scholarly journals Time-dependence of Heterogeneous Ice Nucleation by Ambient Aerosols: Laboratory Observations and a Formulation for Models

2021 ◽  
Author(s):  
Jonas Jakobsson ◽  
Vaughan Phillips ◽  
Thomas Bjerring-Kristensen
Keyword(s):  
Time Dependence ◽  
Time Scales ◽  
Ice Nucleation ◽  
Published Data ◽  
General Tendency ◽  
Time Dependency ◽  
Ambient Aerosol ◽  
Cold Stage ◽  
Natural Time ◽  
Heterogeneous Ice Nucleation

Abstract. The time dependence of ice-nucleating particle (INP) activity is known to exist, yet for simplicity it is often omitted in atmospheric models as an approximation. Hitherto only limited experimental work has been done to quantify this time dependency, for which published data are especially scarce regarding ambient aerosol samples and longer time scales. In this study, the time dependence of INP activity is quantified experimentally for ambient environmental samples. The experimental approach includes a series of hybrid experiments with alternating constant cooling and isothermal experiments using a recently developed cold-stage setup called the Lund University Cold-Stage (LUCS). This approach of observing ambient aerosol samples provides the optimum realism for representing their time dependence in any model. Six ambient aerosol samples were collected representing aerosol conditions likely influenced by these types of INPs: marine, mineral dust, continental pristine, continental polluted, combustion-related and rural continental aerosol. Active INP concentrations were seen to be augmented by about 40 % to 100 % (or 70 % to 200 %), depending on the sample, over 2 (or 10) hours. This degree of time dependence observed was comparable to that seen in previous published works. Our observations show that the minority of active ice nuclei (IN) with strong time dependency on hourly time scales display only weak time dependence on short time scales of a few minutes. A general tendency was observed for the natural time scale of the freezing to dilate increasingly with time. The fractional freezing rate was observed to steadily declines exponentially with the order of magnitude (logarithm) of the time since the start of isothermal conditions. A representation of time dependence for incorporation into schemes of heterogeneous ice nucleation that currently omit time dependence is proposed.

scholarly journals On the Thermodynamic and Dynamic Aspects of Immersion Ice Nucleation

2017 ◽  
Author(s):  
Donifan Barahona
Keyword(s):  
Liquid Phase ◽  
Theoretical Models ◽  
Ice Nucleation ◽  
Ice Formation ◽  
Published Data ◽  
Water Molecules ◽  
New Approach ◽  
Main Pathway ◽  
Nucleation Work ◽  
Heterogeneous Ice Nucleation

Abstract. Heterogeneous ice nucleation initiated by particles immersed within droplets is likely the main pathway of ice formation in the atmosphere. Theoretical models commonly used to describe this process assume that it mimics ice formation from the vapor, neglecting interactions unique to the liquid phase. This work introduces a new approach that accounts for such interactions by linking the ability of particles to promote ice formation to the modification of the properties of water near the particle-liquid interface. It is shown that the same mechanism that lowers the thermodynamic barrier for ice nucleation also tends to decrease the mobility of water molecules, hence the ice-liquid interfacial flux. Heterogeneous ice nucleation in the liquid phase is thus determined by the competition between thermodynamic and kinetic constraints to the formation and propagation of ice. At the limit, ice nucleation may be mediated by the dynamics of vicinal water instead of the nucleation work. This new ice nucleation regime is termed spinodal ice nucleation. Comparison of predicted nucleation rates against published data suggests that some materials of atmospheric relevance may nucleate ice in this regime.

scholarly journals BINARY: an optical freezing array for assessing temperature and time dependence of heterogeneous ice nucleation

2014 ◽  
Vol 7 (9) ◽  
pp. 9137-9172 ◽  
Author(s):  
C. Budke ◽  
T. Koop
Keyword(s):  
Time Dependence ◽  
Ice Nucleation ◽  
Strong Increase ◽  
Cooling Rates ◽  
Class A ◽  
Vapor Transfer ◽  
Ice Nucleators ◽  
Type Water ◽  
Optical Brightness ◽  
Heterogeneous Ice Nucleation

Abstract. A new optical freezing array for the study of heterogeneous ice nucleation in microliter-sized droplets is introduced, tested and applied to the study of immersion freezing in aqueous Snomax® suspensions. In the Bielefeld Ice Nucleation ARraY (BINARY) ice nucleation can be studied simultaneously in 36 droplets at temperatures down to −40 °C (233 K) and at cooling rates between 0.1 K min−1 and 10 K min−1. The droplets are separated from each other in individual compartments, thus preventing a Wegener–Bergeron–Findeisen type water vapor transfer between droplets as well as avoiding the seeding of neighboring droplets by formation and surface growth of frost halos. Analysis of freezing and melting occurs via an automated real time image analysis of the optical brightness of each individual droplet. As an application ice nucleation in water droplets containing Snomax® at concentrations from 1 ng mL−1 to 1 mg mL−1 was investigated. Using different cooling rates a minute time dependence of ice nucleation induced by Class A and Class C ice nucleators contained in Snomax® was detected. For the Class A IN a very strong increase of the heterogeneous ice nucleation rate coefficient with decreasing temperature of λ ≡ −dln(jhet)/dT = 8.7 K−1 was observed emphasizing the capability of the BINARY device. This value is larger than those of other types of IN reported in the literature, suggesting that the BINARY setup is suitable for quantifying time dependence for most other IN of atmospheric interest, making it a useful tool for future investigations.

scholarly journals BINARY: an optical freezing array for assessing temperature and time dependence of heterogeneous ice nucleation

2015 ◽  
Vol 8 (2) ◽  
pp. 689-703 ◽  
Author(s):  
C. Budke ◽  
T. Koop
Keyword(s):  
Time Dependence ◽  
Ice Nucleation ◽  
Small Time ◽  
Cooling Rates ◽  
Vapor Transfer ◽  
Ice Nucleators ◽  
Immersion Freezing ◽  
Type Water ◽  
Optical Brightness ◽  
Heterogeneous Ice Nucleation

Abstract. A new optical freezing array for the study of heterogeneous ice nucleation in microliter-sized droplets is introduced, tested and applied to the study of immersion freezing in aqueous Snomax® suspensions. In the Bielefeld Ice Nucleation ARraY (BINARY) ice nucleation can be studied simultaneously in 36 droplets at temperatures down to −40 °C (233 K) and at cooling rates between 0.1 and 10 K min−1. The droplets are separated from each other in individual compartments, thus preventing a Wegener–Bergeron–Findeisen type water vapor transfer between droplets as well as avoiding the seeding of neighboring droplets by formation and surface growth of frost halos. Analysis of freezing and melting occurs via an automated real-time image analysis of the optical brightness of each individual droplet. As an application ice nucleation in water droplets containing Snomax® at concentrations from 1 ng mL−1 to 1 mg mL−1 was investigated. Using different cooling rates, a small time dependence of ice nucleation induced by two different classes of ice nucleators (INs) contained in Snomax® was detected and the corresponding heterogeneous ice nucleation rate coefficient was quantified. The observed time dependence is smaller than those of other types of INs reported in the literature, suggesting that the BINARY setup is suitable for quantifying time dependence for most other INs of atmospheric interest, making it a useful tool for future investigations.

scholarly journals On the thermodynamic and kinetic aspects of immersion ice nucleation

2018 ◽  
Vol 18 (23) ◽  
pp. 17119-17141 ◽  
Author(s):  
Donifan Barahona
Keyword(s):  
Liquid Phase ◽  
Theoretical Models ◽  
Ice Nucleation ◽  
Ice Formation ◽  
Published Data ◽  
Water Molecules ◽  
New Approach ◽  
Main Pathway ◽  
Nucleation Work ◽  
Heterogeneous Ice Nucleation

Abstract. Heterogeneous ice nucleation initiated by particles immersed within droplets is likely the main pathway of ice formation in the atmosphere. Theoretical models commonly used to describe this process assume that it mimics ice formation from the vapor, neglecting interactions unique to the liquid phase. This work introduces a new approach that accounts for such interactions by linking the ability of particles to promote ice formation to the modification of the properties of water near the particle–liquid interface. It is shown that the same mechanism that lowers the thermodynamic barrier for ice nucleation also tends to decrease the mobility of water molecules, hence the ice–liquid interfacial flux. Heterogeneous ice nucleation in the liquid phase is thus determined by the competition between thermodynamic and kinetic constraints to the formation and propagation of ice. At the limit, ice nucleation may be mediated by kinetic factors instead of the nucleation work. This new ice nucleation regime is termed spinodal ice nucleation. The comparison of predicted nucleation rates against published data suggests that some materials of atmospheric relevance may nucleate ice in this regime.

scholarly journals Development, Characterization, and Validation of a Cold Stage-Based Ice Nucleation Array (PKU-INA)

Atmosphere ◽  
2018 ◽  
Vol 9 (9) ◽  
pp. 357 ◽  
Author(s):  
Jie Chen ◽  
Xiangyu Pei ◽  
Hong Wang ◽  
Jingchuan Chen ◽  
Yishu Zhu ◽  
...  
Keyword(s):  
Ice Nucleation ◽  
Temperature Calibration ◽  
Cold Stage ◽  
Reliable Instrument ◽  
Peking University ◽  
Calibration Protocol ◽  
Immersion Freezing ◽  
And Performance ◽  
Good Agreement ◽  
Heterogeneous Ice Nucleation

A drop-freeze array (PeKing University Ice Nucleation Array, PKU-INA) was developed based on the cold-stage method to investigate heterogeneous ice nucleation properties of atmospheric particles in the immersion freezing mode from −30 to 0 °C. The instrumental details as well as characterization and performance evaluation are described in this paper. A careful temperature calibration protocol was developed in our work. The uncertainties in the reported temperatures were found to be less than 0.4 °C at various cooling rates after calibration. We also measured the ice nucleation activities of droplets containing different mass concentrations of illite NX, and the results obtained in our work show good agreement with those reported previously using other instruments with similar principles. Overall, we show that our newly developed PKU-INA is a robust and reliable instrument for investigation of heterogeneous ice nucleation in the immersion freezing mode.

scholarly journals Efficiency of immersion mode ice nucleation on surrogates of mineral dust

2007 ◽  
Vol 7 (19) ◽  
pp. 5081-5091 ◽  
Author(s):  
C. Marcolli ◽  
S. Gedamke ◽  
T. Peter ◽  
B. Zobrist
Keyword(s):  
Contact Angle ◽  
Active Sites ◽  
Quantitative Agreement ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Aqueous Suspensions ◽  
Freezing Temperatures ◽  
Good Agreement ◽  
Heterogeneous Ice Nucleation

Abstract. A differential scanning calorimeter (DSC) was used to explore heterogeneous ice nucleation of emulsified aqueous suspensions of two Arizona test dust (ATD) samples with particle diameters of nominally 0–3 and 0–7 μm, respectively. Aqueous suspensions with ATD concentrations of 0.01–20 wt% have been investigated. The DSC thermograms exhibit a homogeneous and a heterogeneous freezing peak whose intensity ratios vary with the ATD concentration in the aqueous suspensions. Homogeneous freezing temperatures are in good agreement with recent measurements by other techniques. Depending on ATD concentration, heterogeneous ice nucleation occurred at temperatures as high as 256 K or down to the onset of homogeneous ice nucleation (237 K). For ATD-induced ice formation Classical Nucleation Theory (CNT) offers a suitable framework to parameterize nucleation rates as a function of temperature, experimentally determined ATD size, and emulsion droplet volume distributions. The latter two quantities serve to estimate the total heterogeneous surface area present in a droplet, whereas the suitability of an individual heterogeneous site to trigger nucleation is described by the compatibility function (or contact angle) in CNT. The intensity ratio of homogeneous to heterogeneous freezing peaks is in good agreement with the assumption that the ATD particles are randomly distributed amongst the emulsion droplets. The observed dependence of the heterogeneous freezing temperatures on ATD concentrations cannot be described by assuming a constant contact angle for all ATD particles, but requires the ice nucleation efficiency of ATD particles to be (log)normally distributed amongst the particles. Best quantitative agreement is reached when explicitly assuming that high-compatibility sites are rare and that therefore larger particles have on average more and better active sites than smaller ones. This analysis suggests that a particle has to have a diameter of at least 0.1 μm to exhibit on average one active site.

scholarly journals Simulating the influence of primary biological aerosol particles on clouds by heterogeneous ice nucleation

2018 ◽  
Vol 18 (20) ◽  
pp. 15437-15450 ◽  
Author(s):  
Matthias Hummel ◽  
Corinna Hoose ◽  
Bernhard Pummer ◽  
Caroline Schaupp ◽  
Janine Fröhlich-Nowoisky ◽  
...  
Keyword(s):  
Pseudomonas Syringae ◽  
Aerosol Particles ◽  
Fungal Spores ◽  
Ice Nucleation ◽  
Ice Crystals ◽  
Atmospheric Measurements ◽  
Cloud Ice ◽  
Biological Aerosol Particles ◽  
Ice Phase ◽  
Heterogeneous Ice Nucleation

Abstract. Primary ice formation, which is an important process for mixed-phase clouds with an impact on their lifetime, radiative balance, and hence the climate, strongly depends on the availability of ice-nucleating particles (INPs). Supercooled droplets within these clouds remain liquid until an INP immersed in or colliding with the droplet reaches its activation temperature. Only a few aerosol particles are acting as INPs and the freezing efficiency varies among them. Thus, the fraction of supercooled water in the cloud depends on the specific properties and concentrations of the INPs. Primary biological aerosol particles (PBAPs) have been identified as very efficient INPs at high subzero temperatures, but their very low atmospheric concentrations make it difficult to quantify their impact on clouds. Here we use the regional atmospheric model COSMO–ART to simulate the heterogeneous ice nucleation by PBAPs during a 1-week case study on a domain covering Europe. We focus on three highly ice-nucleation-active PBAP species, Pseudomonas syringae bacteria cells and spores from the fungi Cladosporium sp. and Mortierella alpina. PBAP emissions are parameterized in order to represent the entirety of bacteria and fungal spores in the atmosphere. Thus, only parts of the simulated PBAPs are assumed to act as INPs. The ice nucleation parameterizations are specific for the three selected species and are based on a deterministic approach. The PBAP concentrations simulated in this study are within the range of previously reported results from other modeling studies and atmospheric measurements. Two regimes of PBAP INP concentrations are identified: a temperature-limited and a PBAP-limited regime, which occur at temperatures above and below a maximal concentration at around −10 ∘C, respectively. In an ensemble of control and disturbed simulations, the change in the average ice crystal concentration by biological INPs is not statistically significant, suggesting that PBAPs have no significant influence on the average state of the cloud ice phase. However, if the cloud top temperature is below −15 ∘C, PBAP can influence the cloud ice phase and produce ice crystals in the absence of other INPs. Nevertheless, the number of produced ice crystals is very low and it has no influence on the modeled number of cloud droplets and hence the cloud structure.

scholarly journals Heterogeneous ice nucleation of viscous secondary organic aerosol produced from ozonolysis of <i>α</i>-pinene

2016 ◽  
Vol 16 (10) ◽  
pp. 6495-6509 ◽  
Author(s):  
Karoliina Ignatius ◽  
Thomas B. Kristensen ◽  
Emma Järvinen ◽  
Leonid Nichman ◽  
Claudia Fuchs ◽  
...  
Keyword(s):  
Secondary Organic Aerosol ◽  
Solid Phase ◽  
Particle Surface ◽  
Amorphous Solid ◽  
Organic Aerosol ◽  
Ice Nucleation ◽  
Cloud Formation ◽  
Particle Surface Area ◽  
Semi Solid ◽  
Heterogeneous Ice Nucleation

Abstract. There are strong indications that particles containing secondary organic aerosol (SOA) exhibit amorphous solid or semi-solid phase states in the atmosphere. This may facilitate heterogeneous ice nucleation and thus influence cloud properties. However, experimental ice nucleation studies of biogenic SOA are scarce. Here, we investigated the ice nucleation ability of viscous SOA particles. The SOA particles were produced from the ozone initiated oxidation of α-pinene in an aerosol chamber at temperatures in the range from −38 to −10 °C at 5–15 % relative humidity with respect to water to ensure their formation in a highly viscous phase state, i.e. semi-solid or glassy. The ice nucleation ability of SOA particles with different sizes was investigated with a new continuous flow diffusion chamber. For the first time, we observed heterogeneous ice nucleation of viscous α-pinene SOA for ice saturation ratios between 1.3 and 1.4 significantly below the homogeneous freezing limit. The maximum frozen fractions found at temperatures between −39.0 and −37.2 °C ranged from 6 to 20 % and did not depend on the particle surface area. Global modelling of monoterpene SOA particles suggests that viscous biogenic SOA particles are indeed present in regions where cirrus cloud formation takes place. Hence, they could make up an important contribution to the global ice nucleating particle budget.

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