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Title: Stochastic nucleation processes and substrate abundance explain time-dependent freezing in supercooled droplets

Abstract

Atmospheric immersion freezing (IF), a heterogeneous ice nucleation process where an ice nucleating particle (INP) is immersed in supercooled water, is a dominant ice formation pathway impacting the hydrological cycle and climate. Implementation of IF derived from field and laboratory data in cloud and climate models is difficult due to the high variability in spatio-temporal scales, INP composition, and morphological complexity. We demonstrate that IF can be consistently described by a stochastic nucleation process accounting for uncertainties in the INP surface area. This approach accounts for time-dependent freezing, a wide range of surface areas and challenges phenomenological descriptions typically used to interpret IF. The results have an immediate impact on the current description, interpretation, and experiments of IF and its implementation in models. The findings are in accord with nucleation theory, and thus should hold for any supercooled liquid material that nucleates in contact with a substrate.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [3]; ORCiD logo [3]
  1. Stony Brook Univ., NY (United States)
  2. Paul Scherrer Inst., Villigen (Switzerland)
  3. Weizmann Inst. of Science, Rehovot (Israel)
Publication Date:
Research Org.:
Stony Brook Univ., NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23). Climate and Environmental Sciences Division; German Research Foundation (DFG); Israel Science Foundation; National Aeronautic and Space Administration (NASA)
OSTI Identifier:
1593550
Grant/Contract Number:  
SC0016370; NNX17AJ12G; 213/16
Resource Type:
Accepted Manuscript
Journal Name:
npj Climate and Atmospheric Science
Additional Journal Information:
Journal Volume: 3; Journal Issue: 1; Journal ID: ISSN 2397-3722
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; atmospheric chemistry; climate and earth system modelling; hydrology

Citation Formats

Knopf, Daniel A., Alpert, Peter A., Zipori, Assaf, Reicher, Naama, and Rudich, Yinon. Stochastic nucleation processes and substrate abundance explain time-dependent freezing in supercooled droplets. United States: N. p., 2020. Web. doi:10.1038/s41612-020-0106-4.
Knopf, Daniel A., Alpert, Peter A., Zipori, Assaf, Reicher, Naama, & Rudich, Yinon. Stochastic nucleation processes and substrate abundance explain time-dependent freezing in supercooled droplets. United States. doi:10.1038/s41612-020-0106-4.
Knopf, Daniel A., Alpert, Peter A., Zipori, Assaf, Reicher, Naama, and Rudich, Yinon. Fri . "Stochastic nucleation processes and substrate abundance explain time-dependent freezing in supercooled droplets". United States. doi:10.1038/s41612-020-0106-4. https://www.osti.gov/servlets/purl/1593550.
@article{osti_1593550,
title = {Stochastic nucleation processes and substrate abundance explain time-dependent freezing in supercooled droplets},
author = {Knopf, Daniel A. and Alpert, Peter A. and Zipori, Assaf and Reicher, Naama and Rudich, Yinon},
abstractNote = {Atmospheric immersion freezing (IF), a heterogeneous ice nucleation process where an ice nucleating particle (INP) is immersed in supercooled water, is a dominant ice formation pathway impacting the hydrological cycle and climate. Implementation of IF derived from field and laboratory data in cloud and climate models is difficult due to the high variability in spatio-temporal scales, INP composition, and morphological complexity. We demonstrate that IF can be consistently described by a stochastic nucleation process accounting for uncertainties in the INP surface area. This approach accounts for time-dependent freezing, a wide range of surface areas and challenges phenomenological descriptions typically used to interpret IF. The results have an immediate impact on the current description, interpretation, and experiments of IF and its implementation in models. The findings are in accord with nucleation theory, and thus should hold for any supercooled liquid material that nucleates in contact with a substrate.},
doi = {10.1038/s41612-020-0106-4},
journal = {npj Climate and Atmospheric Science},
number = 1,
volume = 3,
place = {United States},
year = {2020},
month = {1}
}

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Works referenced in this record:

Methodology to quantify the ratio of multiple-to single-charged fractions acquired in aerosol neutralizers
journal, February 2016


Direct observation of ice nucleation events on individual atmospheric particles
journal, January 2016

  • Wang, Bingbing; Knopf, Daniel A.; China, Swarup
  • Physical Chemistry Chemical Physics, Vol. 18, Issue 43
  • DOI: 10.1039/C6CP05253C

Production of secondary ice particles during the growth of graupel by riming
journal, January 1976

  • Mossop, S. C.
  • Quarterly Journal of the Royal Meteorological Society, Vol. 102, Issue 431
  • DOI: 10.1002/qj.49710243104

Characterization of Dust Particles’ 3D Shape and Roughness with Nanometer Resolution
journal, February 2015


High-speed imaging of ice nucleation in water proves the existence of active sites
journal, February 2019

  • Holden, Mark A.; Whale, Thomas F.; Tarn, Mark D.
  • Science Advances, Vol. 5, Issue 2
  • DOI: 10.1126/sciadv.aav4316

On the thermodynamic and kinetic aspects of immersion ice nucleation
journal, January 2018


Analysis of isothermal and cooling-rate-dependent immersion freezing by a unifying stochastic ice nucleation model
journal, January 2016


Loitering of the retreating sea ice edge in the A rctic S eas
journal, December 2015

  • Steele, Michael; Ermold, Wendy
  • Journal of Geophysical Research: Oceans, Vol. 120, Issue 12
  • DOI: 10.1002/2015JC011182

The Role of Organic Aerosol in Atmospheric Ice Nucleation: A Review
journal, January 2018


Dropspots: a picoliter array in a microfluidic device
journal, January 2009

  • Schmitz, Christian H. J.; Rowat, Amy C.; Köster, Sarah
  • Lab on a Chip, Vol. 9, Issue 1, p. 44-49
  • DOI: 10.1039/B809670H

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

  • Alpert, P. A.; Aller, J. Y.; Knopf, D. A.
  • Atmospheric Chemistry and Physics, Vol. 11, Issue 12
  • DOI: 10.5194/acp-11-5539-2011

Experimental study on the ice nucleation ability of size-selected kaolinite particles in the immersion mode
journal, January 2010

  • Lüönd, F.; Stetzer, O.; Welti, A.
  • Journal of Geophysical Research, Vol. 115, Issue D14
  • DOI: 10.1029/2009JD012959

Technical Note: A proposal for ice nucleation terminology
journal, January 2015


Thermodynamic derivation of the activation energy for ice nucleation
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

  • Hiranuma, N.; Augustin-Bauditz, S.; Bingemer, H.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 5
  • DOI: 10.5194/acp-15-2489-2015

Progress in the Analysis of Complex Atmospheric Particles
journal, June 2016


Ice nucleation by particles immersed in supercooled cloud droplets
journal, January 2012

  • Murray, B. J.; O'Sullivan, D.; Atkinson, J. D.
  • Chemical Society Reviews, Vol. 41, Issue 19
  • DOI: 10.1039/c2cs35200a

Water activity as the determinant for homogeneous ice nucleation in aqueous solutions
journal, August 2000

  • Koop, Thomas; Luo, Beiping; Tsias, Athanasios
  • Nature, Vol. 406, Issue 6796
  • DOI: 10.1038/35020537

Resurgence in Ice Nuclei Measurement Research
journal, December 2011

  • DeMott, Paul J.; Möhler, Ottmar; Stetzer, Olaf
  • Bulletin of the American Meteorological Society, Vol. 92, Issue 12
  • DOI: 10.1175/2011BAMS3119.1

Active sites in heterogeneous ice nucleation—the example of K-rich feldspars
journal, December 2016


The Horizontal Ice Nucleation Chamber (HINC): INP measurements at conditions relevant for mixed-phase clouds at the High Altitude Research Station Jungfraujoch
journal, January 2017

  • Lacher, Larissa; Lohmann, Ulrike; Boose, Yvonne
  • Atmospheric Chemistry and Physics, Vol. 17, Issue 24
  • DOI: 10.5194/acp-17-15199-2017

Freezing of Water and Aqueous NaCl Droplets Coated by Organic Monolayers as a Function of Surfactant Properties and Water Activity
journal, June 2011

  • Knopf, Daniel A.; Forrester, Seanna M.
  • The Journal of Physical Chemistry A, Vol. 115, Issue 22
  • DOI: 10.1021/jp2014644

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

  • Augustin-Bauditz, S.; Wex, H.; Kanter, S.
  • Geophysical Research Letters, Vol. 41, Issue 20
  • DOI: 10.1002/2014GL061317

Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles
journal, January 2015

  • DeMott, P. J.; Prenni, A. J.; McMeeking, G. R.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 1
  • DOI: 10.5194/acp-15-393-2015

Frequency of occurrence of rain from liquid-, mixed-, and ice-phase clouds derived from A-Train satellite retrievals: RAIN FROM LIQUID- AND ICE-PHASE CLOUDS
journal, August 2015

  • Mülmenstädt, Johannes; Sourdeval, O.; Delanoë, J.
  • Geophysical Research Letters, Vol. 42, Issue 15
  • DOI: 10.1002/2015GL064604

Surface features on Sahara soil dust particles made visible by atomic force microscope (AFM) phase images
journal, January 2008

  • Helas, G.; Andreae, M. O.
  • Atmospheric Measurement Techniques, Vol. 1, Issue 1
  • DOI: 10.5194/amt-1-1-2008

Interpretation of freezing nucleation experiments: singular and stochastic; sites and surfaces
journal, January 2014


On the ice nucleation spectrum
journal, January 2012


Clarifying the Dominant Sources and Mechanisms of Cirrus Cloud Formation
journal, May 2013


Heterogeneous Ice Nucleation Rate Coefficient of Water Droplets Coated by a Nonadecanol Monolayer
journal, February 2007

  • Zobrist, B.; Koop, T.; Luo, B. P.
  • The Journal of Physical Chemistry C, Vol. 111, Issue 5
  • DOI: 10.1021/jp066080w

Influence of particle size on the ice nucleating ability of mineral dusts
journal, January 2009

  • Welti, A.; Lüönd, F.; Stetzer, O.
  • Atmospheric Chemistry and Physics, Vol. 9, Issue 18
  • DOI: 10.5194/acp-9-6705-2009

On the bipolar charge distribution used for mobility particle sizing: Theoretical considerations
journal, October 2015


Aerosol Effects on Climate via Mixed-Phase and Ice Clouds
journal, August 2017


Heterogeneous ice nucleation on atmospheric aerosols: a review of results from laboratory experiments
journal, January 2012


Warm rain processes over tropical oceans and climate implications: WARM RAIN PROCESSES OVER TROPICAL OCEANS
journal, December 2003


A FIRE-ACE/SHEBA Case Study of Mixed-Phase Arctic Boundary Layer Clouds: Entrainment Rate Limitations on Rapid Primary Ice Nucleation Processes
journal, January 2012

  • Fridlind, Ann M.; van Diedenhoven, Bastiaan; Ackerman, Andrew S.
  • Journal of the Atmospheric Sciences, Vol. 69, Issue 1
  • DOI: 10.1175/JAS-D-11-052.1

BINARY: an optical freezing array for assessing temperature and time dependence of heterogeneous ice nucleation
journal, January 2015


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

  • Westbrook, C. D.; Illingworth, A. J.
  • Quarterly Journal of the Royal Meteorological Society, Vol. 139, Issue 677
  • DOI: 10.1002/qj.2096

Freezing of HNO 3 /H 2 SO 4 /H 2 O Solutions at Stratospheric Temperatures:  Nucleation Statistics and Experiments
journal, February 1997

  • Koop, Thomas; Luo, Beiping; Biermann, Uta M.
  • The Journal of Physical Chemistry A, Vol. 101, Issue 6
  • DOI: 10.1021/jp9626531

A Microorifice Uniform Deposit Impactor (MOUDI): Description, Calibration, and Use
journal, January 1991

  • Marple, Virgil A.; Rubow, Kenneth L.; Behm, Steven M.
  • Aerosol Science and Technology, Vol. 14, Issue 4
  • DOI: 10.1080/02786829108959504

A water activity based model of heterogeneous ice nucleation kinetics for freezing of water and aqueous solution droplets
journal, January 2013

  • Knopf, Daniel A.; Alpert, Peter A.
  • Faraday Discussions, Vol. 165
  • DOI: 10.1039/c3fd00035d

The Generation of Secondary Ice Particles in Clouds by Crystal–Crystal Collision
journal, November 1978


The WeIzmann Supercooled Droplets Observation on a Microarray (WISDOM) and application for ambient dust
journal, January 2018

  • Reicher, Naama; Segev, Lior; Rudich, Yinon
  • Atmospheric Measurement Techniques, Vol. 11, Issue 1
  • DOI: 10.5194/amt-11-233-2018

Parameterizations for ice nucleation in biological and atmospheric systems
journal, January 2009

  • Koop, Thomas; Zobrist, Bernhard
  • Physical Chemistry Chemical Physics, Vol. 11, Issue 46
  • DOI: 10.1039/b914289d

Immersion Freezing of Kaolinite: Scaling with Particle Surface Area
journal, January 2016

  • Hartmann, Susan; Wex, Heike; Clauss, Tina
  • Journal of the Atmospheric Sciences, Vol. 73, Issue 1
  • DOI: 10.1175/JAS-D-15-0057.1

Analysis of the effect of water activity on ice formation using a new thermodynamic framework
journal, January 2014


Breakup of levitated frost particles
journal, June 1998

  • Bacon, Neil J.; Swanson, Brian D.; Baker, Marcia B.
  • Journal of Geophysical Research: Atmospheres, Vol. 103, Issue D12
  • DOI: 10.1029/98JD01162

The fragmentation and electrification of freezing water drops
journal, April 1960

  • Mason, B. J.; Maybank, J.
  • Quarterly Journal of the Royal Meteorological Society, Vol. 86, Issue 368
  • DOI: 10.1002/qj.49708636806

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.
  • Atmospheric Chemistry and Physics, Vol. 12, Issue 1
  • DOI: 10.5194/acp-12-287-2012