Articles | Volume 23, issue 10
https://doi.org/10.5194/acp-23-5623-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-23-5623-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
22 May 2023
Research article |
| 22 May 2023
| 22 May 2023
HUB: a method to model and extract the distribution of ice nucleation temperatures from drop-freezing experiments
Ingrid de Almeida Ribeiro
Department of Chemistry, The University of Utah, 315 South 1400 East,
Salt Lake City, Utah 84112-0850, USA
Konrad Meister
Max Planck Institute for Polymer Research, 55128 Mainz, Germany
Department of Chemistry and Biochemistry, Boise State University,
Boise, Idaho 83725, USA
Valeria Molinero
CORRESPONDING AUTHOR
Department of Chemistry, The University of Utah, 315 South 1400 East,
Salt Lake City, Utah 84112-0850, USA
Related authors
Ravi Kumar Reddy Addula, Ingrid de Almeida Ribeiro, Valeria Molinero, and Baron Peters
Atmos. Chem. Phys., 24, 10833–10848, https://doi.org/10.5194/acp-24-10833-2024, https://doi.org/10.5194/acp-24-10833-2024, 2024
Short summary
Short summary
Ice nucleation from supercooled droplets is important in many weather and climate modeling efforts. For experiments where droplets are steadily supercooled from the freezing point, our work combines nucleation theory and survival probability analysis to predict the nucleation spectrum, i.e., droplet freezing probabilities vs. temperature. We use the new framework to extract approximately consistent rate parameters from experiments with different cooling rates and droplet sizes.
Rosemary J. Eufemio, Ingrid de Almeida Ribeiro, Todd L. Sformo, Gary A. Laursen, Valeria Molinero, Janine Fröhlich-Nowoisky, Mischa Bonn, and Konrad Meister
Biogeosciences, 20, 2805–2812, https://doi.org/10.5194/bg-20-2805-2023, https://doi.org/10.5194/bg-20-2805-2023, 2023
Short summary
Short summary
Lichens, the dominant vegetation in the Arctic, contain ice nucleators (INs) that enable freezing close to 0°C. Yet the abundance, diversity, and function of lichen INs is unknown. Our screening of lichens across Alaska reveal that most species have potent INs. We find that lichens contain two IN populations which retain activity under environmentally relevant conditions. The ubiquity and stability of lichen INs suggest that they may have considerable impacts on local atmospheric patterns.
Julia Canet, Laura Rodriguez, Galit Renzer, Pura Alfonso, Mischa Bonn, Konrad Meister, Maite Garcia-Valles, and Albert Verdaguer
EGUsphere, https://doi.org/10.5194/egusphere-2025-5014, https://doi.org/10.5194/egusphere-2025-5014, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Alkali-feldspars are known to be efficient ice-nucleating particles. Analysis on the efficiency of perthite feldspars show that it depends on crystallographic structure rather than composition. Microcline-perthites displayed a continuous increase in active site density as temperature was cooled down, while orthoclase showed plateaus, reflecting interruptions in the increase of activity with temperature. These results suggest that order enhances while disorder limits ice nucleation activation.
Rosemary J. Eufemio, Galit Renzer, Mariah Rojas, Jolanta Miadlikowska, Todd L. Sformo, François Lutzoni, Boris A. Vinatzer, and Konrad Meister
Biogeosciences, 22, 2087–2096, https://doi.org/10.5194/bg-22-2087-2025, https://doi.org/10.5194/bg-22-2087-2025, 2025
Short summary
Short summary
Biological ice nucleation plays key roles in organism survival and in shaping Earth’s atmospheric patterns. Our pan-American screening of Peltigera lichens reveals that the lichen thalli produce highly active ice nucleators (INs) resistant to freeze–thaw cycles. Notably, a pure fungal culture from Peltigera britannica released the most potent INs reported to date. Given the global abundance of these lichens, the INs may be important contributors to atmospheric processes.
Florian Wieland, Nadine Bothen, Ralph Schwidetzky, Teresa M. Seifried, Paul Bieber, Ulrich Pöschl, Konrad Meister, Mischa Bonn, Janine Fröhlich-Nowoisky, and Hinrich Grothe
Biogeosciences, 22, 103–115, https://doi.org/10.5194/bg-22-103-2025, https://doi.org/10.5194/bg-22-103-2025, 2025
Short summary
Short summary
Betula pendula is a widespread birch tree species containing ice nucleation agents that can trigger the freezing of cloud droplets and thereby alter the evolution of clouds. Our study identifies three distinct ice-nucleating macromolecule (INM) aggregates of varying size that can nucleate ice at temperatures up to –5.4°C. Our findings suggest that these vegetation-derived particles may influence atmospheric processes, weather, and climate more strongly than previously thought.
Ravi Kumar Reddy Addula, Ingrid de Almeida Ribeiro, Valeria Molinero, and Baron Peters
Atmos. Chem. Phys., 24, 10833–10848, https://doi.org/10.5194/acp-24-10833-2024, https://doi.org/10.5194/acp-24-10833-2024, 2024
Short summary
Short summary
Ice nucleation from supercooled droplets is important in many weather and climate modeling efforts. For experiments where droplets are steadily supercooled from the freezing point, our work combines nucleation theory and survival probability analysis to predict the nucleation spectrum, i.e., droplet freezing probabilities vs. temperature. We use the new framework to extract approximately consistent rate parameters from experiments with different cooling rates and droplet sizes.
Rosemary J. Eufemio, Ingrid de Almeida Ribeiro, Todd L. Sformo, Gary A. Laursen, Valeria Molinero, Janine Fröhlich-Nowoisky, Mischa Bonn, and Konrad Meister
Biogeosciences, 20, 2805–2812, https://doi.org/10.5194/bg-20-2805-2023, https://doi.org/10.5194/bg-20-2805-2023, 2023
Short summary
Short summary
Lichens, the dominant vegetation in the Arctic, contain ice nucleators (INs) that enable freezing close to 0°C. Yet the abundance, diversity, and function of lichen INs is unknown. Our screening of lichens across Alaska reveal that most species have potent INs. We find that lichens contain two IN populations which retain activity under environmentally relevant conditions. The ubiquity and stability of lichen INs suggest that they may have considerable impacts on local atmospheric patterns.
Cited articles
Alpert, P. A. and Knopf, D. A.: Analysis of isothermal and cooling-rate-dependent immersion freezing by a unifying stochastic ice nucleation model, Atmos. Chem. Phys., 16, 2083–2107, https://doi.org/10.5194/acp-16-2083-2016, 2016.
Augustin, S., Wex, H., Niedermeier, D., Pummer, B., Grothe, H., Hartmann, S., Tomsche, L., Clauss, T., Voigtländer, J., Ignatius, K., and Stratmann, F.: Immersion freezing of birch pollen washing water, Atmos. Chem. Phys., 13, 10989–11003, https://doi.org/10.5194/acp-13-10989-2013, 2013.
Bigg, E.: The formation of atmospheric ice crystals by the freezing of
droplets, Q. J. Roy. Meteor. Soc., 79,
510–519, 1953.
Bogler, S. and Borduas-Dedekind, N.: Lignin's ability to nucleate ice via immersion freezing and its stability towards physicochemical treatments and atmospheric processing, Atmos. Chem. Phys., 20, 14509–14522, https://doi.org/10.5194/acp-20-14509-2020, 2020.
Broadley, S. L., Murray, B. J., Herbert, R. J., Atkinson, J. D., Dobbie, S., Malkin, T. L., Condliffe, E., and Neve, L.: Immersion mode heterogeneous ice nucleation by an illite rich powder representative of atmospheric mineral dust, Atmos. Chem. Phys., 12, 287–307, https://doi.org/10.5194/acp-12-287-2012, 2012.
Budke, C. and Koop, T.: BINARY: an optical freezing array for assessing temperature and time dependence of heterogeneous ice nucleation, Atmos. Meas. Tech., 8, 689–703, https://doi.org/10.5194/amt-8-689-2015, 2015.
Carte, A.: The freezing of water droplets, P. Phys.
Soc. B, 69, 1028–1037, 1956.
Castillo, E., Hadi, A. S., Balakrishnan, N., and Sarabia, J. M.: Extreme value and related
models in engineering and science applications, John Wiley & Sons, New York, 179,
ISBN 9780471671725, 2005.
Creamean, J. M., Mignani, C., Bukowiecki, N., and Conen, F.: Using freezing spectra characteristics to identify ice-nucleating particle populations during the winter in the Alps, Atmos. Chem. Phys., 19, 8123–8140, https://doi.org/10.5194/acp-19-8123-2019, 2019.
David, H. A. and Nagaraja, H. N.: Order Statistics. Wiley, ISBN 9780471654018, 2004.
de Almeida Ribeiro, I., Meister, K., and Molinero, V.: Codes and data for “HUB: a method to model and extract the distribution of ice nucleation temperatures from drop-freezing experiments” (v1.0), Zenodo [code and data set], https://doi.org/10.5281/zenodo.7901549, 2023.
de Haan, L. and Ferreira, A.: Extreme Value Theory: An Introduction, Springer New
York, ISBN 9780387344713, 2007.
DeMott, P. J., Cziczo, D. J., Prenni, A. J., Murphy, D. M., Kreidenweis, S.
M., Thomson, D. S., Borys, R., and Rogers, D. C.: Measurements of the
concentration and composition of nuclei for cirrus formation, P. Natl. Acad. Sci. USA, 100, 14655–14660,
https://doi.org/10.1073/pnas.2532677100, 2003.
DeMott, P. J., Hill, T. C. J., McCluskey, C. S., Prather, K. A., Collins, D.
B., Sullivan, R. C., Ruppel, M. J., Mason, R. H., Irish, V. E., Lee, T.,
Hwang, C. Y., Rhee, T. S., Snider, J. R., McMeeking, G. R., Dhaniyala, S.,
Lewis, E. R., Wentzell, J. J. B., Abbatt, J., Lee, C., Sultana, C. M., Ault,
A. P., Axson, J. L., Martinez, M. D., Venero, I., Santos-Figueroa, G.,
Stokes, M. D., Deane, G. B., Mayol-Bracero, O. L., Grassian, V. H., Bertram,
T. H., Bertram, A. K., Moffett, B. F., and Franc, G. D.: Sea spray aerosol
as a unique source of ice nucleating particles, P. Natl.
Acad. Sci. USA, 113, 5797–5803, https://doi.org/10.1073/pnas.1514034112, 2016.
Dreischmeier, K.: Heterogene Eisnukleations- und Antigefriereigenschaften
von Biomolekülen, Bielefeld University,
https://doi.org/10.4119/unibi/2907691, 2019.
Fahy, W. D., Maters, E. C., Giese Miranda, R., Adams, M. P., Jahn, L. G.,
Sullivan, R. C., and Murray, B. J.: Volcanic ash ice nucleation activity is
variably reduced by aging in water and sulfuric acid: the effects of
leaching, dissolution, and precipitation, Environ. Sci.-Atmos., 2, 85–99, https://doi.org/10.1039/D1EA00071C, 2022a.
Fahy, W. D., Shalizi, C. R., and Sullivan, R. C.: A universally applicable method of calculating confidence bands for ice nucleation spectra derived from droplet freezing experiments, Atmos. Meas. Tech., 15, 6819–6836, https://doi.org/10.5194/amt-15-6819-2022, 2022b.
Felgitsch, L., Baloh, P., Burkart, J., Mayr, M., Momken, M. E., Seifried, T. M., Winkler, P., Schmale III, D. G., and Grothe, H.: Birch leaves and branches as a source of ice-nucleating macromolecules, Atmos. Chem. Phys., 18, 16063–16079, https://doi.org/10.5194/acp-18-16063-2018, 2018.
Fletcher, N. H.: Active sites and ice crystal nucleation, J.
Atmos. Sci., 26, 1266–1271, 1969.
Froyd, K. D., Yu, P., Schill, G. P., Brock, C. A., Kupc, A., Williamson, C.
J., Jensen, E. J., Ray, E., Rosenlof, K. H., Bian, H., Darmenov, A. S.,
Colarco, P. R., Diskin, G. S., Bui, T., and Murphy, D. M.: Dominant role of
mineral dust in cirrus cloud formation revealed by global-scale
measurements, Nat. Geosci., 15, 177–183, https://doi.org/10.1038/s41561-022-00901-w,
2022.
Gettelman, A., Liu, X., Barahona, D., Lohmann, U., and Chen, C.: Climate
impacts of ice nucleation, J. Geophys. Res.-Atmos.,
117, D20201, https://doi.org/10.1029/2012JD017950, 2012.
Govindarajan, A. G. and Lindow, S. E.: Size of bacterial ice-nucleation
sites measured in situ by
radiation inactivation analysis, P. Natl. Acad.
Sci. USA, 85, 1334–1338, https://doi.org/10.1073/pnas.85.5.1334, 1988.
Harrison, A. D., Whale, T. F., Carpenter, M. A., Holden, M. A., Neve, L., O'Sullivan, D., Vergara Temprado, J., and Murray, B. J.: Not all feldspars are equal: a survey of ice nucleating properties across the feldspar group of minerals, Atmos. Chem. Phys., 16, 10927–10940, https://doi.org/10.5194/acp-16-10927-2016, 2016.
Hartmann, S., Ling, M., Dreyer, L. S. A., Zipori, A., Finster, K., Grawe,
S., Jensen, L. Z., Borck, S., Reicher, N., Drace, T., Niedermeier, D.,
Jones, N. C., Hoffmann, S. V., Wex, H., Rudich, Y., Boesen, T., and
Šantl-Temkiv, T.: Structure and Protein-Protein Interactions of Ice
Nucleation Proteins Drive Their Activity, bioRxiv, 2022.2001.2021.477219,
https://doi.org/10.1101/2022.01.21.477219, 2022.
Herbert, R. J., Murray, B. J., Whale, T. F., Dobbie, S. J., and Atkinson, J. D.: Representing time-dependent freezing behaviour in immersion mode ice nucleation, Atmos. Chem. Phys., 14, 8501–8520, https://doi.org/10.5194/acp-14-8501-2014, 2014.
Knopf, D. A., Alpert, P. A., Zipori, A., Reicher, N., and Rudich, Y.:
Stochastic nucleation processes and substrate abundance explain
time-dependent freezing in supercooled droplets, NPJ Climate and Atmospheric
Science, 3, 2, https://doi.org/10.1038/s41612-020-0106-4, 2020.
Kunert, A. T., Lamneck, M., Helleis, F., Pöschl, U., Pöhlker, M. L., and Fröhlich-Nowoisky, J.: Twin-plate Ice Nucleation Assay (TINA) with infrared detection for high-throughput droplet freezing experiments with biological ice nuclei in laboratory and field samples, Atmos. Meas. Tech., 11, 6327–6337, https://doi.org/10.5194/amt-11-6327-2018, 2018.
Kunert, A. T., Pöhlker, M. L., Tang, K., Krevert, C. S., Wieder, C., Speth, K. R., Hanson, L. E., Morris, C. E., Schmale III, D. G., Pöschl, U., and Fröhlich-Nowoisky, J.: Macromolecular fungal ice nuclei in Fusarium: effects of physical and chemical processing, Biogeosciences, 16, 4647–4659, https://doi.org/10.5194/bg-16-4647-2019, 2019.
Levine, J.: Statistical explanation of spontaneous freezing of water droplets, NACA Tech.
Note, 2234, 1950.
Lukas, M., Schwidetzky, R., Kunert, A. T., Pöschl, U.,
Fröhlich-Nowoisky, J., Bonn, M., and Meister, K.: Electrostatic
Interactions Control the Functionality of Bacterial Ice Nucleators, J. Am. Chem. Soc., 142, 6842–6846, https://doi.org/10.1021/jacs.9b13069,
2020.
Lukas, M., Schwidetzky, R., Eufemio, R. J., Bonn, M., and Meister, K.:
Toward Understanding Bacterial Ice Nucleation, J. Phys.
Chem. B, 126, 1861–1867, https://doi.org/10.1021/acs.jpcb.1c09342, 2022.
Marcolli, C., Gedamke, S., Peter, T., and Zobrist, B.: Efficiency of immersion mode ice nucleation on surrogates of mineral dust, Atmos. Chem. Phys., 7, 5081–5091, https://doi.org/10.5194/acp-7-5081-2007, 2007.
Miller, A. J., Brennan, K. P., Mignani, C., Wieder, J., David, R. O., and Borduas-Dedekind, N.: Development of the drop Freezing Ice Nuclei Counter (FINC), intercomparison of droplet freezing techniques, and use of soluble lignin as an atmospheric ice nucleation standard, Atmos. Meas. Tech., 14, 3131–3151, https://doi.org/10.5194/amt-14-3131-2021, 2021.
Mülmenstädt, J., Sourdeval, O., Delanoë, J., and Quaas, J.:
Frequency of occurrence of rain from liquid-, mixed-, and ice-phase clouds
derived from A-Train satellite retrievals, Geophys. Res. Lett., 42,
6502–6509, https://doi.org/10.1002/2015GL064604, 2015.
Murray, B. J., Broadley, S. L., Wilson, T. W., Atkinson, J. D., and Wills, R. H.: Heterogeneous freezing of water droplets containing kaolinite particles, Atmos. Chem. Phys., 11, 4191–4207, https://doi.org/10.5194/acp-11-4191-2011, 2011.
Murray, B. J., O'Sullivan, D., Atkinson, J. D., and Webb, M. E.: Ice
nucleation by particles immersed in supercooled cloud droplets, Chem.
Soc. Rev., 41, 6519–6554, https://doi.org/10.1039/C2CS35200A, 2012.
Niedermeier, D., Shaw, R. A., Hartmann, S., Wex, H., Clauss, T., Voigtländer, J., and Stratmann, F.: Heterogeneous ice nucleation: exploring the transition from stochastic to singular freezing behavior, Atmos. Chem. Phys., 11, 8767–8775, https://doi.org/10.5194/acp-11-8767-2011, 2011.
Pummer, B. G., Bauer, H., Bernardi, J., Bleicher, S., and Grothe, H.: Suspendable macromolecules are responsible for ice nucleation activity of birch and conifer pollen, Atmos. Chem. Phys., 12, 2541–2550, https://doi.org/10.5194/acp-12-2541-2012, 2012.
Reicher, N., Segev, L., and Rudich, Y.: The WeIzmann Supercooled Droplets Observation on a Microarray (WISDOM) and application for ambient dust, Atmos. Meas. Tech., 11, 233–248, https://doi.org/10.5194/amt-11-233-2018, 2018.
Satopaa, V., Albrecht, J., Irwin, D., and Raghavan, B.: Finding a “Kneedle”
in a Haystack: Detecting Knee Points in System Behavior, 2011 31st
International Conference on Distributed Computing Systems Workshops, 20–24
June 2011, 166–171, https://doi.org/10.1109/ICDCSW.2011.20, 2011.
Schwidetzky, R., Sudera, P., Backes, A. T., Pöschl, U., Bonn, M.,
Fröhlich-Nowoisky, J., and Meister, K.: Membranes Are Decisive for
Maximum Freezing Efficiency of Bacterial Ice Nucleators, J.
Phys. Chem. Lett., 12, 10783–10787, https://doi.org/10.1021/acs.jpclett.1c03118,
2021.
Schwidetzky, R., de Almeida Ribeiro, I., Bothen, N., Backes, A., DeVries, A.
L., Bonn, M., Frhlich-Nowoisky, J., Molinero, V., and Meister, K.: E
Pluribus Unum: Functional Aggregation Enables Biological Ice Nucleation, ChemRxiv, Cambridge Open Engage, Cambridge, https://doi.org/10.26434/chemrxiv-2023-63qfl,
2023.
Sear, R. P.: Generalisation of Levine's prediction for the distribution of freezing temperatures of droplets: a general singular model for ice nucleation, Atmos. Chem. Phys., 13, 7215–7223, https://doi.org/10.5194/acp-13-7215-2013, 2013.
Steinke, I., Hiranuma, N., Funk, R., Höhler, K., Tüllmann, N., Umo, N. S., Weidler, P. G., Möhler, O., and Leisner, T.: Complex plant-derived organic aerosol as ice-nucleating particles – more than the sums of their parts?, Atmos. Chem. Phys., 20, 11387–11397, https://doi.org/10.5194/acp-20-11387-2020, 2020.
Stratmann, F., Kiselev, A., Wurzler, S., Wendisch, M., Heintzenberg, J.,
Charlson, R. J., Diehl, K., Wex, H., and Schmidt, S.: Laboratory Studies and
Numerical Simulations of Cloud Droplet Formation under Realistic
Supersaturation Conditions, J. Atmos. Ocean. Tech.,
21, 876–887, https://doi.org/10.1175/1520-0426(2004)021<0876:Lsanso>2.0.Co;2, 2004.
Turner, M. A., Arellano, F., and Kozloff, L. M.: Three separate classes of
bacterial ice nucleation structures, J. Bacteriol., 172, 2521–2526,
https://doi.org/10.1128/jb.172.5.2521-2526.1990, 1990.
Vali, G.: Quantitative Evaluation of Experimental Results an the
Heterogeneous Freezing Nucleation of Supercooled Liquids, J.
Atmos. Sci., 28, 402–409, https://doi.org/10.1175/1520-0469(1971)028<0402:Qeoera>2.0.Co;2, 1971.
Vali, G.: Freezing rate due to heterogeneous nucleation, J.
Atmos. Sci., 51, 1843–1856, 1994.
Vali, G.: Interpretation of freezing nucleation experiments: singular and stochastic; sites and surfaces, Atmos. Chem. Phys., 14, 5271–5294, https://doi.org/10.5194/acp-14-5271-2014, 2014.
Vali, G.: Revisiting the differential freezing nucleus spectra derived from drop-freezing experiments: methods of calculation, applications, and confidence limits, Atmos. Meas. Tech., 12, 1219–1231, https://doi.org/10.5194/amt-12-1219-2019, 2019.
Vali, G. and Stansbury, E. J.: TIME-DEPENDENT CHARACTERISTICS OF THE
HETEROGENEOUS NUCLEATION OF ICE, Can. J. Phys., 44, 477–502,
https://doi.org/10.1139/p66-044, 1966.
Warren, G. J.: Bacterial Ice Nucleation: Molecular Biology and Applications,
Biotechnol. Genet. Eng., 5, 107–136,
https://doi.org/10.1080/02648725.1987.10647836, 1987.
Wright, T. P. and Petters, M. D.: The role of time in heterogeneous freezing
nucleation, J. Geophys. Res.-Atmos., 118, 3731–3743,
https://doi.org/10.1002/jgrd.50365, 2013.
Wright, T. P., Petters, M. D., Hader, J. D., Morton, T., and Holder, A. L.:
Minimal cooling rate dependence of ice nuclei activity in the immersion
mode, J. Geophys. Res.-Atmos., 118, 10535–10543,
https://doi.org/10.1002/jgrd.50810, 2013.
Zhang, X. and Maeda, N.: Nucleation curves of ice in the presence of
nucleation promoters, Chem. Eng. Sci., 262, 118017,
https://doi.org/10.1016/j.ces.2022.118017, 2022.
Zobrist, B., Koop, T., Luo, B., Marcolli, C., and Peter, T.: Heterogeneous
ice nucleation rate coefficient of water droplets coated by a nonadecanol
monolayer, J. Phys. Chem. C, 111, 2149–2155, 2007.
Short summary
Ice formation is a key atmospheric process facilitated by a wide range of aerosols. We present a method to model and interpret ice nucleation experiments and extract the distribution of the potency of nucleation sites. We use the method to optimize the conditions of laboratory sampling and extract distributions of ice nucleation temperatures from bacteria, fungi, and pollen. These reveal unforeseen subpopulations of nuclei in these systems and how they respond to changes in their environment.
Ice formation is a key atmospheric process facilitated by a wide range of aerosols. We present a...
Altmetrics
Final-revised paper
Preprint