Immersion freezing of water and aqueous ammonium sulfate droplets initiated by humic-like substances as a function of water activity

Rigg, Y. J.; Alpert, P. A.; Knopf, Daniel A.

doi:10.5194/acp-13-6603-2013

Title: Immersion freezing of water and aqueous ammonium sulfate droplets initiated by humic-like substances as a function of water activity

Journal Article · Fri Jul 12 00:00:00 EDT 2013 · Atmospheric Chemistry and Physics (Online)

DOI:https://doi.org/10.5194/acp-13-6603-2013· OSTI ID:1349252

Rigg, Y. J. ^[1]; Alpert, P. A. ^[1]; Knopf, Daniel A. ^[1]

Stony Brook Univ., Stony Brook, NY (United States)

Immersion freezing of water and aqueous (NH₄)₂SO₄ droplets containing leonardite (LEO) and Pahokee peat (PP) serving as surrogates for humic-like substances (HULIS) has been investigated. Organic aerosol containing HULIS are ubiquitous in the atmosphere; however, their potential for ice cloud formation is uncertain. Immersion freezing has been studied for temperatures as low as 215K and solution water activity, a_w, from 0.85 to 1.0. The freezing temperatures of water and aqueous solution droplets containing LEO and PP are 5–15 K warmer than homogeneous ice nucleation temperatures. Heterogeneous freezing temperatures can be represented by a horizontal shift of the ice melting curve as a function of solution aw by Δa_w = 0.2703 and 0.2466, respectively. Corresponding heterogeneous ice nucleation rate coefficients, Jhet, are (9.6 ± 2.5) × 10⁴ and (5.4 ± 1.4) × 10⁴ cm^-2 s^-1 for LEO and PP containing droplets, respectively, and remain constant along freezing curves characterized by Δa_w. Consequently predictions of freezing temperatures and kinetics can be made without knowledge of the solute type when relative humidity and ice nuclei (IN) surface areas are known. The acquired ice nucleation data are applied to evaluate different approaches to fit and reproduce experimentally derived frozen fractions. In addition, we apply a basic formulation of classical nucleation theory (α(T)-model) to calculate contact angles and frozen fractions. Contact angles calculated for each ice nucleus as a function of temperature, α(T)-model, reproduce exactly experimentally derived frozen fractions without involving free-fit parameters. However, assigning the IN a single contact angle for the entire population (single-α model) is not suited to represent the frozen fractions. Application of α-PDF, active sites, and deterministic model approaches to measured frozen fractions yield similar good representations. Furthermore, when using a single parameterization of α-PDF or active sites distribution to fit all individual a_w immersion freezing data simultaneously, frozen fraction curves are not reproduced. This implies that these fitting formulations cannot be applied to immersion freezing of aqueous solutions, and suggests that derived fit parameters do not represent independent particle properties. Thus, from fitting frozen fractions only, the underlying ice nucleation mechanism and nature of the ice nucleating sites cannot be inferred. In contrast to using fitted functions obtained to represent experimental conditions only, we suggest to use experimentally derived J_het as a function of temperature and a_w that can be applied to conditions outside of those probed in laboratory. Finally, this is because J_het(T) is independent of time and IN surface areas in contrast to the fit parameters obtained by representation of experimentally derived frozen fractions.

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Research Organization:: Stony Brook Univ., NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: SC0008613

OSTI ID:: 1349252

Journal Information:: Atmospheric Chemistry and Physics (Online), Vol. 13, Issue 13; ISSN 1680-7324

Publisher:: European Geosciences UnionCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 31 works

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Ice nucleation activity of silicates and aluminosilicates in pure water and aqueous solutions - Part 3: Aluminosilicates Anand, Kumar,; Claudia, Marcolli,; Thomas, Peter, ETH Zurich https://doi.org/10.3929/ethz-b-000343155	text	January 2019
Classical nucleation theory of immersion freezing: Sensitivity of contact angle schemes to thermodynamic and kinetic parameters Ickes, Luisa; Welti, André; Lohmann, Ulrike Atmospheric Chemistry and Physics https://doi.org/10.5194/acp-2015-969	posted_content	January 2016
Cleaning up our water: reducing interferences from nonhomogeneous freezing of “pure” water in droplet freezing assays of ice-nucleating particles Polen, Michael; Brubaker, Thomas; Sullivan, Christopher Carnegie Mellon University https://doi.org/10.1184/r1/7262900	text	January 2018
Laboratory studies of immersion and deposition mode ice nucleation of ozone aged mineral dust particles Kanji, Zamin A.; Welti, André; Chou, Cédric ETH Zurich https://doi.org/10.3929/ethz-b-000071931	text	January 2013
Cleaning up our water: reducing interferences from nonhomogeneous freezing of “pure” water in droplet freezing assays of ice-nucleating particles Polen, Michael; Brubaker, Thomas; Sullivan, Christopher Carnegie Mellon University https://doi.org/10.1184/r1/7262900.v1	text	January 2018
Classical nucleation theory of immersion freezing: Sensitivity of contact angle schemes to thermodynamic and kinetic parameters Ickes, Luisa; Welti, André; Lohmann, Ulrike ETH Zurich https://doi.org/10.3929/ethz-b-000128558	text	January 2017

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