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© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 14 Sep 2018

Research article | 14 Sep 2018

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This discussion paper is a preprint. A revision of the manuscript is under review for the journal Atmospheric Chemistry and Physics (ACP).

A comprehensive characterization of ice nucleation by three different types of cellulose particles immersed in water: lessons learned and future research directions

Naruki Hiranuma1, Kouji Adachi2, David Bell3,a, Franco Belosi4, Hassan Beydoun5, Bhaskar Bhaduri6,b, Heinz Bingemer7, Carsten Budke8, Hans-Christian Clemen9, Franz Conen10, Kimberly Cory1, Joachim Curtius7, Paul DeMott11, Oliver Eppers12, Sarah Grawe13, Susan Hartmann13, Nadine Hoffmann14, Kristina Höhler14, Evelyn Jantsch8, Alexei Kiselev14, Thomas Koop8, Gourihar Kulkarni3, Amelie Mayer12, Masataka Murakami2,c, Benjamin Murray15, Alessia Nicosia4,d, Markus Petters16, Matteo Piazza4, Michael Polen5, Naama Reicher6, Yinon Rudich6, Atsushi Saito2, Gianni Santachiara4, Thea Schiebel14, Gregg Schill11, Johannes Schneider9, Lior Segev6, Emiliano Stopelli10,e, Ryan Sullivan5, Kaitlyn Suski3,11, Miklós Szakáll12, Takuya Tajiri2, Hans Taylor16, Yutaka Tobo17,18, Daniel Weber7, Heike Wex13, Thomas Whale15, Craig Whiteside1, Katsuya Yamashita2,f, Alla Zelenyuk3, and Ottmar Möhler14 Naruki Hiranuma et al.
  • 1Department of Life, Earth and Environmental Sciences, West Texas A&M University, Canyon, TX, USA
  • 2Meteorological Research Institute, Tsukuba, Japan
  • 3Pacific Northwest National Laboratory, Richland, WA, USA
  • 4Institute of Atmospheric Sciences and Climate, National Research Council, Bologna, Italy
  • 5Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA, USA
  • 6Department of Earth and Plane tary Sciences, Weizmann Institute, Rehovot, Israel
  • 7Institute for Atmospheric and Environmental Science, Goethe University of Frankfurt, Frankfurt/M., Germany
  • 8Faculty of Chemistry, Bielefeld University, Bielefeld, Germany
  • 9Max-Planck-Institut für Chemie, Mainz, Germany
  • 10Environmental Geosciences, University of Basel, Basel, Switzerland
  • 11Department of Atmospheric Science, Colorado State University, Fort Collins, CO, USA
  • 12Institute for Atmospheric Physics, University of Mainz, Mainz, Germany
  • 13Leibniz Institute for Tropospheric Research, Leipzig, Germany
  • 14Institute for Meteorology and Climate Research – Atmospheric Aerosol Research, Karlsruhe Institute of Technology, Karlsruhe, Germany
  • 15Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, UK
  • 16Department of Marine, Earth, and Atmospheric Sciences, North Carolina State University Raleigh, NC, USA
  • 17National Institute of Polar Research, Tachikawa, Tokyo, Japan
  • 18Department of Polar Science, School of Multidisciplinary Sciences, SOKENDAI (The Graduate University for Advanced Studies), Tachikawa, Tokyo, Japan
  • anow at: Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
  • bnow at: Department of Soil and Water Sciences, Hebrew University of Jerusalem, Israel
  • cnow at: Institute for Space-Earth Environmental Research, Nagoya University, Nagoya, Japan
  • dnow at: Laboratoire de Météorologie Physique (Lamp-CNRS) Aubiere, France
  • enow at: Water Resources and Drinking Water Department, Eawag, Dübendorf, Switzerland
  • fnow at: Snow and Ice Research Center, Nagaoka, Japan

Abstract. We present the laboratory results of immersion freezing efficiencies of cellulose particles at supercooled temperature (T) conditions. Three types of chemically homogeneous cellulose samples are used as surrogates that represent supermicron and submicron ice nucleating plant structural polymers. These samples include micro-crystalline cellulose (MCC), fibrous cellulose (FC) and nano-crystalline cellulose (NCC). Our experimental data show that particles resembling the MCC lab particle occur also in the atmosphere. Our immersion freezing dataset includes data from various ice nucleation measurement techniques available at seventeen different institutions, including nine dry dispersion and eleven aqueous suspension techniques. With a total of twenty methods, we performed systematic accuracy and precision analysis of measurements from all twenty measurement techniques by evaluating T-binned (1 °C) data over a wide T range (−36 °C < T < −4 °C). Specifically, we inter-compared the geometric surface area-based ice nucleation active surface-site (INAS) density data derived from our measurements as a function of T, ns,geo(T). Additionally, we also compared the ns,geo(T) values and the freezing spectral slope parameter (Δlog(ns,geo) / ΔT) from our measurements to previous literature results. Results show that freezing efficiencies of NCC samples agree reasonably well, whereas the diversity for the other two samples spans for ~ 10 °C. Despite given uncertainties within each instrument technique, the overall trend of the ns,geo(T) spectrum traced by the T-binned average of measurements suggest that predominantly supermicron-sized (giant hereafter) cellulose particles (MCC and FC) generally act as more efficient ice-nucleating particles than NCC with about one order of magnitude higher ns,geo(T). Further, our results indicate significant diversity between dry and aqueous suspension measurement techniques. The ratios of the individual measurements (ns,ind) to the log average of ns,geo(T) range 0.6–1.4 across the examined T range. In general, the ratios of the log average of dry dispersion measurements are higher than those of aqueous suspension measurements. The observed discrepancy may be due to non-uniform active site density for different sizes and/or the alteration in physico-chemical properties of cellulose by liquid-suspending it. Unless otherwise defined, the cellulose system may not be an ideal calibrant. Given such a distinct difference between two subgroups of immersion freezing techniques, standardization of our methods, especially INP sampling and treatment, may be one approach to reduce the measurement diversity and valiability when we deal with a complex material like cellulose. A community-wide effort to identify specimen-specific limitations and characteristics of each technique, as well as consolidating the ns,geo(T) parameterization, is an alternative approach to achieve overall precise and accurate ice-nucleating particle measurements.

Naruki Hiranuma et al.
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Status: final response (author comments only)
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Naruki Hiranuma et al.
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Short summary
Twenty ice nucleation measurement techniques contributed to investigate the immersion freezing behavior of cellulose particles – natural polymers. Our data showed several types of cellulose have the capacity to nucleate ice as efficiently as some mineral dust samples and cellulose has the potential to be an important atmospheric ice nucleating particle. A continued investigation/collaboration is necessary to obtain further insights into consistency or diversity of ice nucleation measurements.
Twenty ice nucleation measurement techniques contributed to investigate the immersion freezing...