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Title: The Fifth International Workshop on Ice Nucleation phase 2 (FIN-02): laboratory intercomparison of ice nucleation measurements

Abstract

The second phase of the Fifth International Ice Nucleation Workshop (FIN-02)involved the gathering of a large number of researchers at the Karlsruhe Institute of Technology's Aerosol Interactions and Dynamics of the Atmosphere(AIDA) facility to promote characterization and understanding of ice nucleation measurements made by a variety of methods used worldwide.Compared to the previous workshop in 2007, participation was doubled,reflecting a vibrant research area. Experimental methods involved sampling of aerosol particles by direct processing ice nucleation measuring systems from the same volume of air in separate experiments using different ice nucleating particle (INP) types, and collections of aerosol particle samples onto filters or into liquid for sharing amongst measurement techniques tha tpost-process these samples. In this manner, any errors introduced by differences in generation methods when samples are shared across laboratories were mitigated. Furthermore, as much as possible, aerosol particle size distribution was controlled so that the size limitations of different methods were minimized. The results presented here use data from the workshop to assess the comparability of immersion freezing measurement methods activating INPs in bulk suspensions, methods that activate INPs in condensation and/or immersion freezing modes as single particles on a substrate, continuous flow diffusion chambers (CFDCs) directly sampling andmore » processing particles well above water saturation to maximize immersion and subsequent freezing of aerosol particles, and expansion cloud chamber simulations in which liquid cloud droplets were first activated on aerosol particles prior to freezing.The AIDA expansion chamber measurements are expected to be the closest representation to INP activation in atmospheric cloud parcels in these comparisons, due to exposing particles freely to adiabatic cooling. The different particle types used as INPs included the minerals illite NX and potassium feldspar (K-feldspar), two natural soil dusts representative of arable sandy loam(Argentina) and highly erodible sandy dry land (Tunisia) soils, respectively,and a bacterial INP (Snomax®). Considered together, the agreement among post-processed immersion freezing measurements of the numbers and fractions of particles active at different temperatures following bulk collection of particles into liquid was excellent, with possible temperature uncertainties inferred to be a key factor in determining INP uncertainties. Collection onto filters for rinsing versus directly into liquid in impingers made little difference. For methods that activated collected single particles on a substrate at a controlled humidity at or above water saturation, agreement with immersion freezing methods was good inmost cases, but was biased low in a few others for reasons that have not been resolved, but could relate to water vapor competition effects. Amongst CFDC-style instruments, various factors requiring (variable) higher supersaturations to achieve equivalent immersion freezing activation dominate the uncertainty between these measurements, and for comparison with bulk immersion freezing methods. When operated above water saturation to include assessment of immersion freezing, CFDC measurements often measured at or above the upper bound of immersion freezing device measurements, but often underestimated INP concentration in comparison to an immersion freezing method that first activates all particles into liquid droplets prior to cooling (the PIMCA-PINC device, or Portable Immersion Mode Cooling chAmber–Portable Ice Nucleation Chamber), and typically slightly underestimated INP number concentrations in comparison to cloud parcel expansions in the AIDA chamber; this can be largely mitigated when it is possible to raise the relative humidity to sufficiently high values in the CFDCs, although this isnot always possible operationally. Correspondence of measurements of INPs among direct sampling and post-processing systems varied depending on the INP type. Agreement was best for Snomax® particles in the temperature regime colder than -10°C, where their ice nucleation activity is nearly maximized and changes very little with temperature. At temperatures warmer than-10°C, Snomax® INP measurements (all via freezing of suspensions) demonstrated discrepancies consistent with previous reports of the instability of its protein aggregates that appear to make it less suitable as a calibration INP at these temperatures. For Argentinian soil dust particles, there was excellent agreement across all measurement methods; measures ranged within 1 order of magnitude for INP number concentrations, active fractions and calculated active site densities over a 25 to 30°C range and 5 to 8 orders of corresponding magnitude change in number concentrations. This was also the case for all temperatures warmer than -25°C in Tunisian dust experiments. In contrast, discrepancies in measurements of INP concentrations or active site densities that exceeded 2 orders of magnitude across a broad range of temperature measurements found at temperatures warmer than -25°C in a previous study were replicated for illite NX. Discrepancies also exceeded 2 orders of magnitude at temperatures of -20 to -25°C for potassium feldspar (K-feldspar), but these coincided with the range of temperatures at which INP concentrations increase rapidly at approximately an order of magnitude per 2°C cooling forK-feldspar. These few discrepancies did not outweigh the overall positive outcomes of the workshop activity, nor the future utility of this data set or future similar efforts for resolving remaining measurement issues. Measurements of the same materials were repeatable over the time of the workshop and demonstrated strong consistency with prior studies, as reflected by agreement of data broadly with para meterizations of different specific or general (e.g., soil dust) aerosol types. The divergent measurements of the INP activity of illiteNX by direct versus post-processing methods were not repeated for other particle types, and the Snomax® data demonstrated that, at least for a biological INP type, there is no expected measurement bias between bulk collection and direct immediately processed freezing methods to as warm as -10°C. Since particle size ranges were limited for this workshop, it can be expected that for atmospheric populations of INPs, measurement discrepancies will appear due to the different capabilities of methods for sampling the full aerosol size distribution, or due to limitations on achieving sufficient water supersaturations to fully capture immersion freezing in direct processing instruments. Overall, this workshop presents an improved picture of present capabilities for measuring INPs than in past workshops, and provides direction toward addressing remaining measurement issues.« less

Authors:
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Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1482744
Alternate Identifier(s):
OSTI ID: 1508243
Report Number(s):
PNNL-SA-141072
Journal ID: ISSN 1867-8548
Grant/Contract Number:  
SC0014487; AC05-76RL01830
Resource Type:
Published Article
Journal Name:
Atmospheric Measurement Techniques (Online)
Additional Journal Information:
Journal Name: Atmospheric Measurement Techniques (Online) Journal Volume: 11 Journal Issue: 11; Journal ID: ISSN 1867-8548
Publisher:
Copernicus Publications, EGU
Country of Publication:
Germany
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

DeMott, Paul J., Möhler, Ottmar, Cziczo, Daniel J., Hiranuma, Naruki, Petters, Markus D., Petters, Sarah S., Belosi, Franco, Bingemer, Heinz G., Brooks, Sarah D., Budke, Carsten, Burkert-Kohn, Monika, Collier, Kristen N., Danielczok, Anja, Eppers, Oliver, Felgitsch, Laura, Garimella, Sarvesh, Grothe, Hinrich, Herenz, Paul, Hill, Thomas C. J., Höhler, Kristina, Kanji, Zamin A., Kiselev, Alexei, Koop, Thomas, Kristensen, Thomas B., Krüger, Konstantin, Kulkarni, Gourihar, Levin, Ezra J. T., Murray, Benjamin J., Nicosia, Alessia, O'Sullivan, Daniel, Peckhaus, Andreas, Polen, Michael J., Price, Hannah C., Reicher, Naama, Rothenberg, Daniel A., Rudich, Yinon, Santachiara, Gianni, Schiebel, Thea, Schrod, Jann, Seifried, Teresa M., Stratmann, Frank, Sullivan, Ryan C., Suski, Kaitlyn J., Szakáll, Miklós, Taylor, Hans P., Ullrich, Romy, Vergara-Temprado, Jesus, Wagner, Robert, Whale, Thomas F., Weber, Daniel, Welti, André, Wilson, Theodore W., Wolf, Martin J., and Zenker, Jake. The Fifth International Workshop on Ice Nucleation phase 2 (FIN-02): laboratory intercomparison of ice nucleation measurements. Germany: N. p., 2018. Web. doi:10.5194/amt-11-6231-2018.
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DeMott, Paul J., Möhler, Ottmar, Cziczo, Daniel J., Hiranuma, Naruki, Petters, Markus D., Petters, Sarah S., Belosi, Franco, Bingemer, Heinz G., Brooks, Sarah D., Budke, Carsten, Burkert-Kohn, Monika, Collier, Kristen N., Danielczok, Anja, Eppers, Oliver, Felgitsch, Laura, Garimella, Sarvesh, Grothe, Hinrich, Herenz, Paul, Hill, Thomas C. J., Höhler, Kristina, Kanji, Zamin A., Kiselev, Alexei, Koop, Thomas, Kristensen, Thomas B., Krüger, Konstantin, Kulkarni, Gourihar, Levin, Ezra J. T., Murray, Benjamin J., Nicosia, Alessia, O'Sullivan, Daniel, Peckhaus, Andreas, Polen, Michael J., Price, Hannah C., Reicher, Naama, Rothenberg, Daniel A., Rudich, Yinon, Santachiara, Gianni, Schiebel, Thea, Schrod, Jann, Seifried, Teresa M., Stratmann, Frank, Sullivan, Ryan C., Suski, Kaitlyn J., Szakáll, Miklós, Taylor, Hans P., Ullrich, Romy, Vergara-Temprado, Jesus, Wagner, Robert, Whale, Thomas F., Weber, Daniel, Welti, André, Wilson, Theodore W., Wolf, Martin J., & Zenker, Jake. The Fifth International Workshop on Ice Nucleation phase 2 (FIN-02): laboratory intercomparison of ice nucleation measurements. Germany. https://doi.org/10.5194/amt-11-6231-2018
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DeMott, Paul J., Möhler, Ottmar, Cziczo, Daniel J., Hiranuma, Naruki, Petters, Markus D., Petters, Sarah S., Belosi, Franco, Bingemer, Heinz G., Brooks, Sarah D., Budke, Carsten, Burkert-Kohn, Monika, Collier, Kristen N., Danielczok, Anja, Eppers, Oliver, Felgitsch, Laura, Garimella, Sarvesh, Grothe, Hinrich, Herenz, Paul, Hill, Thomas C. J., Höhler, Kristina, Kanji, Zamin A., Kiselev, Alexei, Koop, Thomas, Kristensen, Thomas B., Krüger, Konstantin, Kulkarni, Gourihar, Levin, Ezra J. T., Murray, Benjamin J., Nicosia, Alessia, O'Sullivan, Daniel, Peckhaus, Andreas, Polen, Michael J., Price, Hannah C., Reicher, Naama, Rothenberg, Daniel A., Rudich, Yinon, Santachiara, Gianni, Schiebel, Thea, Schrod, Jann, Seifried, Teresa M., Stratmann, Frank, Sullivan, Ryan C., Suski, Kaitlyn J., Szakáll, Miklós, Taylor, Hans P., Ullrich, Romy, Vergara-Temprado, Jesus, Wagner, Robert, Whale, Thomas F., Weber, Daniel, Welti, André, Wilson, Theodore W., Wolf, Martin J., and Zenker, Jake. Mon . "The Fifth International Workshop on Ice Nucleation phase 2 (FIN-02): laboratory intercomparison of ice nucleation measurements". Germany. https://doi.org/10.5194/amt-11-6231-2018.
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@article{osti_1482744,
title = {The Fifth International Workshop on Ice Nucleation phase 2 (FIN-02): laboratory intercomparison of ice nucleation measurements},
author = {DeMott, Paul J. and Möhler, Ottmar and Cziczo, Daniel J. and Hiranuma, Naruki and Petters, Markus D. and Petters, Sarah S. and Belosi, Franco and Bingemer, Heinz G. and Brooks, Sarah D. and Budke, Carsten and Burkert-Kohn, Monika and Collier, Kristen N. and Danielczok, Anja and Eppers, Oliver and Felgitsch, Laura and Garimella, Sarvesh and Grothe, Hinrich and Herenz, Paul and Hill, Thomas C. J. and Höhler, Kristina and Kanji, Zamin A. and Kiselev, Alexei and Koop, Thomas and Kristensen, Thomas B. and Krüger, Konstantin and Kulkarni, Gourihar and Levin, Ezra J. T. and Murray, Benjamin J. and Nicosia, Alessia and O'Sullivan, Daniel and Peckhaus, Andreas and Polen, Michael J. and Price, Hannah C. and Reicher, Naama and Rothenberg, Daniel A. and Rudich, Yinon and Santachiara, Gianni and Schiebel, Thea and Schrod, Jann and Seifried, Teresa M. and Stratmann, Frank and Sullivan, Ryan C. and Suski, Kaitlyn J. and Szakáll, Miklós and Taylor, Hans P. and Ullrich, Romy and Vergara-Temprado, Jesus and Wagner, Robert and Whale, Thomas F. and Weber, Daniel and Welti, André and Wilson, Theodore W. and Wolf, Martin J. and Zenker, Jake},
abstractNote = {The second phase of the Fifth International Ice Nucleation Workshop (FIN-02)involved the gathering of a large number of researchers at the Karlsruhe Institute of Technology's Aerosol Interactions and Dynamics of the Atmosphere(AIDA) facility to promote characterization and understanding of ice nucleation measurements made by a variety of methods used worldwide.Compared to the previous workshop in 2007, participation was doubled,reflecting a vibrant research area. Experimental methods involved sampling of aerosol particles by direct processing ice nucleation measuring systems from the same volume of air in separate experiments using different ice nucleating particle (INP) types, and collections of aerosol particle samples onto filters or into liquid for sharing amongst measurement techniques tha tpost-process these samples. In this manner, any errors introduced by differences in generation methods when samples are shared across laboratories were mitigated. Furthermore, as much as possible, aerosol particle size distribution was controlled so that the size limitations of different methods were minimized. The results presented here use data from the workshop to assess the comparability of immersion freezing measurement methods activating INPs in bulk suspensions, methods that activate INPs in condensation and/or immersion freezing modes as single particles on a substrate, continuous flow diffusion chambers (CFDCs) directly sampling and processing particles well above water saturation to maximize immersion and subsequent freezing of aerosol particles, and expansion cloud chamber simulations in which liquid cloud droplets were first activated on aerosol particles prior to freezing.The AIDA expansion chamber measurements are expected to be the closest representation to INP activation in atmospheric cloud parcels in these comparisons, due to exposing particles freely to adiabatic cooling. The different particle types used as INPs included the minerals illite NX and potassium feldspar (K-feldspar), two natural soil dusts representative of arable sandy loam(Argentina) and highly erodible sandy dry land (Tunisia) soils, respectively,and a bacterial INP (Snomax®). Considered together, the agreement among post-processed immersion freezing measurements of the numbers and fractions of particles active at different temperatures following bulk collection of particles into liquid was excellent, with possible temperature uncertainties inferred to be a key factor in determining INP uncertainties. Collection onto filters for rinsing versus directly into liquid in impingers made little difference. For methods that activated collected single particles on a substrate at a controlled humidity at or above water saturation, agreement with immersion freezing methods was good inmost cases, but was biased low in a few others for reasons that have not been resolved, but could relate to water vapor competition effects. Amongst CFDC-style instruments, various factors requiring (variable) higher supersaturations to achieve equivalent immersion freezing activation dominate the uncertainty between these measurements, and for comparison with bulk immersion freezing methods. When operated above water saturation to include assessment of immersion freezing, CFDC measurements often measured at or above the upper bound of immersion freezing device measurements, but often underestimated INP concentration in comparison to an immersion freezing method that first activates all particles into liquid droplets prior to cooling (the PIMCA-PINC device, or Portable Immersion Mode Cooling chAmber–Portable Ice Nucleation Chamber), and typically slightly underestimated INP number concentrations in comparison to cloud parcel expansions in the AIDA chamber; this can be largely mitigated when it is possible to raise the relative humidity to sufficiently high values in the CFDCs, although this isnot always possible operationally. Correspondence of measurements of INPs among direct sampling and post-processing systems varied depending on the INP type. Agreement was best for Snomax® particles in the temperature regime colder than -10°C, where their ice nucleation activity is nearly maximized and changes very little with temperature. At temperatures warmer than-10°C, Snomax® INP measurements (all via freezing of suspensions) demonstrated discrepancies consistent with previous reports of the instability of its protein aggregates that appear to make it less suitable as a calibration INP at these temperatures. For Argentinian soil dust particles, there was excellent agreement across all measurement methods; measures ranged within 1 order of magnitude for INP number concentrations, active fractions and calculated active site densities over a 25 to 30°C range and 5 to 8 orders of corresponding magnitude change in number concentrations. This was also the case for all temperatures warmer than -25°C in Tunisian dust experiments. In contrast, discrepancies in measurements of INP concentrations or active site densities that exceeded 2 orders of magnitude across a broad range of temperature measurements found at temperatures warmer than -25°C in a previous study were replicated for illite NX. Discrepancies also exceeded 2 orders of magnitude at temperatures of -20 to -25°C for potassium feldspar (K-feldspar), but these coincided with the range of temperatures at which INP concentrations increase rapidly at approximately an order of magnitude per 2°C cooling forK-feldspar. These few discrepancies did not outweigh the overall positive outcomes of the workshop activity, nor the future utility of this data set or future similar efforts for resolving remaining measurement issues. Measurements of the same materials were repeatable over the time of the workshop and demonstrated strong consistency with prior studies, as reflected by agreement of data broadly with para meterizations of different specific or general (e.g., soil dust) aerosol types. The divergent measurements of the INP activity of illiteNX by direct versus post-processing methods were not repeated for other particle types, and the Snomax® data demonstrated that, at least for a biological INP type, there is no expected measurement bias between bulk collection and direct immediately processed freezing methods to as warm as -10°C. Since particle size ranges were limited for this workshop, it can be expected that for atmospheric populations of INPs, measurement discrepancies will appear due to the different capabilities of methods for sampling the full aerosol size distribution, or due to limitations on achieving sufficient water supersaturations to fully capture immersion freezing in direct processing instruments. Overall, this workshop presents an improved picture of present capabilities for measuring INPs than in past workshops, and provides direction toward addressing remaining measurement issues.},
doi = {10.5194/amt-11-6231-2018},
journal = {Atmospheric Measurement Techniques (Online)},
number = 11,
volume = 11,
place = {Germany},
year = {Mon Jan 01 00:00:00 EST 2018},
month = {Mon Jan 01 00:00:00 EST 2018}
}
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journal, February 2018

  • Price, H. C.; Baustian, K. J.; McQuaid, J. B.
  • Journal of Geophysical Research: Atmospheres, Vol. 123, Issue 4
  • DOI: 10.1002/2017JD027560

Leipzig Ice Nucleation chamber Comparison (LINC): intercomparison of four online ice nucleation counters
journal, January 2017

  • Burkert-Kohn, Monika; Wex, Heike; Welti, André
  • Atmospheric Chemistry and Physics, Vol. 17, Issue 18
  • DOI: 10.5194/acp-17-11683-2017

Ice nuclei properties within a Saharan dust event at the Jungfraujoch in the Swiss Alps
journal, January 2011

  • Chou, C.; Stetzer, O.; Weingartner, E.
  • Atmospheric Chemistry and Physics, Vol. 11, Issue 10
  • DOI: 10.5194/acp-11-4725-2011

Atmospheric particles acting as Ice Forming Nuclei in different size ranges
journal, May 2010

Intercomparing different devices for the investigation of ice nucleating particles using Snomax ® as test substance
journal, January 2015

  • Wex, H.; Augustin-Bauditz, S.; Boose, Y.
  • Atmospheric Chemistry and Physics, Vol. 15, Issue 3
  • DOI: 10.5194/acp-15-1463-2015

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

Characterization of iron oxides in mineral dust aerosols: Implications for light absorption
journal, January 2006

  • Lafon, Sandra; Sokolik, Irina N.; Rajot, Jean Louis
  • Journal of Geophysical Research, Vol. 111, Issue D21
  • DOI: 10.1029/2005JD007016

Measurement of concentrations of natural ice nuclei
journal, June 1990

Sources of organic ice nucleating particles in soils
journal, January 2016

  • Hill, Tom C. J.; DeMott, Paul J.; Tobo, Yutaka
  • Atmospheric Chemistry and Physics, Vol. 16, Issue 11
  • DOI: 10.5194/acp-16-7195-2016

Influence of surface morphology on the immersion mode ice nucleation efficiency of hematite particles
journal, January 2014

  • Hiranuma, N.; Hoffmann, N.; Kiselev, A.
  • Atmospheric Chemistry and Physics, Vol. 14, Issue 5
  • DOI: 10.5194/acp-14-2315-2014

Deposition nucleation viewed as homogeneous or immersion freezing in pores and cavities
journal, January 2014

Ice nucleation by fertile soil dusts: relative importance of mineral and biogenic components
journal, January 2014

  • O'Sullivan, D.; Murray, B. J.; Malkin, T. L.
  • Atmospheric Chemistry and Physics, Vol. 14, Issue 4
  • DOI: 10.5194/acp-14-1853-2014

Re-evaluating the Frankfurt isothermal static diffusion chamber for ice nucleation
journal, January 2016

  • Schrod, Jann; Danielczok, Anja; Weber, Daniel
  • Atmospheric Measurement Techniques, Vol. 9, Issue 3
  • DOI: 10.5194/amt-9-1313-2016

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

A technique for quantifying heterogeneous ice nucleation in microlitre supercooled water droplets
journal, January 2015

  • Whale, T. F.; Murray, B. J.; O'Sullivan, D.
  • Atmospheric Measurement Techniques, Vol. 8, Issue 6
  • DOI: 10.5194/amt-8-2437-2015

Single ice crystal measurements during nucleation experiments with the depolarization detector IODE
journal, January 2010

  • Nicolet, M.; Stetzer, O.; Lüönd, F.
  • Atmospheric Chemistry and Physics, Vol. 10, Issue 2
  • DOI: 10.5194/acp-10-313-2010

Single Particle Measurements of the Optical Properties of Small Ice Crystals and Heterogeneous Ice Nuclei
journal, October 2014

Laboratory studies of immersion and deposition mode ice nucleation of ozone aged mineral dust particles
journal, January 2013

Using depolarization to quantify ice nucleating particle concentrations: a new method
journal, January 2017

  • Zenker, Jake; Collier, Kristen N.; Xu, Guanglang
  • Atmospheric Measurement Techniques, Vol. 10, Issue 12
  • DOI: 10.5194/amt-10-4639-2017

The role of time in heterogeneous freezing nucleation: ROLE OF TIME IN ICE NUCLEATION
journal, May 2013

  • Wright, Timothy P.; Petters, Markus D.
  • Journal of Geophysical Research: Atmospheres, Vol. 118, Issue 9
  • DOI: 10.1002/jgrd.50365
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