulated Secondary Organic Aerosol
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Factors controlling the ice nucleating abilities of α -pinene SOA particles : LADINO ET AL.
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Heterogeneous ice nucleation of viscous secondary organic aerosol produced from ozonolysis of α -pinene
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Analysis of isothermal and cooling-rate-dependent immersion freezing by a unifying stochastic ice nucleation model
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A comprehensive laboratory study on the immersion freezing behavior of illite NX particles: a comparison of 17 ice nucleation measurement techniques
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Thermodynamic derivation of the activation energy for ice nucleation
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Analysis of the effect of water activity on ice formation using a new thermodynamic framework
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On the ice nucleation spectrum
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Transient Phase of Ice Observed by Sum Frequency Generation at the Water/Mineral Interface During Freezing
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Environmental scanning electron microscopy (ESEM) as a new technique to determine the ice nucleation capability of individual atmospheric aerosol particles
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The ice nucleating ability of pollen
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A new electrodynamic balance (EDB) design for low-temperature studies: application to immersion freezing of pollen extract bioaerosols
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Suspendable macromolecules are responsible for ice nucleation activity of birch and conifer pollen
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Contribution of pollen to atmospheric ice nuclei concentrations
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Immersion freezing of birch pollen washing water
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Laboratory-generated mixtures of mineral dust particles with biological substances: characterization of the particle mixing state and immersion freezing behavior
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The relevance of nanoscale biological fragments for ice nucleation in clouds
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Organic matter matters for ice nuclei of agricultural soil origin
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Ice nucleation activity of agricultural soil dust aerosols from Mongolia, Argentina, and Germany: Ice Nucleation Activity of Soil Dust
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Sources of organic ice nucleating particles in soils
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Heterogeneous freezing of ice on atmospheric aerosols containing ash, soot, and soil
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Ice nucleation by cellulose and its potential contribution to ice formation in clouds
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The Effects of Low Molecular Weight Dicarboxylic Acids on Cloud Formation
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Depositional Ice Nucleation on Monocarboxylic Acids: Effect of the O:C Ratio
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Immersion freezing of water and aqueous ammonium sulfate droplets initiated by humic-like substances as a function of water activity
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Chemistry and morphology of dried-up pollen suspension residues: Chemistry and morphology of pollen suspension residues
journal, October 2013

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Near-surface and columnar measurements with a micro pulse lidar of atmospheric pollen in Barcelona, Spain
journal, January 2016

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Ambient aerosol concentrations of sugars and sugar-alcohols at four different sites in Norway
journal, January 2007


Influence of rain on the abundance of bioaerosols in fine and coarse particles
journal, January 2017

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Ice nuclei in marine air: biogenic particles or dust?
journal, January 2013

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Ice nucleation from aqueous NaCl droplets with and without marine diatoms
journal, January 2011

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Initiation of the ice phase by marine biogenic surfaces in supersaturated gas and supercooled aqueous phases
journal, January 2011

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Stimulation of ice nucleation by marine diatoms
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Addressing the ice nucleating abilities of marine aerosol: A combination of deposition mode laboratory and field measurements
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Size-resolved characterization of the polysaccharidic and proteinaceous components of sea spray aerosol
journal, April 2017


A Dynamic Link between Ice Nucleating Particles Released in Nascent Sea Spray Aerosol and Oceanic Biological Activity during Two Mesocosm Experiments
journal, January 2017

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Ice nucleation by surrogates for atmospheric mineral dust and mineral dust/sulfate particles at cirrus temperatures
journal, January 2005

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The immersion mode ice nucleation behavior of mineral dusts: A comparison of different pure and surface modified dusts
journal, October 2014

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Ice nucleation of bare and sulfuric acid-coated mineral dust particles and implication for cloud properties: Ice formation on dust particles
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Ice formation on nitric acid‐coated dust particles: Laboratory and modeling studies
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Surface modification of mineral dust particles by sulphuric acid processing: implications for ice nucleation abilities
journal, January 2011

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Impacts of chemical reactivity on ice nucleation of kaolinite particles: A case study of levoglucosan and sulfuric acid: ICE NUCLEATION OF COATED KAOLINITE
journal, October 2012

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Interactions of Water with Mineral Dust Aerosol: Water Adsorption, Hygroscopicity, Cloud Condensation, and Ice Nucleation
journal, March 2016


Effects of sulfuric acid and ammonium sulfate coatings on the ice nucleation properties of kaolinite particles: FREEZING OF COATED KAOLINITE PARTICLES
journal, January 2009

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  • Geophysical Research Letters, Vol. 36, Issue 2
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Effects of sulfate coatings on the ice nucleation properties of a biological ice nucleus and several types of minerals
journal, January 2010

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Morphology and mixing state of aged soot particles at a remote marine free troposphere site: Implications for optical properties: Morphology and mixing state of aged soot
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Morphology and mixing state of individual freshly emitted wildfire carbonaceous particles
journal, July 2013

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Morphology of diesel soot residuals from supercooled water droplets and ice crystals: implications for optical properties
journal, November 2015


A New Ice Nucleation Active Site Parameterization for Desert Dust and Soot
journal, March 2017

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  • Journal of the Atmospheric Sciences, Vol. 74, Issue 3
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Ice nucleation and droplet formation by bare and coated soot particles
journal, January 2011

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Effect of photochemical ageing on the ice nucleation properties of diesel and wood burning particles
journal, January 2013

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Ice‐nucleating particle emissions from photochemically aged diesel and biodiesel exhaust
journal, May 2016

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  • Geophysical Research Letters, Vol. 43, Issue 10
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Lability of secondary organic particulate matter
journal, October 2016

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Factors controlling the evaporation of secondary organic aerosol from α‐pinene ozonolysis
journal, March 2017

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Quantifying the volatility of organic aerosol in the southeastern US
journal, January 2017

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Cloud Processing of Secondary Organic Aerosol from Isoprene and Methacrolein Photooxidation
journal, September 2017

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Evaporation Kinetics of Laboratory-Generated Secondary Organic Aerosols at Elevated Relative Humidity
journal, December 2014

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Optical Properties of Secondary Organic Aerosols and Their Changes by Chemical Processes
journal, February 2015

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Multiphase Chemistry at the Atmosphere–Biosphere Interface Influencing Climate and Public Health in the Anthropocene
journal, February 2015

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Atmospheric Aerosols: Composition, Transformation, Climate and Health Effects
journal, November 2005


Multiphase Chemical Kinetics of NO 3 Radicals Reacting with Organic Aerosol Components from Biomass Burning
journal, May 2012

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Heterogeneous oxidation kinetics of organic biomass burning aerosol surrogates by O3, NO2, N2O5, and NO3
journal, January 2011

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Effects of Chemical Aging on the Ice Nucleation Activity of Soot and Polycyclic Aromatic Hydrocarbon Aerosols
journal, October 2014

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The importance of phase in the radical-initiated oxidation of model organic aerosols: reactions of solid and liquid brassidic acid particles
journal, January 2009

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Gas uptake and chemical aging of semisolid organic aerosol particles
journal, June 2011

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Multiphase Chemical Kinetics of OH Radical Uptake by Molecular Organic Markers of Biomass Burning Aerosols: Humidity and Temperature Dependence, Surface Reaction, and Bulk Diffusion
journal, November 2014

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Multiphase OH oxidation kinetics of organic aerosol: The role of particle phase state and relative humidity
journal, July 2014

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Heterogeneous Oxidation of Atmospheric Organic Aerosol: Kinetics of Changes to the Amount and Oxidation State of Particle-Phase Organic Carbon
journal, September 2015

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OH-Initiated Heterogeneous Aging of Highly Oxidized Organic Aerosol
journal, February 2012

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Mass-based hygroscopicity parameter interaction model and measurement of atmospheric aerosol water uptake
journal, January 2013

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An interfacial mechanism for cloud droplet formation on organic aerosols
journal, March 2016


Ozonolysis of α -pinene at atmospherically relevant concentrations: Temperature dependence of aerosol mass fractions (yields)
journal, January 2007

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Temperature dependence of secondary organic aerosol
journal, July 2009


Temperature dependence of yields of secondary organic aerosols from the ozonolysis of α -pinene and limonene
journal, January 2009

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The effect of sub-zero temperature on the formation and composition of secondary organic aerosol from ozonolysis of alpha-pinene
journal, January 2017

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Adsorptive uptake of water by semisolid secondary organic aerosols: Water uptake of SOA
journal, April 2015

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Classical nucleation theory of immersion freezing: sensitivity of contact angle schemes to thermodynamic and kinetic parameters
journal, January 2017

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Effect of particle surface area on ice active site densities retrieved from droplet freezing spectra
journal, January 2016

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Deposition nucleation on mineral dust particles: a case against classical nucleation theory with the assumption of a single contact angle
journal, January 2012


Heterogeneous ice nucleation: exploring the transition from stochastic to singular freezing behavior
journal, January 2011

  • Niedermeier, D.; Shaw, R. A.; Hartmann, S.
  • Atmospheric Chemistry and Physics, Vol. 11, Issue 16
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Heterogeneous freezing of water droplets containing kaolinite particles
journal, January 2011

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Time-dependent freezing rate parcel model
journal, January 2015


Efficiency of immersion mode ice nucleation on surrogates of mineral dust
journal, January 2007

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  • Atmospheric Chemistry and Physics, Vol. 7, Issue 19
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Experimental study on the ice nucleation ability of size-selected kaolinite particles in the immersion mode
journal, January 2010

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Studies of heterogeneous freezing by three different desert dust samples
journal, January 2009

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Repeatability and randomness in heterogeneous freezing nucleation
journal, January 2008


Sensitivities of immersion freezing: Reconciling classical nucleation theory and deterministic expressions: SENSITIVITIES OF IMMERSION FREEZING
journal, June 2013

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On the representation of immersion and condensation freezing in cloud models using different nucleation schemes
journal, January 2012


The formation of ice in a long-lived supercooled layer cloud: Ice Formation in Altocumulus
journal, January 2013

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Different contact angle distributions for heterogeneous ice nucleation in the Community Atmospheric Model version 5
journal, January 2014


Contributions of Clouds, Surface Albedos, and Mixed-Phase Ice Nucleation Schemes to Arctic Radiation Biases in CAM5
journal, July 2014

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Aerosol–cloud interactions—a challenge for measurements and modeling at the cutting edge of cloud–climate interactions
journal, April 2008


ATMOSPHERE: When Dry Air Is Too Humid
journal, December 2006


Immersion mode heterogeneous ice nucleation by an illite rich powder representative of atmospheric mineral dust
journal, January 2012

  • Broadley, S. L.; Murray, B. J.; Herbert, R. J.
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Toward ice formation closure in Arctic mixed-phase boundary layer clouds during ISDAC
journal, January 2011

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Intercomparison of large-eddy simulations of Arctic mixed-phase clouds: Importance of ice size distribution assumptions
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Sensitivity of modeled arctic mixed-phase stratocumulus to cloud condensation and ice nuclei over regionally varying surface conditions: SIMULATION OF ARCTIC MIXED-PHASE CLOUDS
journal, March 2008

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A Particle-Surface-Area-Based Parameterization of Immersion Freezing on Desert Dust Particles
journal, October 2012

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Ice Nucleating Particle Measurements at 241 K during Winter Months at 3580 m MSL in the Swiss Alps
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