scholarly journals CNT Parameterization Based on the Observed INP Concentration during Arctic Summer Campaigns in a Marine Environment

Atmosphere ◽  
2020 ◽  
Vol 11 (9) ◽  
pp. 916 ◽  
Author(s):  
Ana Cirisan ◽  
Eric Girard ◽  
Jean-Pierre Blanchet ◽  
Setigui Aboubacar Keita ◽  
Wanmin Gong ◽  
...  
Keyword(s):  
Particle Concentration ◽  
Climate Models ◽  
Canadian Arctic ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Atmospheric Models ◽  
Ice Clouds ◽  
Immersion Freezing ◽  
Aerosol Cloud Interactions ◽  
The Right

Aerosol–cloud interactions present a large source of uncertainties in atmospheric and climate models. One of the main challenges to simulate ice clouds is to reproduce the right ice nucleating particle concentration. In this study, we derive a parameterization for immersion freezing according to the classical nucleation theory. Our objective was to constrain this parameterization with observations taken over the Canadian Arctic during the Amundsen summer 2014 and 2016 campaigns. We found a linear dependence of contact angle and temperature. Using this approach, we were able to reproduce the scatter in ice nucleated particle concentrations within a factor 5 of observed values with a small negative bias. This parameterization would be easy to implement in climate and atmospheric models, but its representativeness has to first be validated against other datasets.

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

2013 ◽  
Vol 13 (13) ◽  
pp. 6603-6622 ◽  
Author(s):  
Y. J. Rigg ◽  
P. A. Alpert ◽  
D. A. Knopf
Keyword(s):  
Water Activity ◽  
Active Sites ◽  
Melting Curve ◽  
Contact Angles ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Surface Areas ◽  
Immersion Freezing ◽  
Freezing Temperatures

Abstract. 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 215 K and solution water activity, aw, 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 Δaw = 0.2703 and 0.2466, respectively. Corresponding hetrogeneous 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 Δaw. 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 aw 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 Jhet as a function of temperature and aw that can be applied to conditions outside of those probed in laboratory. This is because Jhet(T) is independent of time and IN surface areas in contrast to the fit parameters obtained by representation of experimentally derived frozen fractions.

scholarly journals A New Ice Nucleation Active Site Parameterization for Desert Dust and Soot

2017 ◽  
Vol 74 (3) ◽  
pp. 699-717 ◽  
Author(s):  
Romy Ullrich ◽  
Corinna Hoose ◽  
Ottmar Möhler ◽  
Monika Niemand ◽  
Robert Wagner ◽  
...  
Keyword(s):  
Active Surface ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Negative Slope ◽  
Organic Carbon Content ◽  
Desert Dust ◽  
Soot Aerosol ◽  
Immersion Freezing ◽  
Heterogeneous Ice Nucleation

Abstract Based on results of 11 yr of heterogeneous ice nucleation experiments at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) chamber in Karlsruhe, Germany, a new empirical parameterization framework for heterogeneous ice nucleation was developed. The framework currently includes desert dust and soot aerosol and quantifies the ice nucleation efficiency in terms of the ice nucleation active surface site (INAS) approach. The immersion freezing INAS densities nS of all desert dust experiments follow an exponential fit as a function of temperature, well in agreement with an earlier analysis of AIDA experiments. The deposition nucleation nS isolines for desert dust follow u-shaped curves in the ice saturation ratio–temperature (Si–T) diagram at temperatures below about 240 K. The negative slope of these isolines toward lower temperatures may be explained by classical nucleation theory (CNT), whereas the behavior toward higher temperatures may be caused by a pore condensation and freezing mechanism. The deposition nucleation measured for soot at temperatures below about 240 K also follows u-shaped isolines with a shift toward higher Si for soot with higher organic carbon content. For immersion freezing of soot aerosol, only upper limits for nS were determined and used to rescale an existing parameterization line. The new parameterization framework is compared to a CNT-based parameterization and an empirical framework as used in models. The comparison shows large differences in shape and magnitude of the nS isolines especially for deposition nucleation. For the application in models, implementation of this new framework is simple compared to that of other expressions.

scholarly journals Classical nucleation theory of immersion freezing: sensitivity of contact angle schemes to thermodynamic and kinetic parameters

2017 ◽  
Vol 17 (3) ◽  
pp. 1713-1739 ◽  
Author(s):  
Luisa Ickes ◽  
André Welti ◽  
Ulrike Lohmann
Keyword(s):  
Experimental Data ◽  
Contact Angle ◽  
Kinetic Parameters ◽  
Aerosol Particles ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Kinetic And Thermodynamic Parameters ◽  
Immersion Freezing ◽  
Thermodynamic And Kinetic Parameters ◽  
Homogeneous Freezing

Abstract. Heterogeneous ice formation by immersion freezing in mixed-phase clouds can be parameterized in general circulation models (GCMs) by classical nucleation theory (CNT). CNT parameterization schemes describe immersion freezing as a stochastic process, including the properties of insoluble aerosol particles in the droplets. There are different ways to parameterize the properties of aerosol particles (i.e., contact angle schemes), which are compiled and tested in this paper. The goal of this study is to find a parameterization scheme for GCMs to describe immersion freezing with the ability to shift and adjust the slope of the freezing curve compared to homogeneous freezing to match experimental data. We showed in a previous publication that the resulting freezing curves from CNT are very sensitive to unconstrained kinetic and thermodynamic parameters in the case of homogeneous freezing. Here we investigate how sensitive the outcome of a parameter estimation for contact angle schemes from experimental data is to unconstrained kinetic and thermodynamic parameters. We demonstrate that the parameters describing the contact angle schemes can mask the uncertainty in thermodynamic and kinetic parameters. Different CNT formulations are fitted to an extensive immersion freezing dataset consisting of size-selected measurements as a function of temperature and time for different mineral dust types, namely kaolinite, illite, montmorillonite, microcline (K-feldspar), and Arizona test dust. We investigated how accurate different CNT formulations (with estimated fit parameters for different contact angle schemes) reproduce the measured freezing data, especially the time and particle size dependence of the freezing process. The results are compared to a simplified deterministic freezing scheme. In this context, we evaluated which CNT-based parameterization scheme able to represent particle properties is the best choice to describe immersion freezing in a GCM.

scholarly journals Classical nucleation theory of immersion freezing: Sensitivity of contact angle schemes to thermodynamic and kinetic parameters

2016 ◽  
Author(s):  
L. Ickes ◽  
A. Welti ◽  
U. Lohmann
Keyword(s):  
Experimental Data ◽  
Contact Angle ◽  
Kinetic Parameters ◽  
Aerosol Particles ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Kinetic And Thermodynamic Parameters ◽  
Immersion Freezing ◽  
Thermodynamic And Kinetic Parameters ◽  
Homogeneous Freezing

Abstract. Heterogeneous ice formation by immersion freezing in mixed-phase clouds can be parameterized in general circulation models (GCMs) by Classical Nucleation Theory (CNT). CNT parameterization schemes describe freezing as a stochastic process including the properties of insoluble aerosol particles, so called ice nuclei, in the droplets. There are different ways how to describe the properties of aerosol particles (i.e. contact angle schemes), which are compiled and tested in this paper. The goal of this study is to find a parameterization scheme for GCMs to describe immersion freezing with the ability to shift and adjust the slope of the freezing curve compared to homogeneous freezing to match experimental data. The results of using CNT are very sensitive to unconstrained kinetic and thermodynamic parameters in the case of homogeneous freezing leading to uncertainties in calculated nucleation rates Jhom of several orders of magnitude. Here we investigate how sensitive the outcome of a parameter estimation for contact angle schemes from experimental data is to kinetic and thermodynamic parameters. We show that additional free parameter can mask the uncertainty of Jimm due to thermodynamic and kinetic parameters. Different CNT formulations are fitted to an extensive immersion freezing dataset as a function of particle diameter (d), temperature T and time t for different mineral dust types, namely kaolinite, illite, montmorillonite, microcline (K-feldspar) and Arizona test dust. It is investigated how accurate different CNT formulations (with the estimated fit parameters) reproduce the measured freezing curves, especially the time and particle size dependence of the freezing process. The results are compared to a simplified deterministic freezing scheme. It is evaluated in this context which CNT based parameterization scheme to represent particle properties is a good choice to describe immersion freezing in a GCM.

scholarly journals Immersion freezing of water and aqueous ammonium sulphate droplets initiated by Humic Like Substances as a function of water activity

2013 ◽  
Vol 13 (2) ◽  
pp. 4917-4961
Author(s):  
Y. J. Rigg ◽  
P. A. Alpert ◽  
D. A. Knopf
Keyword(s):  
Water Activity ◽  
Active Sites ◽  
Melting Curve ◽  
Contact Angles ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Surface Areas ◽  
Immersion Freezing ◽  
Freezing Temperatures

Abstract. 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 215 K and solution water activity, aw, from 0.85–1.0. 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, Δaw, by 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 Δaw. Consequently predictions of freezing temperatures and kinetics can be made without knowledge of the solute type when relative humidity and 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 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. 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 Jhet as a function of temperature and aw that can be applied to conditions outside of those probed in laboratory. This is because Jhet(T) is independent of time and IN surface areas in contrast to the fit parameters obtained by representation of experimentally derived frozen fractions.

scholarly journals Time dependence of immersion freezing: an experimental study on size selected kaolinite particles

2012 ◽  
Vol 12 (20) ◽  
pp. 9893-9907 ◽  
Author(s):  
A. Welti ◽  
F. Lüönd ◽  
Z. A. Kanji ◽  
O. Stetzer ◽  
U. Lohmann
Keyword(s):  
Time Dependence ◽  
Residence Time ◽  
Particle Surface ◽  
Laboratory Data ◽  
Contact Angles ◽  
Ice Nucleation ◽  
Mixed Phase ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Immersion Freezing

Abstract. The time dependence of immersion freezing was studied for temperatures between 236 K and 243 K. Droplets with single immersed, size-selected 400 nm and 800 nm kaolinite particles were produced at 300 K, cooled down to supercooled temperatures, and the fraction of frozen droplets with increasing residence time was detected. To simulate the conditions of immersion freezing in mixed-phase clouds we used the Zurich Ice Nucleation Chamber (ZINC) and its vertical extension, the Immersion Mode Cooling chAmber (IMCA). We observed that the frozen fraction of droplets increased with increasing residence time in the chamber. This suggests that there is a time dependence of immersion freezing and supports the importance of a stochastic component in the ice nucleation process. The rate at which droplets freeze was observed to decrease towards higher temperatures and smaller particle sizes. Comparison of the laboratory data with four different ice nucleation models, three based on classical nucleation theory with different representations of the particle surface properties and one singular, suggest that the classical, stochastic approach combined with a distribution of contact angles is able to reproduce the ice nucleation observed in these experiments most accurately. Using the models to calculate the increase in frozen fraction at typical mixed-phase cloud temperatures over an extended period of time, yields an equivalent effect of −1 K temperature shift for an increase in times scale by one order of magnitude. This suggests that temperature is more important than time.

scholarly journals Parameterization of homogeneous ice nucleation for cloud and climate models based on classical nucleation theory

2012 ◽  
Vol 12 (3) ◽  
pp. 6745-6803
Author(s):  
V. I. Khvorostyanov ◽  
J. A. Curry
Keyword(s):  
Climate Models ◽  
Water Saturation ◽  
Ice Nucleation ◽  
Small Time ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Free Energies ◽  
Elementary Functions ◽  
Analytical Functions ◽  
Semi Empirical

Abstract. A new analytical parameterization of homogeneous ice nucleation is developed based on extended classical nucleation theory including new equations for the critical radii of the ice germs, free energies and nucleation rates as the functions of the temperature and water saturation ratio simultaneously. By representing these quantities as separable products of the analytical functions of the temperature and supersaturation, analytical solutions are found for the integral-differential supersaturation equation and concentration of nucleated crystals. Parcel model simulations are used to illustrate the general behavior of various nucleation properties under various conditions, for justifications of the further key analytical simplifications, and for verification of the resulting parameterization. The final parameterization is based upon the values of the supersaturation that determines the current or maximum concentrations of the nucleated ice crystals. The crystal concentration is analytically expressed as a function of time and can be used for parameterization of homogeneous ice nucleation both in the models with small time steps and for substep parameterization in the models with large time steps. The crystal concentration is expressed analytically via the error functions or elementary functions and depends only on the fundamental atmospheric parameters and parameters of classical nucleation theory. The diffusion and kinetic limits of the new parameterization agree with previous semi-empirical parameterizations.

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